NBS

Publications

AlllQM M33T70

NBSIR 82~2472

Migration of Low Molecular

Weight Additives in Polyolefins

and Copolymers

U.S. OEPARTiVlHNT OF COMMERCE

Natkonal Bureau of Standards

• Center for Materials Science

Polymer Science and Standards Division

Washington. DC 20234

Final Project Report

Issued March 1982

-QC

lOU

.U56

82-2^72

1982

Prepared for Bureau of Foods

Food and Drug Administration

Washington, DC 20201

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or BTAi^Ajuia

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NBSIR 82-2472 ^ 7 ?S82

? • ••

' MIGRATION OF LOW MOLECULAR

WEIGHT ADDITIVES IN POLYOLEFINS

AND COPOLYMERS

S. S. Chang, G. A. Senich and L E. Smith

U.S. DEPARTMENT OF COMMERCE

National Bureau of Standards

Center for Materials Science

Polymer Science and Standards Division

Washington, DC 20234

Final Project Report

Issued March 1982

Prepared for Bureau of Foods

Food and Drug Administration

Washington, DC 20201

U.S. DEPARTMENT OF COMMERCE, Malcolm Baldrige, Secretary

NATIONAL BUREAU OF STANDARDS, Ernest Ambler, Director

Abstract

Food packaging is an essential part of modern life. Any substances

that migrate from packaging material into foods are viewed as indirect

food additives. In addition to toxicological knowledge, it is important

to know the amount of such indirect food additives expected to be present

in the food during storage and processing. This program, sponsored by

the Bureau of Foods of the Food and Drug Administration, is designed to

provide theoretical models, a reliable data base and methodology for

studying migration phenomena and can provide reasonable worst-case estimates for the concentrations of the indirect additives in foods. In

this final report, we present the results of approximately 250 completed

migration experiments based on radiotracer techniques on the migration

of low molecular weight hydrocarbons and antioxidants from polyethylene,

polypropylene, and ethylene-vinyl acetate copolymers. Results of a study for the determination of relative diffusion coefficients of several

probe molecules in the polyethylene melt by inverse gas chromatography

are also presented. Based on these studies, ethanol appears to be a far

more reasonable food-oil stimulating solvent than n-heptane. Other pure

or mixed triglycerides may also be considered as food-oil simulating

solvents, however they may pose the same analytical difficulties associated

with the use of the food oils themselves.

Keywords: antioxidants, diffusion, ethylene-vinyl acetate copolymers,

food additives, food packaging, inverse gas chromatography, migration,

oligomers, polyethylene, polypropylene, radiotracer.
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4
Migration of Low Molecular Weight Additives in Polyolefins and Their Copolymers

1. Introduction I-l

II. Experimental Details of Extraction Experimerlts II-l

Materials II-2

Sample Plaque Preparation • H-2

Experimental Methods II-3

Run Designation II-6

Estimation of Diffusion Coefficients II -6

III. Results of Polyolefin Extraction Experiments III-l

IV. Loss of BHT from Polymers Stored at Ambient Temperature IV-1

V. Migration of BHT from Ethylene-Vinyl Acetate Copolymer V-1

VI. I6C Determinations of the Relative Diffusion

Coefficients of Several Probes in Linear Polyethylene VI-1

A Review of Pertinent Theory for IGC

Absolute Diffusivity Determinations VI-1

Summary of Previous Results for LPE-Octadecane VI -7

Experimental Details VI-16

Relative Diffusivity Determinations VI-19

Future Results VI-23

VII. A Simplified Migration Decision Tree VII-1

Load' Limited Migration' VII-1

Partition Limited Migration VII-2

Diffusion Limited Migration VII-5

VIII. Simulating Solvents VIII-1

IX. Summary of Conclusions IX-1

X. Appendix: Numerical Data for Migration of

Low Molecular Weight Additives from Polyolefins

and Copolymers

Separate

Cover A-1
List of Figures

IV- 1 BHT Content as a Function of Time

V- 1.1 Migration of BHT from E-5% VA Copolymer at 30°C

V-1.2 Migration of BHT from E-5% VA Copolymer at 60°C

V-1.3 Migration of BHT from E-13% VA Copolymer at 30°C

V-1 .4 Migration of BHT from E-13% VA Copolymer at 60°C

V-2.1 Migration of BHT from E-VA Copolymers into n-Heptane

V-2.2 Migration of BHT from E-VA Copolymers into Corn Oil

V-2.3 Migration of BHT from E-VA Copolymers into Ethanol

V- 2.4 Migration of BHT from E-VA Copolymers into 95% Ethanol

VI- 1 Elution Chromatogram Schematic

VI -2 van Deemter Plot

VI-3 Illustration of Polymer Phase Geometries within an IGC Column

VI-4 Typical Recorder Output of a Probe Peak

VI-5 High Speed Chart Record of Five Determinations of t^ with Methane

VI-6 Typical High Speed Chart Record of a Probe Peak and First Time Derivative

VI- 7 Plot of H Vu^ vs. 2p^/(p^- + Pq)

VII- 1 Flow Chart of Decision Tree

VIII- 1 Comparison of Diffusion Coefficients in Pure Triglycerides and Corn Oil

VI 1

1 -2 Comparison of Diffusion Coefficients in Ethanol and Corn Oil

VIII-3 Effect of Accelerating Solvent

VIII-4 Molecular Weight Distributions of Ethanol and n-Heptane Extracts of LPE

VIII-5 Molecular Weight Distributions of Ethanol and n-Heptane Extracts of BPE

IV
List of Tables

II-l Characteristics of Polyolefin Samples

II-2 Characteristics of Ethyl ene- Vinyl Acetate Copolymers

II“3 Characteri sties of Radioactive Tracers

1 1-4 Run Designation Coding--Sol vent, Temperature, Method

II -5 Run Designation Coding--Sampl

e

Migration of n-Octadecane from Linear Polyethylene

.2 Migration of n-Octadecane to/from Linear Polyethylene

.3 Migration of n-Octadecane from Branched Polyethylene

.4 Migration of n-Octadecane to/from Branched Polyethylene

.5 Migration of n-Octadecane from Polypropylene

III-2.1 Migration of n-Dotriacontane from Linear Polyethylene

.2 Migration of n-Dotriacontane from Branched Polyethylene

.3 Migration of n-Dotriacontane from Polypropylene

III-3.1 Migration of BHT from Linear Polyethylene

.2 Migration of BHT from Branched Polyethylene

.3 Migration of BHT from Polypropyl ene

I II -4.1 Migration of n-Octadecane into Triglycerides

.2 Migration of n-Octadecane into Ethanol and n-Octanol

.3 Migration of n-Octadecane into Ethanol /Water Mixture

.4 Migration of n-Octadecane into n-Heptane

.5 Migration of n-Octadecane into n-Octadecane

.6 Migration of n-Octadecane into Water

III-5.1 Migration of n-Dotriacontane into Triglycerides

.2 Migration of n-Dotriacontane into Ethanol, Ethanol/Water Mixture

and n-Octanol

.3 Migration of n-Dotriacontane into n-Heptane

.4 Migration of n-Dotriacontane into Water

V
.2

.3

.4

111^7.1

.2

.3

IV

1

V-1.1

.2

V-2

VI

1

- 2

-3

” 4

- 5

- 6

- 7

VIII-1

- 2

Migration of BHT into Triglycerides

Migration of BHT into Ethanol, Ethanol/Water Mixtures and n-Octanol

Migration of BHT into n-Heptane

Migration of BHT into Water

Activation Energies of Migration of n-Octadecane

Activation Energies of Migration of n-Dotriacontane

Activation Energies of Migration of BHT

Loss of BHT

Migration of BHT from Ethyl ene-5% Vinyl Acetate Copolymer

Migration of BHT from Ethylene-1 3% Vinyl Acetate Copolymer

Diffusion Coefficients and Activation Energies of Migration of BHT

from E-VA Copolymers

Comparison of the C Coefficient Determined by Two Methods for

LPE-Octadecane at 150®C

Effective Layer Thicknesses for Columns with Differing

Polymer Phase Geometry

Influence of Film Geometry on the Diffusion Coefficient of

Octadecane in Linear Polyethylene at 150°C

Effect of Thickness Distribution on Diffusivity in the Polymer Phase

Probe Employed in an IGC Study of Relative Diffusivity in LPE

Exoerimental Data for an IGC Diffusivity Study of Tridecane in

LPE at 150°C

Relative Diffusivity Results for Several Alkanes and BHT in

LPE at 150°C

Extraction of Polyethyl enes by Solvents

Molecular Weight Distributions of Ethanol and n-Heptane Extractions

of Pol y^thyl enes

VI
I. Introduction

As in the proceeding decades, most foods available today are sold

in packaged forms rather than in bulk for reasons of preservation,

convenience and ease of distribution. The Bureau of Foods of the Food

and Drug Administration has regulatory responsibility for the use of

packaging materials in contact with food. Any substances that migrate

from the food packaging materials into foods are considered to be indirect food additives. The regulatory decisions on the types of packaging materials suitable for use with various types of foods are based

on: the indirect food additives that can be expected to migrate from

the package into the food, ones knowledge of toxicology and the expected

amount of migration during storage and usage. Since it is impossible to

test every conceivable combination of polymer-migrant-food, this program

at the National Bureau of Standards, sponsored by the Food and Drug

Administration, is aimed at providing sound technical suggestions and

reliable data to the Food and Drug Administration, and recommending

theoretical or empirical estimation and extrapolation methods to yield

at least a reasonable worst-case estimates for regulatory purposes.

However, this report represents only the technical opinions of the

authors as representatives of the National Bureau of Standards and

should not be taken in any way as containing regulatory decisions or

recommendations of the Bureau of Foods.

A large number of kinetic experiments were performed involving the

14

migration of radioactive C-labeled paraffinic oligomers (n-octadecane

and n-dotriacontane) and an antioxidant ( butyl ated-hydroxytoluene) from

two different polyethylenes (high density or linear polyethylene and low

density or branched polyethylene), isotactic polypropylene and two

(ethylene-vinyl acetate) copolymers of relatively low vinyl acetate

I-l
content into various solvents including a variety of triglycerides,

alcohols, hydrocarbons, and water at temperatures from room temperature

to 60°C.

Among the correlations for various parameters, it was found that

either the pure triglycerides (e.g. tributyrin and trioctanoin) , mixed

triglycerides, or anhydrous ethanol may successfully be employed as

food-oil simulant in all cases studied. The degree of accelerating

action of extracting migrants by n-heptane over that by the food oils is

quantified.

Future works in the additive migration program should be mainly in

the area of migration of additives from glassy polymers, where the

diffusion coefficients are many orders of magnitude slower than those

for the amorphous or semi-crystalline polymers above their glass transition temperatures.

Inverse gas chromatography (IGC) studies have been used to detetmiine

the relative diffusion coefficients of oligomers and antioxidants in

polymers at temperatures above the glass transition region and in the

supercooled-1 iquid or liquid phase. The determinations of the relative

diffusion coefficients of several probe molecules in polyethylene are

i 1 lustrated.

1-2
II. Experimental Details of Extraction Experiments

All scheduled experiments on the migration of additives from

polyolefins ( polyethyl enes and polypropylenes) are now completed. In

this report ws present a complete summary of the polyolefin work, most

of which has been reported in previous NBSIRs [1-6] on this subject, therefore, other than necessary descriptions to make this report selfexplainatory, detailed discussions on each sub-category will not be

repeated here.

As the copolymer work was started in mid-year and was just completed recently, rather detailed descriptions and discussions of it will

be given in this report.

Migrations of low molecular weight additives moving from polymeric

materials into surrounding liquid media under well stirred conditions

were measured in this laboratory for the following combinations* of base ^

polymer, migrant, migrant concentration, solvent and temperature:

Polymers

Migrants

Migrant Concentration

Solvents

Temperatures

Linear Polyethylene (LPE), SRM 1475

Branched Polyethylene (BPE), SRM 1476

Polypropylene (PP)

Ethyl ene-5% Vinyl Acetate Copolymer

Ethylene- 13% Vinyl Acetate Copolymer

n-Octadecane, n-C-igH^g

n-Dotriacontane,

BHT or 3, 5-di-t-butyl-4-hydroxytoluene

From 30 ppm to 10%

Accelerating solvents: n-Heptane, n-Octadecane

Fat and Oil Simulating Solvents: Corn Oil, Ethanol,

n-Octanol , Tributyrin, Trioctanoin, HB307

Aqueous Solvents: Water, Ethanol-Water Mixtures

24, 30, 40, 60°C

The migrants are radiolabeled by carbon-14. The amount of radioactivity is determined by liquid scintillation counting techniques with

detection limit less than 10 pCi.

II-l
Material

The characteristics of the base polymers are listed in Table II-l

and 1 1-2 and those of the base radioactive-labeled migrants are listed

in Table 1 1-3.

Sample Plaque Preparation

The following procedure for the mixing of additives in the polymer

stock and the molding of the sample plaques was chosen. A large quantity

of polyethylene powder stock was prepared from either the National

Bureau of Standards-Standard Reference Material (NBS-SRM) 1475 or 1476

pellets by first dissolving it in hot toluene or xylene. Most of the

polyethylene precipitates out upon cooling. The precipitate, together

with the residue obtained by evaporating the solvent, was dried in a

vacuum oven to remove the last trace of solvent.

A specific amount of labeled additive dissolved in a highly volatile solvent is mixed with a quantity of the polyethylene powder stock.

The mixture, together with a number of glass beads which act as a ball

mill, is then evaporated to dryness in a rotary evaporator under reduced

pressure at relatively low temperatures. Further drying is carried out

in a vacuum oven.

The mixture is then compression molded in a hydraulic press operated at about 180°C for oligomers and 165°C for BHT. Plaques of 125 inn

X 125 mm or less are molded with brass or stainless steel shim stocks of

appropriate thickness sandwiched between two sheets of Teflon or Teflon

coated plates. Teflon surfaces are used to allow easy removal of the

sample plaques without the use of, and subsequent contamination by,

mold-release agents.

The isotactic polypropylene and (ethylene-vinyl acetate) copolymers

were received in granular form from the suppliers. Therefore, they were

used directly to form slurries with the migrants in solution as described above. II-2
Special problems are encountered in the preparation of sample

plaques with BHT as an additive. A much longer time is required to mix

BHT with polymeric powder in a rotating flask with glass beads acting as

a ball mill. Apparently BHT is relatively insoluble in the polymer even

in the molten state, therefore, sample plaques made from such insufficiently mixed batches of powder mixtures yield autoradiographs of distinctively sharp regions of streaks and patches. Each molding at 185°C

seems to "fix" an additional 15-20% of the available BHT, i.e. only 80%

of the avialable BHT before the last molding may be extracted exhaus*

tively even by n-heptane. Only 20% of original amount of BHT can be

extracted from plaques remolded five times at 185°C. The residual BHT

is combined with the polymer. This residual radioactivity stays in tne

polymeric precipitate, even after the plaques were dissolved in toluene

at high temperatures. However, molding of well mixed batches of BHT and

polymeric powder at 165°C seems to result in rather uniformly distributed

sample plaques with less than 5% of BHT being combined with the polymer.

The final fraction extracted from the original loading, by nheptane, as listed in Tables in Section III, gives an indication of the

unreacted fraction of BHT in those samples. Therefore the original loading

M^, is irrelevant and should be replaced by the remaining unreacted

amount, M^, for kinetic and partition calculations. There are

further complications due to the volatility of BHT or its degraded

components as detailed later in Section II.

Experimental Methods

Two extraction methods were used: (1) continuous extraction into a

limited solvent volume and (2) discrete extraction into a simulated

infinite solvent volume.

II-3
In method (1) an extraction vial of 25 ml volume with a Teflon

valved cap is used. The 10 to 15 ml of solvent, in the vial will only

contact glass walls and Teflon surfaces during normal experimental

processes. A silicone plug is situated above the valve. A small area

of the silicone rubber, less than 1 mm in diameter which is used as a

septum for the hypodermic needle, is exposed to the solvent vapor. The

polymer sample was sometimes surrounded by a nichrome or stainless steel

screen to prevent it from sticking to another sample or to the walls, if

the sample has lower density than the solvent.

The total amount extracted, at time t, is the sum of the amount

of migrant in the solution at time t plus that were removed in previous

aliquots, ^_i

M. = C ,W . +

t St st

s i=l

C .W . SI ai

where C^, and represent the concentration of the migrant, total

weight of the solution (including that of the aliquot for the determination of and the weight of the aliquot, respectively. At equilibrium the partition coefficient is estimated as the ratio of the concentrations in solvent and in polymer at equilibrium,

_ S'” S=” p

C M -M

pcD Q oo where is the amount of migrant originally present in the polymer of

weight Wp, and is the total amount extracted at long times.

In method (2), the polymer sample is immersed in about 10 ml of extracting solvent in a typical 20 ml liquid scintillation counting vial.

At specific times the sample is removed from the solvent, rinsed, and

placed in another vial with fresh solvent to repeat the extraction

process. The rinse is then combined with the previous extracting solvent. The total amount of migrant extracted at time t is simply the sum

II-4
of the migrant from all extracts:

t

M. = E M.

^ i = l

^

Method (1) is able to yield information about the equilibrium

partition coefficient at an infinite extraction time. However, this

method suffers from the rigid requirements of knowing accurately the

weight or volume ratio of aliquot to total solution and accounting for

materials lost during the sampling process for material balance purposes. As the extraction time increases, there is only a very small

change in the concentration of extracted material in the solution,

whereas the weighing or ratio error may persist. Therefore, the results

for method (1) at long times or at high degree of extraction will show

considerable scatter.

Method (2) is much simpler in operation, but simulates a condition

of migration into infinite media. It is relatively free from aforementioned experimental difficulties. However, it should only be used

for convenience where the migrant is highly soluble in or miscible with

the solvent and thus the results of method (1) and method (2) are indistinguishable. It can neither be used to generate equilibrium partition

information nor migration kinetics for cases where the migrant is

sparingly soluble in the solvent.

A method often used in the literature consists of replenishing the

amount of solution aliquot removed for testing with the same amount of

fresh solvent, to keep the volume of solvent and exposed surface area

ratio the same throughout the experiment. This method !s a hybrid of

method (1) and method (2), and thus suffers from the same drawbacks as

those of method (2)

.

For both methods (1) and (2) mentioned above, the extraction vials

are shaken inside a temperature controlled aluminum block on a shaking

II-5
table at a rate of about 200 reciprocations per minute.

In order to check the mass balance and variations in the migrant

concentration, radioactivity of the residual low molecular weight species

remaining in the polymeric sample is monitored by dissolving the sample

in toluene at high temperatures after the extraction proceedure is

ended. We have found that the single crystals or precipitates of polymer

in the counting vial do not interfere with the counting efficiency

beyond the normal uncertainty of the counting results.

Experimental Run Designation

The numerical representation of experimental run designations,

PPSSTTN, are assigned as follows:

1) Least significant digit(N)—method of observation and

repetition number.

2) Tens and Hundreds digits(TT)--temperature in °C.

3) Thousands and Ten Thousands digi ts(SS)--solvent code.

4) Hundred Thousands and Millions digits(PP) —sample code.

This coding scheme is described in more detail in Table II-4 and II-5.

Estimation of Diffusion Coefficient

One of the widely used solutions for the Fickian diffusion equations

solved for the case of diffusion between a plane sheet p of thickness li

and a stirred liquid s of finite volume V^, is presented by J. Crank^^^

00

E n=l

2g(1 g)

1 +a + a^q^

n exp (-q^T) ( 1 )

The solution for the non-zero positive roots, q^, of

tan = -aq„

lies between nn when a=0 and (n-l/2)n when a=». At a<<l,

n/ (1 +a)

.

q^l

[o - a/2(l+a)]TT

II-6

For other values of a,
Migration

of

n-Octadecane

from

Linear

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1

1

1-3. 2

Migration

of

BHT

from

Branched

Polyethylene

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III-3.2

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Table

1

1

1-3. 3

Migration

of

BHT

from

Polypropyl

ene

f*) CH oOD fw OfO

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III-4.1

Migration

of

n-Octadecane

into

Triglycenides

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Table

III-4.2

Migration

of

n-Octadecane

into

Ethanol

and

into

n-Octanol

Potyner

Solvent

RUN

NT.

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Table

III-4.3

Migration

of

n-Octadecane

into

ethanol/Water

Mixture

X m

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Table

III-4.5

Migration

of

n-Octadecane

into

n-Heptane

Xm

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c= OD CD 00 00 CD QOOOOOGOOOOOOOOO 00 00 00 CD 00 4 ••• V 1 W»4 »" 4 4P-4 <^-4 <«-4 v4 <v4 *«m4 •v-f s» o o o o o OOOCJOOOO OCJOOO

9k .sr .V «\" -V .N* .V .v- -NT .s? -NT .V .V- •V .V

«*-« •—I *r“* ^r-4 1^^ ^—4 ^‘4 ^-4 ws: «9G> ^*yl »"4 9 2 • • • tt • Jk »— UJ UJ UJ LU Lii 111 liH»i 111 1,)1 til 111 LUOJUiUi o 0.0. 0-0-0- Q-O.O.O-0-O.Q.a. CL Q. 0.0.0.

Q. _J _J _J _J —1 _J_J_J_iOiCD_JO_ _l^_i03 0- o
Table

III-4.6

Migration

of

n-Octadecane

into

n-Octadecane

X m

•a \

S<>ti d X

u

cr*f7ia3<nco<x>cfi<D O<9 <S9 <9 <9 <9 ^9 <9 999<9 <99 <9 9 1 f I f I I I f UiLtilliiiiUiLtlUJlJU ^

fw JO itTi flO f

w

flO 999fw rw fV. <0E> 999^^99*9^9 999999*9 ^9

i I I f I f i f UJ lli lU lii LJ lAi Ui tli «^

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w ro ^ ^ > “^^*^Ohi<yiOiJ<!T*9 09 9‘-^a><^i9l^ri-

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CO 09 <r« 09 9 <^<90099999

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<yi <Ti 9 C^99ii99999

9*9^9*9*9 9^9*^ 9*^09****^*^^^^^

v^ rw-4 <vj «^J *TM <\i ^iroroo-^^^cjoKM

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0*^:0

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OD

3040601
Table

III-4.4

Migration

of

n-Octadecane

into

Water

Mrrr^rt

^m4 X M GS) OO<S3> ri I I I f CO-J UiUJOJlii

Ck Z, 0>OJOO

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m> *'£> mci o # * • • o ‘S) <S> *3>0

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UiLU

o a. 0. 0. 0. O- .J 00 0.0.
Table

III-5.1

Migration

of

n-Dotriacontrane

into

Triglycerides

OICi|Ck|C4C^J<ViCJ <711 0^ (T*! (T** OOO 'V-* 9OOO CD X m <DOOOO<9<9 9 OOOOOOCDGk i f 1 1 f f 1 i 1 1 1 1 f f f f UiUiuiuJLiiuaii Ul UlUiUilXlQJixILliUJ

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2960600
Table

III-5.2

Migration

of

n-Dotriacontane

into

Ethanol,

Ethanol/Water

Mixtures

and

n-Octanol

04^ OtJCTi MOH 9k 0> ^ 00^0 ©

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III-5.3

Migration

of

n-Dotriacontane

into

n-Heptane

00<S>0> rwr^-oofs.

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III-5.4

Migration

of

n-Dotriacontane

into

Water

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01 -V -Nr -NT -V -NT -V -NT C22222222222

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V- -S* .V -N? ^ ^^

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dl X ©©O©©©© ©©©©©©©©©©©©

— Ui UJ LU UJ LU UJ UI Lii Ui Ul LlI UJ UJ LiJ Ixi lii Ui

O a. Ql O- CL O O. Q. CL 0.0. CL 0-0-0. Q. 0.0. 0.0.

Ou _J^_i©©_iOL _| _j _i ©©03 03 03 CD —1 CL
Table

1II-6.4

Migration

of

BHT

into

Water

roojfo

X M ocs»o OOCDO

\ f f f 1 f i f CCM Hi LULU UilxJOJlAi A Z CDOCD a>*-x>iDO

• • •

• • • • coo’tro

•> CDCDfO^

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m 1 1

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<^4 m<7i 'x>

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z • Z 9^

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oorwrw

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• « • » # • •

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ro ro ro 'X) 'd vo vo

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cviior^ (vjroior^

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> <I ^ <I <X <I <X <I

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c »—»——

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xxxx

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CD 'X> CS) O

LkJ IxILlI a_iL. 0_CL.

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Table

III-7.1

Activation

Energies

of

Migration

of

n-Octadecane

o

X

“J*- —om <xi <xj r><M 04 ro oi oi oj cm cm cvjoj<\jcvi-« cm o

u

o •«or.jno>if>r*.^'-»'«r<ykOjr>CDaDcr. —toojc»Nr><MCvjM)'M'cr>

ui X or>mmis»<7)iiO<rkiooo<Dn’CM^a>«^rwOD^aoci»-^a>«-4CD«4CM<^in«-4r*)

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I I t i I I I I f LaiUJUiiUtaJUJliJUJlii oo-^cjfooorwoo-^

0> 9<Tk CD fw CD 00 09 rw 00 <D rw OD 00 CD 0> CMN> ON 00

CD G5'^D^DCD ^D ^D ^D 00 ^D CD Q) 00 ^D 00 CD OO CD

^0 00 C35 ^^5 00 CD 00 00 ^^5 ^^5 OO CD ^D C^^

t } f ( t 1 I I i I f I I I I i I I i t I I iii ij*>j>«iMii«»iiiH*niiiiHiHiiiii iiiiiHiiiiiiiitiJUiUJtiJ

mmCM^^JJ^-M-OOM-SCMCMCDCO-^M^CVlin-— ODCVJVDOO

00 f«0 OS fO fO M) M* CM CM ro ro CM CM CM m^

CM VD

CD 00 00 OS 00 00 CD OCM OS OS CM 00 00 OS 00 00 c?k 00 00 CD CM OS 99 O) 00 «-« 00

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Cl £ roVDM>*^M5® 9CMM*fs-fv-CMmOMS-inOS<JS<JS® ^M'^OlnM•M'^-<MVO*^^

^"4 ^4 fO ^ii4 24 ro—*M> 'M* fO in 4“ ro CM M5 to m 94 4 CM OS in 4 4M

V

> 9 9 9 9 99 9999999 99 99 99 99 in 999 in 9 9 9 9 9

a ro ro M- IS. CM CSJ rr M" «-• CM r) IX 4 4 CM CM 4 in 9 os CM ro 9 4

X 0 OJ CM CNiro rorom in MD rs- IX r- rx 9 9 OS OS OS OS OS os 9 9 9 9 9

OCA CM CM CM CM PO

> O o. a. <2i O X 2; xoa.ciso oC2iO 22 a. o<2l <2k 22 2C crs z 9Ui O z X 9A

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• c 9 00 00 00 CO 9 CD coco 900 00 9 9999 9 9 99 999 9 9 9 99 9 9

cf •—• «-4 *«p-4 -v-( »"4 'V-l ^^4 ^4

i. O o o o oo»-> OC-> oooCJ CJ o OO CJ O CJ CJ CJ oCJ CJ CJ O o o CJ CJ

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CL -J _1 _1 _J _J _l _i -J-J _i 99 9 9999 9 99 99X X X X X
Table

III-7.2

Activation

Energies

of

Migration

of

n-Dotriacontane

o

z

d

u

o ^a>©^0VDir>v0©ir>rvr*>fw>^vorocDrw

LUC mr- ®-»r to a> ®m '»r lo rw ro \ ^4 fK/ «>« CU # Wi4 «h4 «iM “)

^<Ti f'- ^^<7^ ®05 G? ®®<Tk ^v. C7> 09 *03 09 09 ^9 G9 *^9 09 09 09 ^9

irt ©©©©©©©©©©©©©©©©© O \ i I I I f I I I I ( < ( ( ( I i I •^U(M LULULULULUUJLULUUiLUU^lUUilUUJLUUJ

dt z fwo^ti>io-^*^<T»©®rwfwfoiro>rofor?

u •••••••••••«•»•«•

oj <M *p^ fo cvj <vj ro lo

^cj cvj

O CVi <XJ ®CVJ <VI c\| OJ W<VJ ©<M C^i CVJ C9 <VJ

«ii4 Wi« 09

M C9 ^9 09 09 ^9 Q9 49 09 G9 09 ^9 09 09 09 09 09 ^9 Q\ t < I I I 1 I I I f I < f I I I ! rO CV LULULULJLULULULULULULULULULUUJUJLU

Ci z OD'Tror^tn'^^tn<yjtnxTtimn^'^’^a)

u .••••••..«•..•••• rw ro cu ©^© ro vi> 0^1 iM ctj -i-4 cr>

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CO

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O ZOLUZOI— I— inOUiXO»-OLUX

CO OS

(=o

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.NT .V •'>? -V -V .V .s.? .'vT .V .X- .X* -X" .X“ -X'

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Q_ CDcniXiOQaicQi:DLn_j_j_i_/_jti_a-Qua.

l^.C32

TB

2960
Poly

MicjrQTit

Solv

Sample

D30

D60

E

E

Solv

cn2/s

kJ^'mol

kcal.^'wc

r«><5><D^i>rwvr)i<7if^roa>^CD'^a>oDro(TkOS—•a>^roQ>mcvjcM<90>osa>CD

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CJ ro ^O VO '4’ 9i CVi VO 07 ®f*> CD VO VO <M Cil CVJ ®OS ® ^ CVJ (M ®® ® ro — oioi wf^oo<^<>i <M 4. 4. CM CM ro ro in m in ro OS CM CM r<-

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<Ni CVi <VJ on <Vi Oi Oi CViOl Ci <M<V<<MCVKM CM CM CM CM CM CM CM CM CM CM CM CM CM CM CM CM

o Q- Q. oO Q-O. xxmoox Q.Q. Q. oO X 2; Q. z -r- ffi 0

z

Ui Q. 0

o Ui X X 1— O UJ XX oo»— XOUJ UJ XX 1— <_> Ui Ui X 00»- <x in

CJS X C7

>— »— h- —1— »— H* 1— !—»—»— *— f— »— 1— I— “ — — »— »— »— H“ H- X X X X X X X XX xxxxxx X XX X XX X XX X X X X HZ X X

m CQ CD OQ 07 177 OQ 07 07 07 07 CQ CQ mmCD CD CQ 07 07

•V .V .V .ST .sr .sr N.® -v.v-v.v.'c.sr .sr.s? .V • >? .NT .V .V .sr .Sf .sr •N* •V .s? .Sf •V

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UJLUUJllJLULULULiJLxJUJLLlliJL£iUJLiJLLiUJUiUiLLlLLlLLiLiJlJJLiJLLilJJUJLLlUJ

a.a-Q.CL.u-Q_a.a.Q_ciLa.a_a.Q.a-i7.Q.a.Q.a.i]L.a.a.ii.a.Q-a.Q-CLa.a. _j_j_j_i_j_i_j_j_j_i_j_{_jcoa7GQa7a7CDCDa7a7ma7a7a7i]Qa7m-ja.
01'-:BHT

EN

2720

6.2E-012

9.6E-010

^-TKCCO

Q5 «>5«-4 <D<DO

I f I iLfUJUi

r-wQo

09wr>

0&

<S 09 f 1 I 111 liHfl r^mo

• 9 • •^mro

*S> fl>G> ro^oo

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r\j<vj<Nj

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X»“<I

H-V-h- XXX

CQCQOQ

.Nr.y.v

O G><5>

Q. 0. 0. 0- 0. 0. Q.X
I
may be used as the starting value in a reiterative numerical computation.

Equation (1) converges rather slowly, at small value of T, ihus a

sufficient number of terms must be used to avoid premature termination

of the computation. At T << 1, approximately terms are

required to reach a reasonable precision. The following approaches

may be used to simplify the computational effort depending on the

conditions and ranges of applications.

Simplified Computation

At small values of a(<<l), a master curve of the quantity M^/(l+a)M^5

which is equal to for absorption or extraction, as

a function of T/a may be constructed from equation (1). However, by

limiting the computations to 0.1>T>0.001, the number of terms required

may be limited to about 5 at T'^^O.l and about 45 at T'^^0.001 for reasonable

« accuracy. The values of M^/(l+a)M^ at small a, but at the same T/a^,

are equal to the values calculated for large a. The results of this

selective computation deviates from the more rigorous and tedious computations by about 0.001% at T'^^0.1, and much less than 0.001% at lov«/er

T values.

The diffusion process may be divided into three regions of T:

Region I, T<0.1. The system is far from equilibrium, M^/(l+a)M^

2

IS a function of T/a only.

Region II, 5>T>0.1. The system is approaching equilibrium and

detailed computation must be carried out for different a values (only 2

to 6 terms are required for equation (1) in this region). For a<<! and

T/a^>10^, M^/(l+a)M^ = 1 - a/(7rT)'*^^ before reaching equilibrium.

Region III, T>5. For all practical purposes, equilibrium has been

reached with the deviation 6 = l-M./M < lO'"'", where M = M /(1+a) for

t — 00 so II-7
the case of absorption and = Mp^a/(l+a) for the case of extraction.

For a<l, equilibrium may be reached much earlier.

Computation for Migration into Infinite Media

When a-^, spP’^osches a limit, and equation (1) can be reduced

to a function of T only: m = i - 2 E -S exp (-q^T) (2)

t' oo , q^ ' ^n

n=l ^n

1 /2 where q^ = (n-l/2)Tr. For T<0.1, M^/M^ is a linear function of T .

M^/M = 2(T/tt)^'^^ = 1.128379 (3)

Deviations of equation (3) from equation (2) is less than 10~^^ at

T<0.05, about 10~^ at T = 0.1, about 5 x lO"^ at T = 0.2 and becomes

much greater than 0.01 at T = 0.3 or higher.

Alternate Approximation

An alternative form of the solution^^^

2 M./M = (1+a) [1 - e^^"" erfc(T^'^^/a)],

z °°

may be used in some cases and is relatively simple to compute. One of

the rational approximations^^^ for the error function yields the following

5 ^ M/(l+a)M^ = 1 - s a + £ (5)

^ n=l

^

where t=1/(1+0. 3275911 T^^^/a), a^=0. 254829592, a2=-0. 28449636, a 3

=l .421413741

,

a^=-l. 453152027, a^=l . 061 405429, and U|<u3l.5 x 10"^.

At a<<l, results computed from equation (2) or (3) deviates less

than 0.0001 from that of equation (1) at T/a^<5 or at M^/( l+a)M_^<0. 75.

0

Maximum deviation of 0.0035 occurs at T/a 'V'500 or at M^/(l+a)M^'^^0.97.

Therefore, equation (4) or (5) may be used to generate the master curve

for equation (1) at T<0.1 (Region I). However equations (4) or (5) do

not yeild any information about the region approaching equilbrium at

larger values of a, and hence should be used with discretion.

II-8
By combining Equation (4) or (5) at T<0.1 (Region I) and

Equation (1) at T>0.1 (Region II and III), computational requirements

for the solution of the diffusion equation between a plane sheet and a

well stirred liquid may be reduced to a minimum.

Diffusion coefficient at any point may be estimated from the above

computation method by means of regression.

Effect of Swelling

The diffusion coefficients in the tables are calculated based on

the original measured thickness of the sample, which is also given in

the tables. The final sample is usually swollen with solvent. For

volatile solvents, the absorbed solvent will leave the polymer soon

after the sample is taken out of the extracting solvent. In these

cases, the final sample weight is determined immediately after the

surface of sample has been wiped free of the solvent. The dimensions of

the final sample are generally not measured, however they may be estimated from the amount of solvent absorption by assuming an isotropic

expansion. The diffusion coefficient may be adjusted to reflect the

increase in the thickness as follows:

0 „ 0

= 0

0

ri . ^

1-Sf Pj

where 6^ = (W^-W^)/W^. D, L, V, M and p are the diffusion coefficient,

thickness, volume, weight and density respecti vely . The subscripts o,

f, and s denote the original polymer, final polymer and solvent respectively. The sum of fractional weight increase 6^ and the fractional

decrease in weight due to the migrant loss is given also in the table

and indicates the weight percent of solvent content in the final sample.

Therefore, the diffusion coefficients based on the final sample thickness

II-9
are increased from those based on the original thickness by approximately

the same order of magnitude as the increases in weight.

II-IO
Table II-l

Characteristics of Polyolefin Samples

Linear Branched Iso tactic

Polyethyl ene Polyethyl ene Polypropyl ene NBS-SRM 1475 NBS-SRM 1476 Pro-fax 6301*

Molecular Weights M

n 18,310 (GPC)

M

w 53,070 (GPC) 290,000

Mw 52,000 (LS)

M /M 11 w n Limiting Viscosity CN 0.890 0.8132

Number

TCB 1.010 ^.9024

[n],dl/g

DHN 1.180 1 .042 2.1

Melt Flow

Rate, g/1 0 min

2.07 1.19

3 Density, g/cm 0.97844 0.9312

Isotacticity, % 95-96

GPC -- Gel Permeation Chromatography

LS -- Light Scattering

CN -- 1-chloronaphthalene

TCB -- 1 ,2,4-trichlorobenzene

DHN -- decahydronaphthal ene (Decal in)

t [n] = 130®C for polyethyl enes, 135°C for polypropyl ene

Melt Index by Procedure A, ASTM Method D 1238-65T, Test Condition D, 190°C,

load 325 g for SRM 1475 and 1260 g for SRM 1476.

Density by ASTM Method D 1505-67; sample prepared by Procedure A, ASTM

Method D 1928-68.

Isotacticity is determined as fractional insoluble in Decal in at room temperature

after the entire sample has been dissolved at 160°C and allowed to cool.

Certain commercial materials and equipment are identified in this papger to

adequately specify the experimental procedure. This identification does not

imply recommendation or endorsement by the National Bureau of Standards, nor does it imply that the material or equipment identified is necessarily the best

available for the purpose.
Table II-2

Characteristics of Ethyl ene- Vinyl Acetate Copolymers

Designation Vinyl Acetate

Content %

M

n M

n Melt Index

g/10 min

Density

g/cm^

Petrothene

NA294-00

5.1 15000 89300 1.9 0.925

Ul trathene

UE657-00

13.4 18700 1 03000 0.46 0.935
Table 1 1-3

Characteristics of Radioactive Tracers

yC^./mg ng/25 dpm

14

'’'’'18*^38"'' 86.0 0.13

13.3 0.83

n-C32H56-16.17-l^C 45.5 0.25

3,5-di-tert-butyl -4

hydroxytol uene-7-*‘*C

(BHT)

57.9 0.19
Table II-4

Solvent Temperature Method

CO o

r— X XI 0^ X

-J o

o

10, Corn Oil (CO) 24, 24°C 0, Limited Solvent Volume (L)

20, Ethanol (EN) 30, 30°C 1, Unlimited Solvent Volume (U)

40, 40°C 2-8, Duplicate (or Renewed

Extractions

21, 10% Ethanol (.1 EN) 60, 60°C 9, Absorption Experiment (A)

23, 30% Ethanol (.3 EN)

25, 50% Ethanol (-5 EN)

27, 70% Ethanol (.7 EN)

29, 90% Ethanol (.9 EN)

30, n-Heptane (HP)

40, n-Octadecane (OD)

50, n-Octanol (ON)

60, Tributyrin (TB)

70, Trioctanoin (TO)

80, Water (AQ)

90, HB307 (HB)

Synthetic Triglyceride Mixture

95, 95% Ethanol (.95 EN)

Letters in paratheses are abbreviations used in tables.
Table II-5

Nominal

Sample Cede

xlO^

Polymer Migrant Migrant Cone. ,% Sp. Act.

yCi/

g. Polymer

Thickness

cm

1 LPE o

—

1

00 0.64 2.1 0.072

2 LPE C18 0.63 2.2 0.019

3 LPE Cl 8 0.013 1.6 0.070

4 LPE C18 0.01 0.96 0.020

5 LPE C18 5.2 0.14 0.084

6 LPE Cl 8 5.5 0.13 0.027

7 BPE C18 0.85 0.020 0.064

8 BPE C18 9.8 0.23 0.066

9 BPE C18 0.85 0.17 0.057

11 LPE C18 0.009 1.1 0.263

13 BPE C18 0 0.064

14 LPE Cl 8 0 0.064

15 BPE C32 1.86 93. 0.064

16 BPE C32 2.26 113. 0.028

17 BPE C32 0

18 LPE C32 0

19 LPE C32 1.0 5.2 0.059

20 LPE BHT 0.0062 3.6 0.060

21 LPE BHT 0.0069 4.0 0.025

22 LPE BHT 0.0072 4.2 0.027

23 BPE BHT 0.0052 3.0 0.061

24 BPE BHT 0.0030 1.8 0.028

25 BPE BHT 0.0045 2.6 0.027

26 LPE BHT 0.0095 5.5 0.025

27 PP BHT 0.0029 1.8 0.027

28 PP C18 0.82 4.9 0.027

29 PP C32 0.97 5.3 0.027

30 PP Cl 8 6.8 0.16 0.028

31 E-5% VA BHT 0.0091 5.3 0.029

32 Z-13% VA BHT 0.0057 3.3 0.069
References

1. Sanchez, I. C. , Chang, S. S., McCrackin, F. L. and Smith, L. E.

"An Evaluation of Existing Models Describing the Migration of

Additives in Polymers," NBSIR 78-1499, 1978.

2. Smith, L. E., Sanchez, I.C., Chang, S. S. and McCracking, F. L.,

"Models for the Migration of Paraffinic Additives in Polyethylene,

NBSIR 79-1598, 1979.

3. Smith, L. E., Sanchez, I. C. , Chang, S. S., McCrackin, F. L.,

and Senich, G. A., "Models for the Migration of Additives in Polyolefins," NBSIR 79-1779, 1979.

4. Smith, L. E., Chang, S. S., McCrackin, F. L., Sanchez, I. C. and

Senich, G. A., "Models for the Migration of Additives in Polyolefins," NBSIR 80-1999, 1980.

5. Smith, L. E., Chang, S. S., McCrackin, F. L., Senich, G. A. and

Wang, F. W. , "Models for the Migration of Low Molecular Weight

Additives in Polyolefins," NBSIR 81-2264, 1981.

6. Smith, L. E., Chang, S. S. and Senich, G. A., "Migration of Low

Molecular Weight Additives in Polymers," NBSIR 81-2314, 1981.

7. Crank, J. "The Mathematics of Diffusion," Oxford University

Press, 1975.

8. Abramowitz, M. and Stegun, L. A., "Handbook of Mathematical

Functions," AMS 55, National Bureau of Standards, GPO, 1964.
III. Results of Polyolefin Extraction Experiments

The results of extraction experiments are summarized in Table III.l

through III. 3 for the extraction of n-octadecane, n-dotriacoFItane and BUT

by triglycerides, ethanol, n-octanol , ethanol/water mixtures, n-heptane,

n-octadecane, and water.

The tables provide information on the test pieces as to their

weight, thickness L, exposed area A, specific activity of polymer,

amount extracted at the end of experiment the amount of solvent

retained in the final sample and the observed maximum of the diffusion

coefficient.

The value for in the tables is the final fraction of total

additives migrated at the end of the experiment. It may be either an equilibrium

value or a non-equilibrium value after a long time (6 months to one

year) lapse. In the case of BHT experiments, most of the values for

migration into good solvents denote the available fraction of BHT in the

sample, which varies with the conditions underwhich the sample was

prepared. Therefore, in calculating diffusion coefficients for samples

containing BHT, an adjusted is assigned to each sample according to

the equilibrium values observed in the good solvents. For the

case of '^^ 22^55 polypropyl ene or other samples which exhibit surface

blooming of migrants, the total amount of migrant is also adjusted for

the amount of migrant on the surface, before diffusion coefficients

calculating from it.

Tables III-l through III-3 summarize the experimental results

arranged by migrant or additive and then according to the type of polymer,

additive concentration, sample thickness, and, finally, solvents and

temperature. In order to provide easy cross-references , Tables III-4

III-l
through I I 1-6 sumnarize the experimental results which are arranged

first by solvent and then by additive and other parameters.

The activation energies, E, calculated by a simple Arrhenius

equation:

D = A exp (-E/RT)

are given in Table III-7.

III-2

I
IV. Loss of BHT from Polymers in Ambient Atmosphere

ADL, Inc. had reported through private communications concerning

the high volatility of BHT from their samples. When we examined our

observed total BHT contents from various experiments over all/2 year

period on a branched polyethylene sample, code 25, containing 45 ppm of

BHT, we found a rather noticeable trend of decreasing radioactivities as

a function of starting date of the experiment, Figure IV-1, although the

sample plaque was always wrapped in aluminum foil except during short

periods when pieces were cut from the plaque.

The volatility of BHT is further indicated by the following experiment. A piece of E-13% VA copolymer containing 60 ppm of BHT

(sample code 32), 61 mg in weight with about 2 cm of surface area, was

placed in a sealed 20 ml vial. The bottom of the vial was kept at 30°C

and the vial cap at 22-23°C. After 63 hours it was found that the

aluminum cap liner had a radioactivity of 0.51% of the test piece and

the glass wallof the vial had a radioactivity of 0.95% of the test

piece. Thus in a relatively short period, 1.5% of the BHT was sublimed

from the test piece at rather low temperatures in a closed vessel.

A further test was performed on both sample plaques 25 and 32.

Four pieces were cut from each of the sample plaques. These four pieces

were subjected to the following tests:

(A) The test piece was dissolved in o-xylene to check the current

specific activity.

(B) The test piece was extracted immediately by ethanol at 60°C for

three days. The residual specific activity and the activity of

the extract were recorded.

(C) The test piece was suspended in a ventilation hood at room temperature for three days before procedure (B) was performed.

IV-1
(D) The test piece was placed in a vial. Forced air was blown into

the vial for three days at room temperature before procedure (B)

was performed.

The results of these tests are presented in Table II-l. The test

pieces A and B were used as controls. Apparently 30 to 50% BHT is lost

from thin sheets of BPE or E-VA copolymer in mobile air at room temperature

for three days. The specific activity of sample code 25, BHT in BPE,

at the time of these tests was only 50% of the original specific activity

of 2.8 viCi/g polymer, determined 16 months earlier.

These experiments and our prior experience indicate that; (1) the

amount of additive remaining in the polymer after processing to produce

plaques is a fraction of the additive mixed into the raw polymer, (2)

for certain reactive additives, only a fraction of additive in the

polymer may be extractable, the rest may be chemically bound to the

polymer, (3) the total activity of the test pieces should be checked for

each experiment not only to measure the uniformity of the additive

concentration but also to measure the change in additive content as a

function of time. Therefore reports which the results are normalized to

the amount of additive supposely added to the polymer or to the total

amount of additive present in the polymer when it was manufactured,

without paying further attention to the amount of additive either

reacted or lost, may yield seriously incorrect kinetics of migration.

IV-2
Table IV'l

Percent of Original

Sample Code Test Piece

Specific Activities, pCi/g polymer

Residue Total

Activity

(Average of A + B)

A

-- 1.28 100

25

BHT in BPE

B 0.042 1.30 100

C 0.053 .93 72

D 0.052 .89 69

A 3.29 100

32

B 0,.077 3.45 100

BHT in E-13% VA

C 0.081 2.18 65

D 0.068 1.49 44
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IV-1

Loss

of

BHT

from

Sample

25,

BHT/BPE
V. Migration of BHT from Ethylene- Vinyl Acetate Copolymers

Ethylene-vinyl acetate (E-VA) copolymers of relatively low vinyl

acetate contents have been used in increasing quantities in recent years

as food-contact polymer films. The migration of the antioxidant BHT

from two copolymers having 5 and 13% vinyl acetate content into corn

oil, anhydrous ethanol, 95% ethanol, water and n-heptane was observed

14 with C- labeled BHT. The characteristics of these polymers were shown

earlier in Table 1-2. The characteristics of the additive BHT were

presented earlier in Table 1-3. The sample plaques were prepared in

similar manner to those of polyethylene and polypropylene samples described earlier, except that lower molding temperatures were used for the

E-VA copolymers. The E-5% VA and E-13% VA samples were designated as

plaque 31 and 32 with thickness of 0.027 and 0.068 cm and BHT contents

of 9 and 57 PPM, respectively.

The results for individual extraction experiments are summarized in

Table V-1. E-VA copol,'/mers absorb a fair amount of solvents as shown in

the table. The listed values are fractional weights of solvent contained

in the final sample. Thus for experiment 3230600, the final sample

contained n-heptane amounting to about 120% of the original weight of

the polymer. The 12% corn oil content for sample 3210600 is higher than

all other corn oil experiments.

The results of all extraction experiments for individual E-VA

copolymers are shown graphically in Figures V-1.1 through V-1. 4 for the

migration of BHT from E-5% VA ao 30 and 60°C, and from E-13% VA at 30

and 60°C, respectively . There are three illustrations for each figure,

2 i.e., (A) M^/Mq is plotted against t/L in a log-log plot to indicate

the migration behavior over several orders of magnitudes in both M^/M^

and time, (B) M^/M^ is plotted against t ' /L for the short time region

V-1
to indicate the behavior observed during fast extractions, and (C) M^/M^

1/2

is plotted against t

' /L for the entire length of time of experiments.

From both Tables V-1 and Figures V-1, the residual BHT content in

the 5% vinyl acetate copolymer samples, code 31, at the end of extration

are seen to vary from 7 to 12%. It is estimated from graphical extrapolation

that approximately 7-8% of the original BHT content is not extractable

even by good solvents, such as n-heptane. Almost all of the BHT content

in the 13% vinyl acetate copolymer is extractable. The 5% water content

in 95% ethanol has no noticeable effect on the BHT extractabi 1 ity for

the copolymers. No partitioning of BHT was observed between the copolymers

and solvents such as n-heptane, corn oil, anhydrous ethanol and 95%

ethanol, due to the near-complete of extraction of all available BHT

from the copolymers by these solvents.

Figures V-2.1 through 5 show the migrational behavior of BHT from

E-VA copolymers into various solvents, n-heptane, corn oil, ethanol, 95%

0 ethanol and water. These illustrations offer comparisons of behavior

among different E-VA copolymers and/or at different temperatures of extraction.’

In a more concise comparison of this behavior, the apparent maximum

diffusion coefficients of the swollen polymers are listed in Table V-2

together with the activation energies for diffusion. In all cases

except water, the diffusion coefficient for the 13% vinyl acetate copolymer

is about 2 to 3 times greater than that for the 5% copolymer. Increasing

in the temperature from 30 to 60°C generally increases the diffusion

coefficient by 10 to 20 fold, although the changes for the solvent nheptane are only on order of 4 to 6.

The diffusion coefficients in 95% ethanol are only slightly less

than those for anhydrous ethanol, about 10-15% less for 5% vinyl acetate

copolymers and about 25-45% less for 13% copolymer. Both diffusion

V-2
coefficients for experiments in anhydrous ethanol and 95% ethanol are

greater than those for corn oil by similar magnitudes.

The migrational behavior of BHT from the two E-VA copolymer into

water is rather unusual, as can be seen in figure V-2.5. The log

versus log (t/L ) representation in Figure V-2.5 is changed for Figures

1 /2 V-3.B and V-3-C into the more familiar versus t representation.

Figure V-3-B is the short-time portion of Figure V-3-C which covered the

entire time scale of experiment. These results indicate that the

migration of BHT from E-VA copolymer into water occurs in two distinct

stages, and that in contrast to the observations for other solvents, the

diffusion coefficients of BHT from E-13% VA copolymer are slower than

those from E-5% VA copolymer in the first stage. In the second stage

the diffusion coefficients from E-13% VA are apparently approaching

those from E-5% VA and can even surpass the latter when the time of

experiment is lengthened to allow equilibrium extraction.

In the first stage, 10-50 hours, approximately 15% of the BHT from

E-5% VA copolymer and about 1% of the BHT for E-13% VA copolymer, were

extracted by water before the release of BHT levels off into a second

stage behavior. It has not been determined whether the second stage of

extraction, with its distinctly different diffusion coefficient, is due

to the distribution of BHT in phase-separated regions of the copolymers

or due to the reaction of water and BHT over prolonged periods.

Another plausible explantion for the two stage behavior would be

surface blooming, or a very high migrant concentration near the surface

layer, although the time lapse of 10 to 50 hours seems to be longer than

usually needed to remove migrant from the surface or surface layer. By

extending the second stage behavior to t=0, one may estimate from

V-3
Figure V-3-B that there might exist surface blooming of BHT amounts to about

7.5 and 11% for the E-5% VA copolymer and 0.6 and 0.57% for the E-13% VA copolymer, for 30 and 60°C experiments, respectively.

The diffusion coefficients presented in Table V-2 were calculated by

* first adjusting the original loading, M^, to the available BHT, M^, when

necessary. The first stage diffusion coefficients were calculated based on

* the above mentioned percentages for By substracting the first stage

M^, normalizing and then applying equilibrium partitioning when applicable,

the second stage diffident coefficients were estimated.

Equilibrium partitioning of BHT between the copolymers and solvents

was observed only for the case of E-5% VA and water at SO'^C. In all other

experiments with water, a time lapse of six months was not long enough to

establish an equilibrium conditions.

V-4
Migration

of

BHT

from

E-5%

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Copolymer

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Table V-2

Diffusion Coefficients and Activation Energies of

Migration of BHT from Ethylene- Vinyl Acetate Copolymers into Various Sol vents

D (10 ^ cm^s

max

^ E

"1 30°C 60°C kj mol

Sol vent E5%VA El 3%VA E5%VA El 3%VA E5%VA E13%VA

n-Heptane 14 30 57 180 39 51

Corn Oil 0.15 0.37 2.3 4.9 76 72

Ethanol 0.19 1 .0 3.7 10 83 .65

95% Ethanol 0.19 0.55 3.2 7.5 82 73

Water - 1st Stage 0.0046 0.00007 0.005 0.00034 67 44

2nd Stage 0.000096 0.000023 0.0028 0.0010 94 106
Figure V-1 . 1 -A, B, C

Figure V-1 . 2-A, B, C

Figure V-1 ,3-A, B, C

Figure V-1 .4-A, B, C

Migration of BHT from E-5% VA Copolymer at 30°C

Migration of BHT from E-5% VA Copolymer at 60°C

Migration of BHT from E-13% VA Copolymer at 30°C

Migration of BHT from E-13% VA Copolymer at 60°C

Legends for Figure V-1.1

Corn Oil

* Ethanol

95% Ethanol

n-Heptane

Water

A

o

0

+

*
Figure

V-l

. 1

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niGRATlON

OF

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FROM

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ACETATE

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200

400

600

800

1000

1200

1400

1600

1800

2000

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MIGRATION

OF

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FROM

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MINYL

ACETATE

COPOLYMER

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400

500

600

700

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Figure V-2.1

Figure V-2.2

Figure V-2.3

Figure V-2.4

Migration of BHT from E-VA Copolymers

Migration of BHT from E-VA Copolymers

Migration of BHT from E-VA Copolymers

Migration of BHT from E-VA Copolymers

into n-Heptane

into Corn Oil

into Ethanol

into 95% Ethanol

Legends for Figure V-2

E-5% VA

30°C +

60°C X

E-13% VA

o
MIGRATION

OF

BHT

FROM

ETHYLENE-MINYL

ACETATE

COPOLYMERS

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Figure

V-2.3

MIGRATION

OF

BHT

FROM

ETHYLENEMIHYL

ACETATE

COPOLYMER

into

ETHANOL

•»-» o ®

X so

t/L2,

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BHT

FROM

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ACETATE

COPOLYMER

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95^

ETHANOL

u>

G>

O IG>

N. o

t/L2,

h/cn2
Figure V-3 A, B* C Migration of BHT from E-VA Copolymers into Water

Legends

E-5% VA E-13% VA

30°C + O

60°C X
Figure

V-3-A

MIGRATION

OF

BHT

FROM

ETHYLEHE-UINYL

ACETATE

COPOLYMER

INTO

MATER

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1
VI. IGC Determinations of the Relative Diffusion Coefficients of Several

Probes in Linear Polyethylene

Inverse gas chromatography (IGC) studies on the determination of

diffusion constants in polyethylene were reported in the previous annual

report [1]. These findings indicate that while accurate absolute diffusivity

measurements seem beyond the reach of the IGC method, the possibility

exists for using the technique to rank the relative ease of diffusion of

many probes in a given polymer. A calibration of a specific column can be

accomplished by conducting experiments with a probe-polymer combination of

known diffusivity to calculate the mean polymer layer thickness from the

measured peak broadening. The same column can then be used under similar

operating conditions to determine other probe diffusivities and a relative

ranking of many probe diffusion coefficients can be established. Experiments

on several series of compounds have been conducted and those for whifh the data

analysis and reduction have been completed will be used to illustrate the

procedure of relative diffusivity determinations. Preceding this discussion,

however, will be: a review of tne theory for determining absolute diffusion

constants from IGC studies, a summary of results from polyethylene-octadecane

experiments to be used in the relative diffusivity determinations, and a

section giving experimental details on the relative diffusivity measurements.

A Review of Pertinent Theory for IGC Absolute Diffusivity Determinations

The probe or migrant injected onto a chromatographic column resides

partly in the carrier gas and partially in the polymer or stationary phase

during transit through the column. Diffusion of the probe vapor in the gas

phase can occur parallel to the background flow of carrier gas sweeping the

vapor through the column both in the direction of and opposed to the carrier

flow. This longitudinal or axial gaseous diffusion process causes an increase

VI-1
in width of the eluted peak over its initial injection distribution. An

additional gas phase peak spreading mechanism originates in the multiplicity

of path lengths possible around the packed support particles and leads to

an associated broadened distribution of elution times. Peak spreading can

also be attributed to diffusive processes in the stationary phase. If the

carrier gas flow rate is very rapid, steady-state partitioning of the vapor

between the gas and stationary phases cannot be established. The residence

time in the stationary polymer phase is then influenced by both the diffusivity of the probe in the polymer and the distance in the stationary phase

over which diffusion must occur, among other factors. The peak broadening

processes discussed above are commonly quantified by the convenient construct

of the height equivalent to a theoretical plate, H, which is related to the width

at half-height, Wy2

> eluted Gaussian-shaped peak as follows:

( 1 )

where L is the column length, and t^^ the retention time of the peak at the

maximum. The determination of these quantities from a Gaussian-shaped experimental chromatogram with a peak standard deviation of a is illustrated in the

schematic of Figure VI-1.

An equation attributed to van Deemter et al . [2] is often used to

relate H to the local carrier gas flow velocity, u, and is of the form:

H = A + B/u + Cu (2)

The A term arises from the number of possible gas paths through the column;

B is from longitudinal diffusion of the probe in the carrier gas; and C

originates from the resistance to mass transfer in the polymer or stationary

VI-2
phase. The coefficients in equation 2 are defined as follows:

A = 4Ar (3)

B = 2yD

* g

(4)

C =

8 s^k

0^(1 + k )2

(5)

where A is a measure of support packing irregularities, r the average

support particle radius, y a correction coefficient for constriction and

tortuosity of the gas flow path in the column, the probe diffusivity in

the gas phase, s the effective thickness of the stationary phase film,

the diffusivity of the probe in the stationary phase, and k the column

capacity factor commonly given as:

( 6 )

where t,^. is the time taken to elute an unsorbed marker material from the

column. Equation 2 indicates that, at large values of the flow rate, H will

be proportional to the flow rate. The probe-polymer diffusion coefficient can

then be determined from the constant of proportionality C by equation 5 i'" the

effective film thickness is known. Equation 5 is not applicable for columns

packed with glass bead support particles. In such cases of diffusion into a

uniform stationary phase film on a solid surface, a similar relation for C

appl ies:

2 s^k

C =

p (7)

3 D^(l + k)^

VI-3
While equation 2 gives a suitable explanation of peak spreading in

some cases, other results have raised questions about its utility, particularly when significant gas phase diffusion can occur. These discrepancies

indicate that the simplifications made by van Deemter in neglecting other

mechanisms of diffusion are not valid for all systems. Giddings and coworkers [3] examined several modified forms of the van Deemter equation and

found that none could account for the experimental results obtained on

columns of varying length and outlet pressure.

An aquation proposed by Jones [4] takes several additional sources of

peak spreading into consideration: resistance to mass transfer in the gas

phase normal to the carrier gas flow direction (D), carrier gas velocity

distribution effects (E), and a correlation between these two processes

(F). This equation is given as:

H = A + B/u + (C + D + E + F)u (8)

where C is as in equation 7 and

D =

r 1,2 2 S g

Og(l + k)'

E =

4C^

F = 46(CqC^)^^^ k r g

D (1 + k)

g

(9)

( 10 )

( 11 )

g being the diffusion path length in the gas, 9 the correlation coefficient

between the D and E terms, and and geometric constants.

VI-4
The radial diffusion 0 term was discounted by van Deemter and co-workers

in the derivation of equation 2 because of the much greater magnitude of

compared to D^. This simplification is valid for the thick liquid films used

in their work, studies of columns with roughly 0.3 mass fraction stationary

phase loading. The diffusion distances s and g are roughly comparable under

these circumstances. If low column loadings which reduce s to about O.Olg are

used, then the much larger probe diffusivity in the gas phase is overcome by the

ease of mass transfer through the thinly-spread liquid phase and the D term

cannot be ignored.

The E contribution to spreading arises from diffusion caused by differences in the velocity of the carrier gas in various parts of the column.

Velocity differences can arise from both short and longer range channels formed

by support packing irregularities and from trans-column effects caused by the

influence of the tube walls. These effects are summarized by Giddings [5]

who estimates approximate magnitudes for contributions of the many possible

velocity gradients combined in the E term of equation 8.

While the first three terms in equation 8 are independent of one

another, the D and E terms are not since molecules which have a lower

average velocity will spend a smaller fraction of time in the gas phase and

therefore not experience as great a percentage of gaseous diffusion as

2 molecules with higher than average velocity. The total variance, . , of

' 3 2 ? two such dependent contributors, a. and aJ , is given as:

2 - 2 ^2 ^ a. . = a. + a . + 20 . .a.a

ij ^ j 'J 1 J

( 12 )

where the correlation coefficient between the two contributors is denoted

as 6. The F term of equation 11 originates from the final term in the

above relation and corresponds to the interaction between the D and E

terms.

VI-5
Giddings [6] has given an expression said to account for all known

plate height terms contributing at least one percent of the total plate

height for packed GC columns in the absence of interfacial adsorption as:

The G term represents the contribution of column-wide velocity inequality

effects, such as that arising from column coiling, and could alternatively

be included in E. This equation is otherwise similar to equation 8 except

for its omission of the interaction term F, A compilation of the C, D, and

E coefficients expected to apply in various situations and a means of

calculating their magnitude from measurable column parameters is given in

reference [5].

The plate height equations discussed up to this point apply only to the

peak spreading in a short region of the chromatographic column where the

carrier velocity u is a constant local to that region. A final modification

can be made to equation 8 or 13 to account for the variation in local

carrier velocity along the column caused by the drop in pressure from

column inlet to outlet. The effect of this correction is primarily on the

liquid mass transfer term, as discussed by Dal Nogare and Juvet [7]. The

final expression for the dependence of the experimentally accessible column

average plate height, H, on the carrier gas outlet velocity, u^, is similar

to equation 8 and is given as:

(13)

H = A + — +

u + D + E + F + G u 0 (14)

VI-6
where and are the column inlet and outlet pressure. The gas phase

diffusivity found in equations 4, 9, 10, and 11 must also be restated at

the outlet pressure of the column. The form of this modification is based

on the relationship between the local column velocity and the average

carrier gas velocity. The preceeding treatment assumes a distance average

of this velocity. Other methods [3] involve the use of a pressure average

velocity and yield a slightly different equation for H but agree reasonably

well with equation 14 even at large values of the inlet pressure.

The magnitudes of coefficients in equation 14 and the configuration of

the polymer film on the surface of the supporting beads can have a significant

influence on the methods used in interpreting data derived from IGC determinations of diffusive peak broadening as discussed in the previous annual

report. These effects will be reviewed briefly for the experimental determination of the diffusivity of normal octadecane in high density polyethylene

considered there.

Summary of Previous Results for LPE-Qctadecane

As discussed earlier, IGC determinations of diffusivity in the polymer

phase are made from a study of probe peak broadening at varying carrier gas

velocities; a schematic illustration of the results is shown in Figure VI-2.

The local plate height and carrier velocity of equation 2 are commonly

replaced by the measured average quantities in experimental determinations

of column efficiency. Such H vs u plots for eight flow velocities in the

flow rate region from about 10 to 100 cm/s yielded a slope C for column A

of 7.05 ms with calculated standard deviation of 8.8 percent and 18.9 ms

with calculated standard deviation of 7.4 percent for B. The van Deemter

treatment provides for the calculation of the diffusivity of C,p in linear

VI-7
polyethylene from these C values by equation 7 when the polymer film thickness in each column is known. Such a procedure is proper only if the other

contributions to peak spreading discussed earlier are small when compared

to that arising from polymer or stationary phase mass transfer. This

assumption has been made in many previous studies of probe-polymer diffusion.

However, if the other gas phase kinetic processes are operating to a significant extent then the limiting slope at high flow rate of Figure VI-1 should

also reflect these contributions, as indicated by equations 8 and 14. It

was important, therefore, to estimate the relative magnitude of the gas

phase terms as compared to the stationary phase contribution to determine

if such a simplified data analysis procedure could be applicable.

A further consideration is the nature of the carrier velocity on which

the plate height depends. Equation 14 indicates that while the plate

height contribution of the B, D, E, and F terms are directly or inversely

proportional to the carrier outlet velocity u^, the C term contribution to

H depends on the average velocity. Consequently, the often-employed plot

of H vs average carrier velocity suggested by equation 2 will not be linear

at high flow velocity for any variant of velocity if both stationary and

gas phase mass transfer effects are nonnegl igible.

The estimated gas phase contributions to peak spreading were computed

for both columns and compared to the limiting slope C calculated from the

van Deemter equation least squares fit. It was evident that the peak spreading

attributed to gas phase diffusion made a significant contribution to the

overall kinetic broadening for column A. In instances of this nature, where

gas phase diffusion terms make a significant contribution to peak spreading,

difficulty can be encountered in deciding which are important and calculating

their values. Alternatively, it is possible to resolve the gas and stationary

VI-8
phase mass transfer contributions without directly estimating the magnitude

of the gas phase terms. Purnell [8] has suggested a method which involves

first determining A and B of equation 14 and employing these values to reduce

the experimental H to the peak spreading arising only from mass transfer

effects, H*. In terms of an equation:

HVu^ =

0 H - A

- C + D + E + F + G (15)

When the left-hand side of this equation is plotted against the pressure

correction 2p^/(p^. + p^), a jstraight line with slope C and intercept (D + E

+ F + G) should be obtained.; Evaluation of the constants A and B requires

that experiments be conducted over a wide range of carrier gas flow velocities.

[ Limited low velocity data often precludes experimental determination of

these constants in many cases; however, they can be estimated from theoretical considerations and experimental results. The multipath A term defined

in equation 3 has been determined to have a \ value between one half and

unity in many cases [9] and a value of 0.5 was assumed here. The longitudinal

diffusion B term most often has a y value near one [9] and unity was utilized

in the determinations. These values were used to calculate the A and 6

terms of equation 19 and a fit of HVu^ against the pressure correction

term gave a linear least squares line with a slope of 16.4 ms and calculated

standard deviation of 5.5 percent for column A and 21.9 ms with calculated

standard deviation of 6.6 percent for B. These results are compared to the

van Deemter fit slopes in Table VI-1 on the following page. The smaller standard

deviations of the Purnell method slopes compared to the correspond! ng values for

the van Deemter fit discussed earlier indicated the better applicability of the

Purnell method. The C value obtained by this method for column A was more

VI-9
Table VI-1

Comparison of the C Coefficient Determined by Two Methods

for LPE-Octadecane at 150 °C

Column Column Loading ^van Deemter ^Purnel

Code (Mass Fraction Polymer) (Eq. 2) (Eq. 15)

A 6.10 X 10*^ 7.05 ms 16.4 ms

B 5.71 X lO’^ 18.9 ms 21.9 ms

than twice that obtained from the van Oeemter analysis. This was attributed

to the latter's combination of the effects of polymer and gas phase mass

transfer in a nonlinear manner, which can be noted by comparing the C term

appearing in equation 2 to its complement in equation 14, the expression in

parenthesis. For the case of column A where the gas phase terms contributed

significantly to the peak broadening, the van Deemter equation-based analysis

underestimated the magnitude of C. Gas phase mass transfer effects for

column B contributed only slightly to the total broadening and this was

reflected in the similar results of the two mechods for determining C which

differed by only 15 percent, as indicated in Table VI-1.

While the method of determining the polymer phase mass transfer contribution can be important under certain column conditions, the most significant

parameter which affected the diffusivity determination was the distance over

which diffusion occurred. This distance is commonly identified with the

effective film thickness s of equation 7. It is often assumed that the

stationary phase is distributed as a uniform thin film over the entire surface of the spherical glass bead column packing. The effective film thickness for this geometry can be calculated from the expression:

VI-10
s (16)

2 Akt Np^

where M is the mass of polymer phase in the column, N the number of support

particles in the column, and the polymer density. Such a configuration

requires a high amount of stationary phase surface area, however, and a

geometry in which the stationary phase is confined by capillary forces into

annular regions around the contact points between support particle spheres

has been advocated as a means of minimizing the exposed stationary phase

surface area. This geometry has been observed for both low molecular

weight [6] and polymeric [10] stationary phases coated onto glass bead

supports and is illustrated schematically in Figure VI-3. A stationary phase

film may also be present on surfaces where the beads are not in contact, as

indicated in the inset. Its thickness, however, should be much less than

that of the stationary phase in the region of adjacent support beads.

The different diffusion path lengths expected for the two extremely

different polymer distributions described above can exert a significant

influence on determinations of polymer-probe diffusivity by IGC. Giddings [11]

has compared the contribution to peak spreading expected from a hypothetical

support coated with two regions, a thin film of uniformly adsorbed stationary

phase and a second region where the liquid stationary phase collects at the

support contact points. He concludes that for glass bead supports at mass

fraction loadings up to about 0.015, the bulk of the stationary phase is

present at the bead contact points and controls the plate height performance

by virtue of its greater thickness. An equation has been proposed [12] to

relate C to measurable column parameters for this geometry and is as follows:

VI-11
1/2

( 17 )

where p is the density of the support particles and the mass fraction of

polymer phase in the column. This treatment assumes that the spherical

support particles pack randomly and are surrounded by 6.25 nearest neighbors.

The relation for C is similar in form to equation 7. If the differing

variables are combined into an explicit expression for s in terms of the

particle size, the following relation is obtained:

This equation provides for the calculation of a value of s which, when

substituted into equation 7, yields a result for C identical to the C term

determined by equation 17.

A computation of s by these methods was useful for comparing the effective

film thicknesses of the two stationary phase arrangements considered.

The average film thicknesses calculated in the above manner for a polymer

stationary phase collected at bead contact points were much greater than the

thicknesses corresponding to the uniform layer geometry, as can be noted

from the following table.

(18)

Table VI-2

Effective Layer Thicknesses for Columns with

Differing Polymer Phase Geometry

Effective Layer Thickness, s(pm)

Column Code Uniform Thin

Surface Film

(Eq. 16)

Annular Film at

Contact Points

(Eq. 18)

A

B 0.043

0.404

5.58

9.77

VI-12
Both equations 7 and 17 were used to calcualte the diffusion coefficient of octadecane in HOPE. For column A assuming a thin uniform film,

was calculated from the C coefficient obtained with the Purnell treatment

-11 2

by substituting equation 16 into equation 7; a result of 3.8 x 10 cm /s

was obtained. Assuming a geometry where the polymer collects at the bead

contact points for column A, was calculated according to equation 17 and

-7 2 a value of 6.4 x 10 cm /s determined. These results and the corresponding

values for column B are summarized in Table VI-3 below.

Table VI-3

Influence of Film Geometry on the Diffusion Coefficient

of Octadecane in Linear Polyethylene at 150 °C

2 -1

Diffusion Coefficient (cm *s ) Column Code Uniform Thin Annular Film at

Surface Film Contact Points

(Eqs. 7 and 16) (Eq. 17)

A 3.8 X lO"^^ 6.4 X lO"^

B 4.1 X 10 2.4 X 10

^

It was evident that the uniform thin film geometry assumption led to unreasonably low values of the diffusion coefficient. In addition, an order of

magnitude discrepancy existed between results for the two columns. The assumption of a collection of the polymer stationary phase at bead contact points yielded

diffusion coefficients of reasonable magnitude for the temperature of the

experiment and col umn-to-col umn agreement within a factor of three. This

threefold difference in the diffusivity results may be attributed to the effects

of differing probe concentrations in the polymer phase of the two columns.

Diffusivity values are often quite sensitive to the concentration of

the diffusing species, depending approximately either linearly or exponentially

VI-13
on concentration [13]. In these IGC determinations the probe concentration

in the polymer film varied both along the column length due to increasing

peak broadening with transit time and with the depth of penetration into

the polymer film expected from Fickean diffusion. The diffusivity determined

was therefore a concentration-averaged value over all column conditions.

The actual concentration of octadecane in the polyethylene film was

estimated to range from 0.01 to 1.5 percent by mass for column A and from

0.001 to 0.16 percent by mass for column B. The diffusion coefficient

calculated from the column B results corresponded to probe concentrations

about an order of magnitude lower than for column A. This could account

for the lower value of probe diffusivity determined with column B. For

either a linear or exponential dependence of the diffusion coefficient on

concentration, the diffusivity should be less at lower diffusant concentrations, as found here. A determination of the functional relationship of

the diffusivity on diffusant concentration was not possible, however,

because of the variation in probe concentration along the column length and

the limited amount of data available.

Limited data are available in the literature on diffusion of the

higher alkanes in LP£; however, studies of similar diffusants, linear

aliphatic esters with 25 to 45 backbone units, have been conducted by Klein

and Briscoe [14]. Extrapolating their experimental results to an 18 unit

"6 2 chain leads to an expected diffusion coefficient of 5 x 10 cm /s in

linear polyethylene at 152 °C. This result is about an order of magnitude

greater than the IGC determinations for a polymer film collected at the

support bead contact points.

The distribution of film thickness also plays an important role in

/ determining the magnitude of the diffusivity. The previous calculations

VI-14
I assumed that the film thickness was constant. In an actual column, howevc

the film thickness would be expected to be distributed about the mean

values employed here. An alternate form of equation 7 can be used to

estimate the effects of different film thicknesses [15]. The equation is;

“s = C(1 + k) :t2 (19)

where

q^ is a configuration factor and x^. the volume fraction per unit

column volume of stationary phase segments with thickness s^. . Assuming a

uniform configuration factor and holding x^. constant gives:

D

s kqx

C(1 + k)^

( 20 )

which reduces to: I

( 21 )

for a uniform film of thickness s. For a distribution with an equal volume

of film 0.1s and 10s in thickness:

0^ = Z [5(0. Is)^ + 0.05(10s)^] = 5.05 Zs^ ( 22 )

This distribution, resulting from the same volume of stationary phase

present in the uniform thickness case, leads to a diffusivity value five

times larger than that corresponding to a uniformly distributed film.

Table VI-4 summarizes the effects of different thickness distributions on the

I diffusion coefficient 0^ compared t.g that expected from a uniform film of

thickness s, 0^. All the geometries considered require the same volume of

stationary phase per unit column volume and have an average thickness of s.

It is evident from these examples that thick sections of the polymer film

VI-15
Table VI-4

Effect of Thickness Distribution on Diffusivity

in the Polymer Phase

Thin Section

Depth

Thick Section

Depth DVD

s s

0.50s 2s 1.25

0.25s 4s 2.13

0.10s 10s 5.05

0.02s 50s 25.01

0.01s 100s 50.01

can exert a disproportionate influence and lead to a considerable increase

in the polymer-probe diffusion coefficient when compared to the value

calculated for an IGC experiment with an assumed ideal polymer layer of

uniform thickness. An experimentally difficult determination of the variability of the polymer film in the IGC column would be necessary in order

to correct the calculated diffusivity values for the actual polymer layer

nonuni formity.

Experimental Details

The column used throughout the relative diffusivity study was prepared

from glass support beads coated with a layer of the linear polyethylene (LPE)

NBS SRM 1475 and packed into a 6.35 mm outer diameter stainless steel tube,

as described in the previous annual report [1]. After installation in the

gas chromatograph, a final drying and column conditioning step was carried

out by purging with dry, deoxygenated helium followed by heating to 150 °C

for a 24-hour period. The column used is identical to column B in the pre-

-3

vious annual report and contains 5.71 x 10 mass fraction of LPE. It was

chosen because of the relatively small contribution which gas phase mass

transfer made to the overall peak spreading when compared to column A of

that report.

VI-16
Several alkane probes and an antioxidant were employed as diffusants

and are listed in the table below [16]. All were dissolved in hexane

(Burdick and Jackson Labs.) to give solutions of about 0.02, 0.2, and

2.0 percent by mass.

Table VI-5

Probes Employed in an IGC Study of Relative

Diffusivity in LPE

Probe Code Source

n-octadecane 00 I

1

(_) Supelco

n-hexadecane ^16 Aldrich Chemical

2-methyl pentadecane 2MeC^5 Alfa Products

2, 2, 4, 4, 6,8,8-

heptamethyl nonane 7MeCg Aldrich Chemical

n-tridecane 43 American Petroleum Institute

# l,3-di-tert-butyl-2- • hydroxy-5-methyl benzene BHT Polysciences

Approximately 1 pi of each solution was injected into the flash vaporization injector of a gas chromatograph, maintained at 180 °C. The column

oven was held at 150 °C ± 0.3 °C throughout. The eluted peaks were monitored

with a flame ionization detector (FID) held at 190 °C, whose signal at 10 A/mV

sensitivity was fed to an electronic integrator connected to a strip chart

recorder and to a high acquisition speed recorder-plotter. The former

setup was employed to time the peak maxima to within 0.01 min and for

manual measurements of the chart width at half maximum at chart speeds up

to 1 cm/s. Typical results are shown in Figure VI-4.

The rapid collection capabilities of the high speed recorder-plotter

allowed the FID output to be sampled at 10 ms intervals, facilitating analysis

VI-17
of the marker and solvent peaks. A typical trace is shown in Figure VI-5 for

five repeated determinations. Data collection was triggered upon injection

of the methane and hexane vapor sample and the time to the methane peak maximum, assumed to have k = 0, was employed to determine tj^ of equation 6 and to

calculate the column average linear flow velocity, u, from the expression:

u = L/t|^ (23)

The quantity of interest, the column outlet velocity, was then calculated

from *j as follows:

(Pi/P„)^

(24)

Column inlet and outlet pressures were monitored with calibrated pressure

gauges of appropriate range. The outlet pressure was very near to atmospheric

in all cases. The helium carrier gas volumetric flow rate was measured

with a soap film flow meter, when necessary. The data were collected over

a corrected flow rate range of about 1 to 5 ml /s.

The first derivative of a chromatographic peak with respect to time can be

used to aid in determinations of the maximum height and peak widths indicated in

Figure VI-1. At a point where the chromatogram is at a maximum, the first derivative will be zero while the second derivative is negative. Determination of the

first derivative zero point is illustrated with curve B of Figure VI-6, the

first derivative of curve A obtained by experiment. The inflection points of

the chromatogram are also readily indicated by maxima or minima in the derivative

curve. The magnitude of the derivative at this point gives the slope of a

tangent to the peak. The ratio of the absolute values of the derivative maximum

and minimum gives a measure of peak symmetry.

VI-18
For the purposes of this study, a symmetric peak is defined as that ha-'ing

a front to rear tangent slope ratio of 1 ± 0.2. The highly asymmetric peaks

that result from excessive probe concentrations or adsorption, two of the many

factors which can cause deviations from Henry's law in the chromatographic

column, are not amenable to analysis by the methods outlined here for

Gaussian-shaped peaks. The time period between maximum and minimum of the

derivative curve can be measured easily and is equal to twice the standard

deviation of the peak, as illustrated in Figures VI-1 and VI-6. The above

procedure was used to collect information on the center position, standard

deviation, and symmetry of the eluted diffusant peaks.

Relative Diffusivity Determinations

As noted earlier, the probes listed in Table VI-5 were studied in the same

LPE-containing column. This allows the diffusivity of one probe in LFE to be

compared to that of another, irrespective of the method of any calculation of

the absolute diffusivity of the probes in the polymer. The experimental data

acquired for tri decane in LPE is given in Table VI-6 and can be used to give an

indication of typical values of the various parameters utilized in these

determinations. The variables p., p , and t,. are used in the calculation of u

1 0 M c by equations 23 and 24. The plate height is determined from Wj and t^ with

equation 1 or from w^. and tj^ by the following expression:

When values of A and B are available, the plot suggested by equation 15 can

be constructed from the data of Table VI-6. The previous annual report [1]

contains a more detailed example of the calculation of these two constants

from equations 3 and 4 than the abbreviated discussion given here. The

« I values used in calculating H /u^ are given in a footnote to Table VI-6.

VI-19
Table

VI-6

IGC

Diffusivity

Study

of

Tridecane

in

Linear

Polyethylene

at

150

°C c

(TJ

i-O

(T3

<0 o

IT} C

O)E* 1“

i.

O)OlX

LU

VI-20 9i! iiIiiiIIPIIi
Plots of H /u^ against the 2p^/(p^ + p^) term are shown for five

diffusants in Figure VI-7. The slopes of these plots provide a value for the

C constant needed in a diffusivity determination, ^hese C values are

listed in Table YI-7, accompanied by the corresponding value of k for each

Relative Di ffusivi ty Results for

Table VI-7

Several Alkanes and BHT in LPE at 150 °C

Probe C (ms)±c(%) k±a(%) ^Probe °Probe^°C^g D (10^-cm^/s)

^18 21. 9± 7 119 ±3 0.38 Y 1 2.4

^16 7.3±14 60.911 2.05 Y 5.4 13

2MeC^3 8.7112 49.011 2.25 Y 6.0 14

7MeCg 18 ±11 12.811 3.74 Y 9.9 24

^3 12 ± 9 12.111 5.74 Y 15.2 36

BHT 9.9111 32.412 2.94 Y 7.8 19

probe as calculated from the data of Table VI-6 by equation 6. This information

can then be used to determine a value for the relative diffusivity by the

following procedure. Equation 17 can be rearranged to collect all the variables used only to characterize the polymer packing into one term and solved

for the diffusivity. The following expression results when this is done:

°s =

C(1 + k)‘

(26)

The first term in the above equation contains the variables which

characterize the interactions between the probe and polymer while the square

room term consists of variables which describe polymer layer and support

VI-21
particle characteristics only. These latter variables are constant throughout

all determinations with this particular column and this collection of

parameters can be abbreviated as the constant Y. The following version of

equation 26 is consequently obtained:

D. = p

• Y (27)

® C(1 + k)“^

This equation was used to determine the probe diffusivity values given in

the fourth column of Table VI-7. If one of the probes is selected as a reference, in this instance octadecane, the diffusivity of a probe in the

polymer relative to the diffusivity of the reference probe in that polymer

can be obtained from a ratio of the respective results from equation 27.

These values are given in the fifth column of Table VI-7.

An alternate determination of the relative diffusivity might be based

on equation 7. In this instance the following expression would be obtained

for D : C

D =

s C(1 + k)‘ 3 C(1 + k)'

Y' (28)

Equations 27 and 28 are identical except for the constants Y and Y , which

are derived from different collections of parameters used to describe the

distribution of the polymer phase on the support. The numerical front-factor

I for Y is identical to that given for Y in column four of Table VI-7 since it

depends only on the values of C and k, which are the same for either method.

I The relative diffusivity results would also be identical as the Y or Y

constant is eliminated by the ratioing method used to obtain this quantity.

An absolute diffusion constant for each probe in the polymer can readily

be obtained from the relative diffusivity values if an absolute diffusion coeffiVI-22
cient for any of the probes in that polymer exists. Taking the previously cited

-7 2

value in Table VI-3 for column B of 2.4 x 10 cm /s for octadecane in LPE

at 150 °C as accurate, the absolute diffusivities in column six of Table VI-7

were otained by multiplying the relative diffusion coefficients of column

five by this factor.

Future Results

Results on lower molecular weight alkanes, principally isomers of octane

and normal decane and tri decane, at temperatures below the LPE melting point

will be given in a later report. They will allow a more rigorous evaluation

of the IGC relative diffusivity technique as many more absolute diffusivity

determinations have been conducted with these compounds. Independent values

for the absolute diffusion coefficient of tri decane in LPE will then be available at two temperatures, one below^and one above the polymer melting point.

By using an appropriate activation energy to extrapolate one of the results

and making allowances for the expected effects of polymer crystallinity on

the diffusion coefficient, a direct comparison of the two results will be

possible. Unfortunately, it is not possible to study the alkanes from

octane to octadecane at a single temperature due to the great differences

in volatility among these compounds. This necessitates the temperature

extrapolation for a common probe described above as a means of connecting

the two bodies of data collected at different temperatures and allowing for

a critical evaluation of the method. Additional results for BHT at lower

temperatures will also be provided.

VI-23

Figure

VI-1:

Elution

chromatogram

schematic

showing

a

marker

peak

att^

and

Gaussian

probe

peak

at

tj^.

Various

methods

of

determining

the

standard

deviation

a

are

indicated.
Figure

VI-2:

van

Deemter

plot

of

the

height

equivalent

to

a

theoretical

plate

against

the

average

carrier

gas

flow

velocity.
c

toc

•rU)

<u

•r“(- •P

(Ue

0

O)O)

01 P

to o

x: CL

Q. a.

Z3 U U)

o;E -a

>> to r— <1> O P

a.

VA

0) (A I— to •—

•I— oi

lA

lA <0 o

a. oi

c

0) TjC C P •»-lO p p

o c

o

c u

o

•I- c P E

to 3

U r— P o

lA U

3

r— O r- C3

• « ro

I >

<uu

3

O)
4> SZ c

O) <u C O)

•rC 3 (TJ 0 +i

in T3c

(O

<0

<D e

Q. 3E

01 *r* ja X O rtJ «- e

Q.

<f- (O r—

rfl »4- SZ o

+j <TS 3

Q.J3

+J -•-> 3 T3 O ‘r-3 u

<U 01 a ja

t- -•-* ou o>

OJ c

i- *r-c p •«- i- E

(d s. SZ 0) UP . 0) Q.-0

•r—s. P o

«» s- I— lO . <0 "O v» U O 0) ^ CL Q.P O

>>

U /-

>“ E w*

'O'I

0)u.3

o> IIpIi I) II IIIiwi

IIii
Figure

VI-5:

High

speed

chart

record

of

five

determinations

of

t^^

with

methane

as

the

marker.

A

hexane

solvent

peak

is

also

present.
I
Figure

VI‘7:

Plot

ofH

/u^

vs

2p^/(p.

+

p^)

suggested

by

equation

15

for

five

diffusants

in

LPE

at

150

°C.
References and Notes

1. L. E. Smith, S. S. Chang, F. L. McCrackin, G. A. Senich, and F. W.

Wang, “Models for the Migration of Low Molecular Weight Additives in

Polyolefins," NBSIR 31-2264, April 1981.

2. J. J. van Deemter, F. J. Zuiderweg, and A. Klinkenberg, Chem. Eng.

Sci. 5, 271 (1956).

3. J. C. Giddings, S. L. Seager, L. R. Stucki , and G. H. Stewart, Anal.

Chem. 867 (1960).

4. W. L. Jones, Anal. Chem. 33, 829 (1961).

5. J. C. Giddings, Dynamics of Chromatography, Marcel Dekker, New York

(1965) Ch. 2.

6. J. C. Giddings, Anal. Chem. 85, 439 (1963).

7. S. Dal Nogare and R. S. Juvet, Gas-Liguid Chromatography, Interscience,

New York (1962) Ch. 5.

8. H. Purnell, Gas Chromatography , Wiley, New York (1962) Ch. 8.

9. H. Purnell, Gas Chromatography , Wiley, New York (1962) Ch. 9.

10. G. J. Courval and 0. G. Gray, Can. J. Chem. 54, 3496 (1976).

11. J. C. Giddings, Anal. Chem. 458 (1962).

12. J. C. Giddings, K. L. Mallik, and M. Eikelberger, Anal. Chem. 1026

(1962).

13. J. Crank and G. S. Park, Diffusion in Polymers, Academic Press, London

(1968) p. 17.

14. J. Klein and 3. J. Briscoe, Proc. R. Soc. Lond. A. 365 , 53 (1979).

15. J. C. Giddings, Dynamics of Chromatography, Marcel Dekker, New York

(1965) p. 141.

16. Certain commercial eguipment, instruments, or materials are identified

in this paper in order to adeguately specify the experimental procedure.

Such identification does not imply recommendation or endorsement by

the National Bureau of Standards, nor does it imply that the materials

or equipment identifiea are necessarily the best available for the

purpose.
VII. A Simplified Migration Decision Tree

One of the most important parameters in indirect food additive regulation is the maximum allowable concentration or a critical concentration

of the species of concern in food, C . This value is based upon toxilogical studies and from the fractional amount of total food consumed, that

would be in- contact with the packaging material of concern.

Acceptable migration would be the case in which an upper bound level

of migration for the maximum time and temperature for storage and usage, based

upon either actual tests of sound estimations, is less than the critical

or threshol d 1 evel

To this end, we have exemplified and simplified our decision tree

described earlier (NBSIR 79-1 779) as a flow chart shwon in Figure VII-1.

1 . Load Limited Migration

In the ultimate case, all the migrant of concern moves from the

packaging material into food. The concentration of the migrant in food is:

where is tlffe original concentration of the migrant in the packaging

material, and are the volumes of the packaging material and food

or solvent respectively. Migration is acceptable if this concentration is

less than the critical concentration, C .

VII-1
2 2

In general, 10 g food is considered in contact with 1 in (6.45 cm )

of the packaging material (CRF Title 21, Part 21, Part 177). In other

_3 words, by approximating the density of foods as 1 gem , the ratio of

the volumes of the packaging material to food V /V is 0.645 i where i

r ^ is the thickness of the packaging material in cm. Comnonly this ratio

is less than 1:40 or the thickness of the packaging material is less

than 0.04 cm.

Therefore, the migration level is acceptable if the following conditions are met:

''s *

p

or 1.53

if no less than 10 g of food

is in contact with 6.45 cm^

of packaging material.

or

C < 40C

0

If V_ is l^ss than 1/40 of V,

2. Solubility Limited Migration

For the case in which the loading of the migrant of concern is

greater than the above limit, the saturation solubility of the

migrant in the particular type of food or food simulant is examined in

order to find out whether the saturation solubility is less than the

critical concentration. Special attention should be given to cases

where surfactant or emulsification action may tend to increase the

actual migrant concentration in food beyond the saturation concentration. The migration level is acceptabe if

•^sat

^ C

VII-2
3. Partition Limited Migration

If both the loading and the solubility exceed the limiting threshold, then the partitioning of the migrant between the packaging material

and the food or the simulant should be examined. The partition

coefficient k is defined as the quotient of the activities, a, of the

migrant in the food and in the polymer at equilibrium. It may also be

approximated by the ratio of the solubilities in the solvent and in the

where is the original loading of migrant in the polymer. For the

final concentration in food or solvent to be less than the threshold.

polymer.

1 ^s ^sat

K a^ . p p,sat

By defining a the ratio of the amount of migrant in the solvent, M^,

versus that in the polymer, M , at equilibrium

rMV VC

= T7^ k = V.C

then the final fraction of original amount of additive migrated,

M

OD a M

G

1 + a

S

or

1 + c; a

< C , *

it requires that C . *

Thus Step 1 is just a special case of step 3.

VII-3
In the case that the partition coefficient or the saturation concentration of the migrant in the polymer is unknown or difficult to

determine, the partition coefficient may be assigned a value as in our

previous reports (NBSIR 79-1598 and 79-1779)

£nk = + X” + 1 = 2,nC + 2

sat p sat

In general, x” ts in the range of 0 to 2. Thus

This assigns a solubility of Cp of > 0.05. Therefore the requirement

is simplified as, ^ Cq < (K + 40) C ,

or ^0 "" 20C

+ 40

sat

However, this simplification is applicable only when the saturated

solubility in the food or solvent is relatively low and the solubility

in the polymer relatively high.

4. Diffusion Limited Migration

When the equilibrium properties such as the additive loading in the

polymer, the solubility of the additive in the solvent, and the partitioning of the additive between the polymer and solvent all yield too

high a final concentration of the additive in the food or the solvent

* beyond the threshold concentration C , then it is necessary to find out

kinetically whether, under the particular storage condition and in the

limited storage time, the amount of the additive migrated would produce

an additive concentration in the solvent less than that of the threshold

limit. The Kinetics of migration depends upon additive, polymer, and

solvent combinations, as well as effects of temperature and stirring.

The combination of additive, polymer, and solvent or food is the most

important factor influencing the diffusion coefficient. This diffusion

coefficient is also dependent upon temperature, with an activation

VII-4
energy in the order of 10-20 kcal/mol for polymers in the rubbery state.

A further relatively minor influence in comparison to the above factors

may be observed due to the changes in the degrees of crystallinity and

molecular weights of the polymer. Stirring speeds up the approach of an

equilibrium condition.

If the migration is kinetically limited, i.e. much less than half

of additive is migrated, then we are only interested in the short time

behavior; otherwise, the estimation of total migration from step 1 would

be sufficient.

For a single-sided extraction, at t when M^/M^ < 0.5, we may apply

the simple equation

In other words

or

-A = 2

(")

“I

r

J/2

'o’

A C . Vs

t = 2 "

where i is the thickness of the film and A is the area of contact. For

an upper limit, D is assigned the value of the diffusion coefficient

measured on the polymer swollen by the solvent concerned. In the upper

bound case, all migrants are assumed to be able to migrate from the

polymer into solvent, i.e., M = If partitioning exists, M

should be reduced from according to that described in step 3.

By assuming a storage time, t, of 1 year (3.15 x lO^s) and a container thickness of 0.04 cm (calculated from a food to container contact

2 area of 10 g/in and a container to food weight ratio of 1:40), one may

obtai

or

M./M = 1.6 X 10^

t “

M^/A = 6300

VII-5
or

t = 4100 . t 0

-11 2-1

For M^/M^ = 0.5, a diffusion coefficient of D = 10 cm s is required

to meet the threshold limit. Therfore, with the above mentioned storage

-11 2-1

conditions, only in the cases where D is less 10 cm~s will diffusion

limited migration be important enough to be considered. Otherwise

equilibrium conditions should be used for estimation. For thinner

packaging materials, D should be even less or at less than 6.2 x -92 2-1

10 2, cm s in order for the kinetic criteria for migration to apply.

For polyolefins, the glass transition temperature is lower than

-20 °C. Hence, the semicrystal 1 ine solid polymers are, in general,

utilized in the condition of mixed rubbery (amorhpous portion) and

crystalline states. It is usually assumed that the additive migration

occurs in the amorphous region. The diffusion coefficients of migrant

for the rubbery state are generally many orders of magnitude higher than

those for the glassy state. • For oligomers up to ^^32^66 and antioxidant molecules such as BHT, the apparent diffusion coefficients into

either corn oil, triglycerides or ethanol are near or greater than

-11 2-1

10 cm s above 30 °C. The influence of solvent, temperature, and

crystal 1 ini ty on the diffusion coefficients of BHT in polyethylene have

been summarized earlier in this report. Therefore, for polyolefins, the

diffusion limited case exists for these migrants and solvents only at a

storage temperature lower than ambient, or at a much shorter storage

time (a 10- fold reduction in the amount migrated requires a 100- fold reduction in time), or for a very thick container. The diffusion limited

case may also exist for extraction with poor solvents for the migrant.

However, in the case with poor solvents, the solubility limit or partition

limit requirements may often suffice.

VII-6
Fig. VII-1. A Simplified Additive Migration Decision Flow Chart

3 .
Figure VII-1. (Continued)

Glossary:

- Original concentration of migrant in polymer.

C* - Critical or acceptable concentration of migrant in food or

solvent of concern.

C^^^ - Solubility of migrant in food or solvent of concern.

K - Distribution or partition coefficient of migrant in polymer

and in food or solvent at equilibrium, ^poiy/^solv*

D - Apparent diffusion coefficient of migrant in polymer chain

by food or solvent of concern.

I C^ - Concentration of migrant in food or solvent after contact

time t.

Notes

1. This flow chart is based upon 1;he assumption of a volume

ratio of packaging material/food of 1:40 or 10 g of food

are in contact with 1 in^ or 6.45 cm^ of packing material.

Consult text for other conditions.

2. Along the decision or branching points, move to the next

step if the parameter in the particular step is unknown

or not determined, the particular step may be skipped and

the criteria of the next step will be tested.
VIII. Simulating Solvents

Within the limited temperature range of food utilization and st aae,

solvent is the single most important parameter affecting both the amount

of migrant extractable and the diffusion coefficient of the migrant,

acting through its solubilities in and its swelling action upon the

polymer.

By correlating diffusion coefficients in other solvents to that in

one of the solvents, e.g. ethanol, while keeping all other parameters

constant, it is possible to reduce the large spread of diffusion coefficiO

ents of the order of 10 to within a factor of 5 or less.

For partitioning or low solubility solvents, the correlations

depend not only on the solvent but also on the migrant and/or the polymer.

However, for solvents having moderate solubilities toward the migrant,

' the correlation seems to be independent of migrant, polymer or temperature.

The most significant correlations are those found for pure triglycerides and ethanol as food oil simulants and that for the accelerating

solvent, n-heptane. As shown in Figure VIII-I, the diffusion coefficients

of migrants (n-octadecane, n-dotriacontane or 3HT) moving from polyolefins

(LPE, BPE, PP) or E-VA copolymers into either tributyrin, trioctanoin or

synthetic triglyceride mixture HB307 at either 30 or 60 °C are almost

the same as the corresponding diffusion coefficient in corn oil. The

diffusion coefficients in the pure triglycerides are slightly higher

than that in corn oil with a ratio of D(pure triglycerides)/D(corn oil)

less than 1.5 over most of the range studied. Ethanol seems to behave

almost identically to the lower members of pure triglycerides in its

extraction behavior as shown in Figure VIII-2. However the correlation

for the data of ethanol extractions shows more scatter than that for

triglycerides within a factor of less than 3 or less.

VIII-1
From the above observations, either ethanol or low members of pure

triglycerides may be used successfully for most occasions as food oil

simulants, regardless of dissimilarities in viscosities, solvation power

for the migrants, and swelling power for the polymers.

The accelerating action of n-heptane over that of food oil has long

been recognized. The amount extractable by food oil was sometimes

considered to be 1/5 of that by n-heptane. However we found that no

constant factor will describe this accelerating action. Beside the

differences in solubilities and in partition coefficents, the accelerating power of n-heptane is clearly demonstrated in Figure VIII-3,

where diffusion coefficients in n-heptane and in triglycerides (including

corn oil) are plotted against those in ethanol for identical test samples

and conditions. Regardless of polymer, migrant and temperature, the

accerating power is greater at low diffusion coefficients than that at

high diffusion coefficients. While, at D(ethanol) around 10 cm s ,

accelerating power is greater at low diffusion coefficients than that at

1000 at D(ethanol) around 10'^^ or 10"‘^cm^s'^.

The accelerating action of n-heptane compared to that of ethanol

(and that of triglycerides) , coupled with the differences in solubilities

of oligomers of polyolefins, has dramatic effects on the total extractables of polyolefins. We, therefore, subjected large quantities (50 g)

of the raw polymer stocks of SRM 1475 (LPE) and SRM 1476 (LPE) to extraction by 500 ml of ethanol n-heptane at 70 °C for 160 days with

occasional shaking. By assigning a minimum diffusion coefficient of

-9 2-1

about 10 cm s for ^nd a pellet radius of 0.1 cm, the

2 effective time T = Dt/£ is 1.4. Thus according to the generalized

solution for the diffusion equation, the extraction should be at least

95% complete. The results of the 160-day extractions are listed in

VIII-2
Table VIII-I. For each polymer, about 6 to 8 times as much of polymer

fraction was extracted by n-heptane than by ethanol.

The extracts were then subjected to gel permeation or size exclusion chromatographic analysis by Roger C. Snyder of FDA to find out

their molecular weight distributions, as summarized in Table VIlI-2 and

shown in Figure VI I 1-4 for linear polyethylene SRM 1475 extracts, respectively. The molecular weight scales were calibrated by means of

analyzing five NBS polyethylene standard reference materials, three nalkanes (C-jq, C

2 q> and test mixtures containing known amounts of nalkanes from C- to The molecular weight scale for branched polyethylene is only approximately correct, however it should be sufficient

for comparison purposes.

The extracts from the linear polyethylene show rather normal symnetrical

distributions with peaks of molecular weight centering at about 300 for

ethanol and at about 800 for n-heptane extracts. Such results are

expected from the practice of molecular weight fractionation by solvents

of different solubility power. On the low molecular weight side, e.g.,

n-C^8*''*38’ ^ large enough solubility or even total miscibility

of the oligomer fraction in both solvents, such that almost all of the

low molecular weight fraction will be dissolved by the extraction processes, cf. labels A in Figures VIII-4 and VIII-5. As molecular weight

becomes higher, e.g., the solubility in the solvent, especially

in ethanol, decreases which causes a partitioning of the particular

component between the polymer and the extracting solvent to occur, cf.

labels B in Figures VIII-4 and VIII-5. The partitioning of

been confirmed by extraction experiments with ethanol. The diffusion

coefficients for larger molecules also drop significantly. Thus the

combination of the effects of solubility, partitioning and diffusion

created the shape of the molecular weight distribution curve beyond the

peak molecular weight extracted,

^
A similar comparison for branched polyethylene is seen in Figure

VII 1-5. The skewed curves are most likely due to the incorrectness of

the size versus molecular weight calibration which was based on nparaffins and linear polyethylene fractions. The peak of apparent

molecular weight extracted is about 350 for ethanol and about 3200 for

n-heptane extracts.

Therefore, n-heptane can not only accelerate the diffusion process

but also remove high molecular species of oligomers that may be hardly

present in ethanol or triglyceride extracts.

VIII-4
Table VIII-1

Extraction of Polyethyl enes

.-by solvents at 70°C for 160 days

Solvent

Ethanol

n-Heptane

Fraction

LPE

SRM 1475

0.0008

0.0047

Extracted

BPE

SRM 1476

0.0023

0.018
Table VIII-2

Molecular Weight Distributions of Ethanol and

n-Heptane Extractions of Polyethyl enes

Sol vent LPE

SRM 1475

BPE

SRM 1476

Ethanol 250 : 310 310 : 410

n-Heptane 560 : 1020 62'0 : 3000
D(corn

oil),

cm

/s

Figure

VIII-l

Comparison

of

Diffusion

Coefficients

in

Triglycerides

and

in

Corn

Oil
D(corn

oil),

cm

/s

Figure

VIII-2

Comparison

of

Diffusion

Coefficients

in

Ehanol

and

in

Corn

Oil
•4->

(/>

CM

E

o

o

c

CQ

O

O

(S/^LUO)a

Figure

VIII-3

Effect

of

Accelerating

Solven
n-Heptane

0.06

Ethanol

jeuiAjOd aiOMM %
Figure

VIII-3

Effect

of

Accelerating

Solvent
n-Heptane

0.06

Ethanol

jaiuA|Od 9|oq/w %
n-Heptane

Ethanol

j0iuA|Od 9|OMM % Figure

VIII-5

Molecular

Weight

Distributions

of

Ethanol

and

n-Heptane

Extracts

of

BPE
IIIIIIIpIIII. J IIpII

il

II
IX. Summary of Conclusions

* Maximum amount of extractables depends on the original migrant

concentration in the polymer, the solubilities and the partition

of the migrant in solvent and in polymer. ^

* Migration behavior is mainly Fickian.

* Diffusion coefficient may be increased by absorption of tne

solvent or swelling of the polymer by the solvent.

* Activation energies for the change of diffusion coefficient as

a function of temperature generally lie between 40 and 200 kJ

mol'\ In general, the activation energy is lower at higher

diffusion coefficients.

* Lower members of pure triglycerides may be used to simulate

the extraction behavior of corn oil in oligomers and antioxidants, such as BHT, from polyolefins.

* Anhydrous ethanol may also be considered as food-oil simulant.

* Accelerating action of n-heptane over that of food-oils or oil

simulates is'more pronounced at lower diffusion coefficients.

* n-Heptane will remove high molecular weight fractions of

oligomers which may hardly be present in food oil or oil

simul ants.

* Diffusion coefficient increases with increased oligomer content.

* Increase of amorphous content in a polyolefin produces a

corresponding change in diffusion coefficient.

* The following is the ranking of the importance of zhr- parameters

effecting the diffusion coefficient of a migrant from polymer

matrix into surrounding media:

Solvent > Temperature (limited range) > Swelling

> Migrant Concentration > Amorphous content.

IX-1

NBSIR 82-2472

Migration of Low Molecular Weight Additives

in Polyolefins and Copolymers

X. Appendix

Numerical Data of Migration of Low Molecular

Weight Additives from Polyolefins and Copolymers

Experimental Run Designat1ons--cf page II-6, Tables II-4 and II-5

110300

110600

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U.S. OEPT. OP COMM. 1. PUBLICATION OR 2. Performing Organ. Report No. 3. Publication Date

BIBLIOGRAPHIC DATA

REPORT NO.

SHEET (See instructions) NBSIR 82-2472 March 1982

I

4. TITLE AND SUBTITLE

Migration of Low Molecular Additives in Polyolefins and Copolymers

I

5. AUTHOR(S)

S. S. Chang, G. A. Senich, and L. E. Smith

i. PERFORMING ORGANIZATION (If joint or other than NSS, see instructions) 7. Contract/ Granc No. I

national bureau of STANDARDS

DEPARTMENT OF COMMERCE

WASHINGTON, O.C. 20234

4. Type of Report d, Perioo Coven

3. SPONSORING ORGANIZATION NAME AND COMPLETE ADDRESS (Scree:. Cic/. State, ZIP)

10. supplementary notes

Other Related Publications 73-1499 30-1999

79-1598 81-2264

79-1779 31-2314

'! Document describes a comouter program; SF-185. FlPS Software Summary, is attac^ied.

11. ABSTRACT lA 200->*ora or less factual summery of mosc si ^mficant mfarmaaan. if bi bliograohy or literature survey, mention it here)tCjment induces a significant

Food packaging is an inseparable part of modern life. Any substance

that migrates from the packaging material inco foods is viewed as indirect:

food additives. In connection with toxicological knowledge, it is important

to know the amount of such indirect food aedi lives expected to be present in

the food during storage and processing. This program, sponsored by “he

Bureau of Foods of the Food and Drug Admini stration is to provide theoretical

models, reliable data base, methodology to study the migration phenomena and

to provide reasonable worst-case estimates for the concentrati ons of the indirect additives in food. In this final reoort we present the results of

approximately 250 completed migration experiments based on radiotracer techniques on the migration of low molecular weight hydrocarbons and antioxidants

from polyethylene , polypropy lene and ethylene-vinyl acetate cooolymers.

Results of a study for the determination of relative diffusion coefficients

of several probe molecules in the oolyethylane melt by inverse gas chromatography are also presented. Based on these studies, ethanol aopears to be

a far m.ore reasonaole fooc-oil stimulating solvent than n-heptane. Otner

pure or mixed tri glycerides may also be considered as fooa-oil s''mulating

solvents, however they may pose the same analytical difficulties as tnat of

the food oi 1 i tsel f

.

I

12. <£Y WORDS iSj* CO twelve entries; alonabeticat oraer; caoitalize only preoer names; ana separate <ev nords oy samicoicnS/H

antioxidants; diffusion; ethylene-vinyl acetate cooolymers; food cackaging;

inverse gas chromatography ; migration; oligomers; polyethylene; polypropyl ene

; ^

TRrii nr >*-irQr H

13. availability

1 X i Unlimited

14. NO. OF

PRINTED PAGE.j

1

1 1 For Official Distribution. Qo Not Release to NTIS

i i Order From Sucserintenoent of Documents, U.S. Government Printing Office, Washington, Q.C.

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