Health and Environmental Assessment

of the Use of Ethanol as a Fuel Oxygenate

UCRL-AR-135949 Vol. 2

Report to the 

California Environmental 

Policy Council 

in Response to 

Executive Order 

D-5-99

AIR RESOURCES BOARD

V

Background

OLUME2

Information on the

Use of Ethanol as 

a Fuel Oxygenate

December 1999
Front Cover Back

Page left intentionally blank
UCRL-AR-135949 Vol. 2

Volume 2: Background Information on

the Use of Ethanol as a Fuel Oxygenate

Author

David W. Rice*

Editor

G. Cannon*

Contributor

R. Depue*

December 1999

*Lawrence Livermore National Laboratory, Livermore, CA 94550

 University of California • Livermore, CA 94550

Lawrence Livermore National Laboratory

 Environmental Restoration Division
Work performed under the auspices of the U. S. Department of Energy by Lawrence Livermore National

Laboratory under Contract W-7405-Eng-48.
UCRL-AR-135949 Vol. 2 Background Information on the Use of Ethanol as a Fuel Oxygenate December 1999

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Table of Contents

1.1. Scope of Report to the California Environmental Policy Council...........................................1

1.2. Clean Air Act and the Use of Oxygenated Fuels.....................................................................1

1.3. Requirement for a Multimedia Assessment of New Fuel Components...................................2

1.3.1. Regulatory and Legislative Requirements...................................................................2

1.3.2. Systems-based Approach to Evaluating New Fuel Components.................................3

1.4. Use of Ethanol as a Transportation Fuel Oxygenate ...............................................................4

1.5. Production of Ethanol ..............................................................................................................5

1.6. Chemical and Physical Properties of Ethanol in Gasoline.......................................................5

1.7. Increased Use of Alkylates as a Transportation Fuel Component...........................................6

1.8. References................................................................................................................................7
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Background Information on the

Use of Ethanol as a Fuel Oxygenate

1.1. Scope of Report to the California Environmental Policy

Council

Governor Gray Davis issued Executive Order D-5-99 on March 25, 1999, calling for the

removal of methyl tertiary butyl ether (MTBE) from gasoline at the earliest possible date but

no later than December 31, 2002 (State of California, 1999). Task 10 of the Executive Order

states “the California Air Resources Board (CARB) and the State Water Resources Control

Board (SWRCB) shall conduct an environmental fate and transport analysis of ethanol in air,

surface water, and groundwater. The Office of Environmental Health Hazard Assessment

(OEHHA) shall prepare an analysis of the health risks of ethanol in gasoline, the products of

incomplete combustion of ethanol in gasoline, and any resulting secondary transformation

products. These reports are to be peer reviewed and presented to the Environmental Policy

Council by December 31, 1999 for its consideration.”

This report has been prepared by the CARB and SWRCB in response to the Executive

Order D-5-99 and is divided into five volumes:

• Volume 1: Executive Summary.

• Volume 2: Background Information on the Use of Ethanol as a Fuel Oxygenate.

• Volume 3: Air Quality Impacts of the Use of Ethanol in California Reformulated

Gasoline.

• Volume 4: Potential Ground and Surface Water Impacts.

• Volume 5: Potential Health Risks of Ethanol in Gasoline.

This Volume 2 provides background information on the use of oxygenated fuels in general,

the production of ethanol and its role as a fuel oxygenate, and the physical and chemical

properties of ethanol as well as background information on key air and water issues associated

with the multimedia evaluation of ethanol as a fuel oxygenate.

1.2. Clean Air Act and the Use of Oxygenated Fuels in

California

Under the Clean Air Act (CAA) Amendments of 1990, areas of the country with poor air

quality must add an oxygen-containing, organic compound to their gasoline to reduce air

emissions. All gasoline sold in the specified, carbon monoxide nonattainment areas during

winter months must contain at least 2.7% oxygen (by weight) unless a state obtains a waiver

from the U.S. Environmental Protection Agency (US EPA) to implement a different oxygen

standard in oxygenated fuel. California’s oxygenated gasoline program limits oxygen content

to a maximum of 2.2% to limit increases in nitrogen oxides (NOx) emissions that occur from

adding oxygen to gasoline (Gomez et al., 1998). Areas that exceed the ozone standard must
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meet federal requirements for the use of reformulated gasoline (RFG). The CAA requirements

for RFG mandate that it must contain a minimum average of 2% oxygen (by weight), no more

than 1% benzene (by weight), and no heavy metals. Throughout this report the use of the

general term “gasohol” refers to either oxygenated fuel or RFG containing ethanol.

The 1977 CAA Amendments set requirements for “substantially similar gasoline” which

mandate oxygenates be approved by the US EPA before they are allowed to be used in

gasoline. Ethanol (EtOH), methanol (MeOH), MTBE, and ethyl tertiary butyl ether (ETBE)

are currently added to gasoline to meet criteria for the CAA Amendments. Because 10%

ethanol by volume blends did not meet the substantially similar definition, the US EPA has

granted a waiver for blends of gasoline containing ethanol (Gomez et al., 1998).

MTBE is the most commonly used fuel oxygenate (US EPA, 1999). It is added at 15% by

volume to oxygenated fuel or at 11% to RFG and is currently used in over 85% of the nation’s

reformulated gasoline (US EPA, 1999). Concerns have been raised about the recently

discovered widespread distribution of MTBE in ground and surface waters (Moran et al., 1999;

Zogorski et al., 1997), consumer complaints of the pungent odor, and possible health effects.

(Peaff, 1994; Bedard, 1995).

The state of California has also implemented its own RFG program—the California

Cleaner Burning Gasoline (CBG) Program (Gomez, et al., 1998). Although MTBE has been

the oxygenate used most frequently to meet the goals of this program, up to 10% ethanol (by

volume) in gasoline would also be allowed. Currently, about 70% of the gasoline sold in

California is RFG (California Energy Commission [CEC], 1999b).

1.3. Requirement for a Multimedia Assessment of New Fuel

Components

1.3.1. Regulatory and Legislative Requirements

As required by California Senate Bill 521, the University of California conducted a

comprehensive assessment of the current health and environmental impacts of MTBE use in

California (Keller et al., 1998). The findings of this assessment formed the basis for Executive

Order D-5-99 issued by Governor Davis. That Executive Order precipitated this ethanol fateand-transport analysis.

United States Environmental Protection Agency Administrator Carol Browner appointed a

Blue Ribbon Panel (BRP) in November 1998 to investigate the air-quality benefits and waterquality concerns associated with oxygenates in gasoline and to provide independent advice and

recommendations on ways to maintain air quality while protecting water quality (US EPA,

1999). Similar to the requirement in the Executive Order D-5-99, the BRP concluded that the

US EPA should conduct a full, multimedia assessment (on air, soil, and water) of any major

new additive to gasoline prior to its introduction. The BRP (1999) also recommended the

establishment of routine and statistically valid methods for assessing the actual composition of

reformulated gasoline and its air quality benefits, including the development of field

monitoring and emissions characterization techniques to assess “real world” effects of different

blends on emissions.
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Recent legislation (Stats. 1999 Ch. 813; SB 529, Bowen) enacted Health and Safety Code

Sec. 43840.8, which imposes new requirements regarding multimedia environmental

assessments of proposed amendments to ARB's motor vehicle fuels specifications. There is a

streamlined environmental review mechanism for amendments proposed prior to January 1,

2000 and adopted prior to July 1, 2000.

California Senate Bill 989 (California State Senate, 1999b) incorporates into state statues

most of the provisions of the Governor’s MTBE Executive Order. Among the bill’s other

provisions is the requirement that the SWRCB, on or before June 1, 2000, initiate a specified

research program to quantify the probability and environmental significance of releases from

petroleum underground storage tank (UST) systems that meet certain upgrade requirements

and identify those areas of the state where groundwater is the most vulnerable to MTBE

contamination, and to prioritize cleanups based on that identification. Additionally, after

January 1, 2000, the bill prohibits the ARB from adopting new fuel specifications until a

“multimedia” evaluation has been performed and submitted to the California Environmental

Policy Council for final review and approval.

1.3.2. Systems-based Approach to Evaluating New Fuel Components

New fuels or potential additives must be evaluated against not only engine performance

and emission requirements but also health and environmental criteria involving airborne toxics

and associated health risks, ozone formation potential, and groundwater contamination

resulting from production, distribution, and use. A systems-based approach is needed to

evaluate risk management trade-offs and to assess health and environmental consequences of

the use of ethanol as a fuel oxygenate. A thorough, systems-based approach would include:

1. Identification of the key attributes of gasohol production, distribution, and use, including a

fuel-cycle characterization.

2. Screening-level analysis and models to predict the likely environmental fate(s) of ethanol,

gasohol, and alkylated-fuel components released into reference landscapes and

consideration of potential exposure pathways. This assessment would contain:

• A review of the existing state of knowledge,

• The identification of physiochemical properties of the compounds of concern, and

• Environmental-fate simulations for airborne emissions and subsurface releases.

3. Exposure assessments, including toxicity evaluations of ethanol, gasohol, and alkylatedfuel components that may be released.

4. Identification of key data and knowledge gaps and the specification of the kinds of studies

needed to obtain the necessary data and to address any methodological issues related to

assessing the use of ethanol, gasohol, and alkylated fuel.

5. Performance of selected experiments to address the identified data gaps.

6. Refinement of conceptual models and integration of new data into critical analyses of

environmental transport and fate and multipathway exposures.
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1.4. Use of Ethanol as a Transportation Fuel Oxygenate

Ethanol is also widely used in oxygenated gasoline (8% in oxyfuel or 6% in RFG, by

volume) because it is a renewable, biomass-based source of fuel and because it is perceived

that its environmental impacts are less than those associated with the use of MTBE. To

promote markets for ethanol, the United States Congress has approved a 5.4-cents/gal federal

subsidy for its use in gasoline. Because of the subsidy, ethanol is sometimes used at 10% by

volume in gasoline, even in areas that are not required to use RFG (RFA, 1999).

The use of fuel alcohols as gasoline additives is increasing worldwide, both as a substitute

fuel for imported oil, and as oxygenates to minimize air pollution from combustion. In Brazil,

for example, approximately one-half of all automobiles run on gasoline containing 22%

ethanol with the remainder operating on hydrated ethanol (Petrobrás, 1995). In the United

States, gasohol is already available in many states. A recent effort by some members of the

House of Representatives to repeal the 5.4-cents/gallon tax subsidy for gasoline with ethanol

earlier than its original (year 2000) end date was defeated. Instead, the tax subsidy was

extended (Chemical Market Reporter, 1998). In addition, ongoing advances in biotechnology

will continue to lower ethanol production costs (Lugar and Woolsey, 1999; Carver, 1996).

At the federal level, the BRP was convened in late 1998 to study the benefits and risks of

the federal RFG program. In the final BRP report (US EPA, 1999), the Panel recommended

that the use of MTBE in the nation’s gasoline be substantially reduced. Based on these

recommendations, the United States Senate passed a resolution expressing support for a

nationwide phase-out of MTBE and supported ethanol as its replacement.

In separate federal initiatives, the use of ethanol as a fuel source is being advocated as a

means of promoting the use of renewable biomass fuels. President Clinton signed an Executive

Order this year to accelerate the development and use of biomass fuels, products, and

chemicals. Joined by the heads of the United States Departments of Agriculture and Energy,

US EPA, and Senator Richard Lugar, Clinton announced the goal of tripling the use of

bioenergy and bioproducts by 2010 (RFA, 1999).

Illinois Governor George Ryan recently dedicated the first fleet of urban transit buses in the

country powered by E-15 Oxygenated Diesel, a blend of ethanol and diesel fuel that shows

promise for cleaning up the environment while benefiting rural America. Known as E-15

OxyDiesel, the new fuel is a mixture of 15% ethanol, 80% diesel fuel, and 5% additives. The

Illinois governor stated that the E-15 OxyDiesel promises a substantial reduction in black

diesel exhaust and its effects, expanded opportunities in the ethanol industry, and new markets

for Illinois corn (RFA, 1999). Prior to being tested in Chicago Transit Authority buses,

E-15 OxyDiesel was tested in trucks operated by Archer Daniels Midland Corporation.

1.5. Production of Ethanol

The ethanol used for fuel is made primarily from grains or other renewable agricultural and

forestry feedstocks (Canadian Renewable Fuels Association [CRFA], 1999). However, any

feedstock that contains sugar, starch, or cellulose can be fermented and distilled into ethanol.

The fact that ethanol can be made from liquid or solid waste (such as wood byproducts) or
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agricultural wastes (such as rice straw) is an advantage. In the United States, most ethanol is

produced directly from corn (RFA, 1999).

There are basically seven steps in the whole-grain fermentation processes for producing

ethanol (American Coalition for Ethanols [ACE], 1999):

1. The grain (such as corn) is milled into a fine powder called meal.

2. The meal is liquefied with the addition of water, enzymes, and heat (120o–150oC).

3. During the process called saccharification, the liquefied starch is converted to

fermentable sugars (dextrose).

4. Yeast is added to ferment the sugars to ethanol and carbon dioxide.

5. The alcohol is distilled to increase the ethanol content from 10% alcohol by volume to

about 96%.

6. The alcohol is dehydrated to remove the remaining water. Most distillers use a

molecular sieve for this step to produce anhydrous ethanol.

7. The ethanol is then denatured with 2–5% of some product that is added to make it unfit

for human consumption. (California is specifying that unleaded gasoline be the

denaturant used in fuel-grade ethanol.)

Although some smaller distillers produce ethanol as described above, most larger facilities

separate the starch from the grain prior to fermentation (“wet-millers”) (ACE, 1999). The use

of highly purified starch as the feedstock results in a much cleaner fuel product, whereas the

ethanol fuel from whole-grain process contain a lot more impurities (Karaosmanoglu et al.,

1996) which do not need to be removed for ethanol to be suitable as a fuel additive.

1.6. Chemical and Physical Properties of Ethanol in Gasoline

Malcolm Pirnie, Inc. (1998) has published a good summary of the physical properties of

ethanol compared to MTBE. Ethanol is a small chain molecule (C2H5OH) that contains

34.7% oxygen by weight and is infinitely soluble in water. In its pure form, ethanol is a

flammable, colorless liquid with a sweet alcohol odor. Ethanol is lighter than water; and if

released rapidly in bulk onto water, it will tend to remain on the surface of the water. When

gasoline-containing ethanol is in contact with even small quantities of water, the ethanol will

separate from the gasoline into the water. Pure ethanol and ethanol blends of gasoline are

heavier than unblended gasoline.

Ethanol is very volatile and evaporates into air approximately five times faster than MTBE.

Like gasoline vapors, ethanol vapors are denser than air and tend to settle near the ground in

low areas. In open-air areas, these vapors disperse rapidly.

When burned, ethanol releases less heat than gasoline. One and a half gallons of ethanol

have approximately the same fuel combustion energy as 1 gallon of gasoline. Ethanol has a

higher ignition temperature than gasoline (approximately 850°F versus approximately 495°F).

When pure ethanol is burned, the flame is less bright than a gasoline flame but is easily visible

in daylight. Both ethanol and MTBE have similar octane ratings of about 110 and, when

added to gasoline, increase the octane rating. (The long chain, branched hydrocarbon known
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as octane is used as a standard and is equal to a rating of 100 [Center for Transportation

Research, no date]).

Though pure ethanol is poisonous, it is less acutely toxic than the benzene, toluene, ethyl

benzene, and xylene (BTEX) components in gasoline. Ethanol is present in pharmaceuticals,

mouthwash products, alcoholic beverages, cleaning products, solvents, dyes, and explosives

(Verschueren, 1983). Humans frequently ingest fermented beverages that contain about 12%

by volume ethanol. Because ethanol is a metabolic byproduct, many organisms tolerate

concentrations that may be encountered during accidental releases into the environment

(Dagley, 1984). A variety of indigenous microorganisms within the environment are capable

of using ethanol as an energy source and will preferentially utilize ethanol over other gasoline

hydrocarbons, such as benzene (Alvarez and Hunt, 1999).

Ethanol and ethanol blends of gasoline conduct electricity. In contrast, unblended gasoline

is an electrical insulator. For this reason, pure ethanol is more corrosive than gasoline and

materials-compatibility must be considered when designing large-volume, bulk-ethanol storage

tanks. Aluminum, zinc, tin, lead-based solder, or brass fittings should not be used with pure

ethanol or gasoline with high percentages of ethanol. When in contact with liquids that contain

high percentages of ethanol, some nonmetallic materials also degrade, including natural rubber,

polyurethane, cork-gasket materials, leather, polyester-bonded fiberglass laminate, polyvinyl

chloride, polyamides, and methyl-methacrylate plastics (Center for Transportation Research,

no date).

1.7. Increased Use of Alkylates as a Transportation Fuel

Component

Because the California Energy Commission (CEC, 1999a) anticipates that alkylates1 will be

used in non-oxygenated gasoline and some ethanol-containing gasolines in California to

replace the octane2 normally provided by MTBE, these compounds are also a focus of the

analysis included in this report.

Alkylates consist of branched alkanes and cycloalkanes, mostly with 6 to 9 carbons, such

as iso-octane (2,2,4-trimethylpentane) and methylcyclopentane. Alkylates are already

components in gasoline, but additional amounts will be required to maintain octane levels in

gasoline after removal of MTBE, which is a high-octane, anti-knock additive. Even though

ethanol also has a high-octane level, its oxygen content is about twice that of MTBE and,

consequently, less is required to meet a specified oxygen content (for example, 2.5 wt%

oxygen). The resulting octane deficit must be compensated for by adding high-octane blending

components, such as alkylates.

 

1 Alkylates are a gasoline blendstock produced by reacting isobutane with light olefins in the presence of strong

acid catalysts. They typically consist of branched alkanes, have very low aromatic content, and no sulfur or

olefins (Northeast States for Coordinated Air Use Management [NESCAUM], 1999).

2

 MTBE has a 110 octane rating, ethanol has a 115 octane rating; alkylates provide 91 to 99 octane ratings, and

aromatic compounds have a 100 octane rating (CEC, 1999a).
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1.8. References

ACE (American Coalition for Ethanol) (1999). Ethanol information: How ethanol is made

(online). Available: <http://www.ethanol.org/ethanol_info.html>.

Alvarez, P.J.J., and C. S. Hunt (1999). The effect of ethanol on BTEX biodegradation and

natural attenuation. In Health and Environmental Assessment of the Use of Ethanol as a

Fuel Oxygenate—Report to the California Environmental Policy Council in Response to

Executive Order D-5-99, Vol. 4, Potential Ground and Surface Water Impacts. D.W. Rice

and G. Cannon (Eds.), Lawrence Livermore National Laboratory, Livermore, CA,

UCRL-AR-135949 Vol. 4 Ch. 3.

Bedard, P. (1995). Why reformulated gas makes people sick. Car and Driver. Sept. 32.

BRP (Blue Ribbon Panel) (1999). Executive Summary and Recommendations. United States

Environmental Protection Agency, Washington, DC.

CEC (California Energy Commission) (1999a). Evaluation of Biomass-to-Ethanol Fuel

Potential in California: A Report to the Governor and the Agency Secretary, California

Environmental Protection Agency (pdf online). In Ethanol-powered Vehicles. Available:

<http://www.energy.ca.gov/afvs/index.html>.

CEC (California Energy Commission) (1999b) Timetable for the Phase-out of MTBE from

California’s Gasoline Supply. Prepared by Fuel Resources Office, Energy Information

and Analysis Division, Docket No. 99-GEO-1, June. Available:

<http://www.energy.ca.gov/ mtbe/1999-06-25_MTBEREPORT.PDF>.

California State Senate (1999a). Senate Bill 529 (Bowen) Motor Vehicles Fuels. Available:

<http://www.sen.ca.gov/>.

California State Senate (1999b). Senate Bill 989 (Sher) Pollution: Groundwater: MTBE.

Available: <http://www.sen.ca.gov/>.

Carver, M. (1996). Renewable Fuels and the Future Security of U. S. Energy Supplies. Report

to Senate Committee on Agriculture, Nutrition and Forestry, October 2.

Center for Transportation Research, Argonne National Laboratory (no date). Guidebook for

Handling, Storing, and Dispensing Fuel Ethanol (pdf online). Prepared for the

Department of Energy. Argonne National Laboratory, Chicago, IL. Available:

<http://www.ethanol.org/pdf/dispense_e85.pdf>.

Chemical Market Reporter (1998). Ethanol lobbyists display political clout in renewing the

fuel’s tax subsidy. November 30: 25.

CRFA (Canadian Renewable Fuels Association) (1999). Fact sheet: Questions and Answers

on ethanol (online). Available: <http://www.greenfuels.org/ethaques.html/>.

Dagley, S. (1984). Microbial degradation of aromatic compounds. Develop. Indust. Microbiol.

25: 53–65.

Gomez, J., T. Brasil, and N. Chan (1998). An Overview of the Use of Oxygenates in Gasoline.

California Air Resources Board, Stationary Source Division, Sacramento, CA. September.
UCRL-AR-135949 Vol. 2 Background Information on the Use of Ethanol as a Fuel Oxygenate December 1999

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Karaosmanoglu, F., A. Isigigur, and H. Ayse Aksoy (1996). Effects of a new blending agent on

ethanol-gasoline fuels. Energy & Fuels 10: 816–820.

Keller, A., J. Froines, C. Koshland, J. Reuter, J. Suffet, and J. Last. (1998). Health and

Environmental Assessment of MTBE—Report to the Governor and Legislature of the State

of California as Sponsored by SB 251: Volume I, Summary and Recommendations (pdf

online). University of California at Davis, Davis, CA. Novermber. Available:

<http://tsrtp.ucdavis.edu/mtberpt/>.

Lugar, R.G., and R.J. Woolsey (1999). The new petroleum. Foreign Affairs 78: 88–102.

Malcolm Pirnie, Inc. (1998). Evaluation of the Fate and Transport of Ethanol in the

Environment. Report prepared for American Methanol Institute, Washington, DC.

Malcolm Pirnie, Inc., Oakland, CA. November. Report No. 3522-001.

Moran, M.J., J.S. Zogorski, and P.J. Squillace (1999). MTBE in ground water in the United

States—Occurrence, potential sources, and long-term range transport. In Proceedings of

the 1999 Water Resources Conference. American Water Works Association, in press.

NESCAUM (Northeast States for Coordinated Air Use Management) (1999) Air quality, fuel

supply and cost impacts of MTBE and its alternatives, Attachment III of RFG/MTBE

report. August. Available: <http://www.nescaum.org/pdf/MTBE_PH2/Ph2AQ_costs.pdf>.

Peaff, G. (1994). Court ruling spurs continued debate over gasoline oxygenates. Chem. &

Engrg. News September 24: 4.

Petrobrás (1995). Relatório Anual de Atividades (Annual Report). Rio de Janeiro, RJ, Brazil.

RFA (Renewable Fuels Association) (1999). Governors send strong message to US EPA:

Preserve ethanol’s role in RFG. Ethanol Report (pdf online). Issue 89. February 11.

Available: <http://www.ethanolrfa.org/EReports/er021199.html/>.

State of California (1999). Executive Order D-5-99. Available:

<http://www.ca.gov/s/governor/ d599.html>.

US EPA (United States Environmental Protection Agency) (1999). Achieving Clean Air and

Clean Water: The Report of the Blue Ribbon Panel on Oxygenates in Gasoline (online).

EPA420-R-99-021, September 15. Available: <http://www.epa.gov/oms/consumer/fuels/

oxypanel/r99021.pdf>.

Verschueren, K. (1983). Handbook of Environmental Data on Organic Chemicals. Van

Nostrand Reinhold Co., New York, NY.

Zogorski, J.S., A. Morduchowitz, A.L. Baehr, B.J. Bauman, D.L. Conrad, R.T. Drew,

N.E. Korte, W.W. Lapham, J.F. Pankow, and E.R. Washington (1997). Chapter 2: Fuel

oxygenates and water quality. In Interagency Assessment of Oxygenated Fuels. National

Science and Technology Council (NSTC) Committee on Environment and Natural

Resources, Office of Science and Technology Policy, Executive Office of the President of

the United States; Global Change Research Information Office (GCRIO), Palisades, NY.
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