Mi·n ralogical Characterization 

of the Shelburne %' 1; :;,< Marbl.e 

and the Salem Limestone--

Test Stones Used to Stutiy 

the Effects··elf Acid R. in. · 
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and publications. 
Mineralogical Characterization 

of the Shelburne Marble 

and the Salem LimestoneTest Stones Used to Study 

the Effects of Acid Rain 

By Elaine S. McGee 

Shelburne Marble and Salem Limestone samples selected for 

exposure studies are compositionally homogeneous 

and are representative of marbles and limestones 

used in buildings and monuments 

U.S. GEOLOGICAL SURVEY BULLETIN 1889 
DEPARTMENT OF THE INTERIOR 

MANUEL LUJAN, Jr., Secretary 

U.S. GEOLOGICAL SURVEY 

Dallas L. Peck, Director 

Any use of trade, product, or firm names in this publication is for descriptive purposes 

only and does not imply endorsement by the U.S. Government 

UNITED STATES GOVERNMENT PRINTING OFFICE: 1989 

For sale by the 

Books and Open-File Reports Section 

U.S. Geological Survey 

Federal Center, Box 25425 

Denver, CO 80225 

Library of Congress Cataloging in Publication Data 

McGee, E.S. 

Mineralogical characterization of the Shelburne Marble and the Salem limestone-Test stones used to study the effects of acid rain I by Elaine S. 

McGee. 

p. cm.-(U.S. Geological Survey bulletin ; 1889) 

Includes bibliographical references. 

1. Marble-Composition 2. limestone-Composition. 3. Building stonesTesting. I. Title. II. Series. 

QE75.B9 no. 1889 [QE475.M3] 

557.3 s-dc20 [5521.4] 89-600193 

CIP 
CONTENTS 

Abstract 1 

Introduction 1 

The Experiment 2 

Selection of the Study Stone 6 

Shelburne Marble 6 

Salem Limestone 7 

Geologic Description 7 

Shelburne Marble 7 

Salem Limestone 8 

Mineralogical Description 8 

Methods Used 9 

Mineralogy of the Shelburne Marble 11 

Mineralogy of the Salem Limestone 15 

Stone Durability 20 

Summary 23 

Acknowledgments 23 

References Cited 23 

Figures 

1. Photograph and diagram showing block of Salem Limestone 3 

2. Photograph and diagram showing block of Shelburne Marble 3 

3. Photograph of Salem Limestone briquettes in sample rack 4 

4. Photograph of briquette sample racks at the Washington, D.C., site 5 

5. Diagram of the briquette rack showing the positions of the mineralogy briquettes by year of withdrawal 6 

6. Photograph of Shelburne Marble slab showing characteristic dark and light 

streak patterns caused by inclusions in the marble 11 

7. Photomicrograph of phlogopite and dolomite inclusions in the Shelburne 

Marble 12 

8. Al20rK20-MgO ternary diagram that shows chemical compositions of layer 

silicate minerals in the Shelburne Marble 15 

9. Photomicrographs of pyrite and calcite on a fracture surface of unexposed 

Shelburne Marble 16 

10. Photomicrograph showing pyrite and phlogopite in the Shelburne Marble 18 

11. Transmitted light image of fossil fragments in the Salem Limestone 18 

12-16. Photomicrographs of: 

12. Echinoderm fragments and bryozoan pieces, Salem Limestone 19 

13. Oblique section of an echinoderm spine piece, Salem Limestone 19 

14. Bryozoan fenestra, Salem Limestone 21 

15. Ostracod, echinoderm plates, and bryozoan fragments, Salem 

Limestone 21 

16. Gastropod, echinoderm plates and spines, and bryozoan fragments, Salem 

Limestone 21 

Contents Ill 
IV Contents 

17. Backscattered electron images of a polished section of Salem Limestone and 

energy dispersive spectra of a hematite inclusion 22 

18. Photograph showing deterioration in a column from the Jefferson Memorial, 

Washington, D.C. 23 

Tables 

1. Sample numbers, slot numbers, and year of withdrawal of briquettes of the Salem 

Limestone and Shelburne Marble used for mineralogy studies 5 

2. Notable buildings constructed of Vermont marble 6 

3. Notable buildings constructed of Indiana limestone 7 

4. Whole rock analysis of the H1-3 slab, Shelburne Marble 9 

5. Whole rock analysis of the Salem Limestone 9 

6. Sulfur in Salem Limestone 10 

7. Whole rock analyses of typical Vermont marble and Indiana limestone 10 

8. Porosity of the Shelburne Marble and the Salem Limestone 10 

9. Physical measurements of the Salem Limestone 11 

10. Physical measurements of typical Vermont marble and Indiana limestone 11 

11. Modal abundances in samples of the Shelburne Marble 12 

12. Largest dimensions of mineral grains for the Shelburne Marble 13 

13. Compositional ranges of minerals in the Shelburne Marble 14 

14. Representative mineral compositions in the Shelburne Marble 15 

15. Modal abundances in samples of the Salem Limestone 18 

16. Range of fossil and mineral compositions in the Salem Limestone 19 

17. Representative analyses of fossil fragments and calcite in the Salem 

Limestone 20 

18. Echinoderm chemical analyses, by type of fragment, in the Salem Limestone 20 
Mineralogical Characterization of the 

Shelburne Marble and the Salem LimestoneTest Stones Used to Study the Effects of Acid Rain 

By Elaine S. McGee 

Abstract 

The Shelburne Marble and the Salem Limestone 

have been used extensively in buildings and monuments, 

and for this reason they were selected as test stones for 

the National Acid Precipitation Assessment Program stone 

exposure studies. Mineralogical characterization of fresh 

Shelburne Marble and fresh Salem Limestone provides a 

basis for recognizing mineralogical changes that may 

occur in samples when they are weathered. 

The Royal variety of Shelburne Marble is a white 

marble that has gray streaks of inclusions. It is composed 

predominantly of calcite (97 percent) but contains inclusions of dolomite, layer silicates, framework silicates, and 

nonsilicates. The inclusions are heterogeneously distributed in the rock and commonly form linear clusters that 

are dominated by dolomite + phlogopite ± rutile ± 

chlorite. Less abundant inclusions are muscovite, talc, 

quartz, feldspar, pyrite, and apatite. All of the minerals 

that constitute the Shelburne Marble have nearly endmember compositions. Mineral composition, grain size, 

and inclusion associations may significantly contribute to 

the durability (or weakness) of marble used in buildings or 

monuments that are exposed to acid precipitation. 

The select buff Salem Limestone is a beige-colored, 

homogeneous, fossiliferous limestone. It is composed of 

nearly equal amounts of echinoderm and bryozoan fragments, cemented by calcite with fragments and whole 

specimens of Endothyra, ostracods, gastropods, brachiopods, and pellets. The average fossil size ranges from 0.2 

to 0.5 millimeter, but in some areas, the average size is 0.7 

millimeter. Fossil constituents such as fenestrate bryozoans (as large as 3.7x2.3 millimeters), echinoderm columnals (diameters from 0.3 to 1.4 millimeters), and ostracods 

(up to 1 millimeter) are noticeable in some areas because 

of their large size or unusual shape. The fossils are 

composed of calcite that does not differ much in composition from the matrix calcite. In the fossils, the average 

CaO is 55.14 percent, and in the matrix calcite, the average 

CaO is 55.27 percent. Both the fossils and the matrix 

contain small amounts of MgO (~0.55 percent). There is 

Manuscript approved for publication April 6, 1989. 

no significant compositional difference between the various types of fossils. Very minor quartz and hematite are 

present as small inclusions in some fossil fragments, 

particularly in echinoderm columnals, bryozoan stem 

pieces, and gastropods. The fossil fragments have a pitted 

surface in polished section, compared with the matrix 

calcite, that may be caused by very small inclusions that 

make the fossil fragments more resistant to polishing (and 

possibly resistant to weathering) than the calcite cement. 

The Shelburne Marble and Salem Limestone are 

typical of marbles and limestones that have been used in 

many buildings and monuments. The baseline characteristics determined for these stones show that the samples 

used in this study are representative of these types of 

building stones, and thus they are appropriate materials to 

use to study the effects of acid rain on marbles and 

limestones. 

INTRODUCTION 

Stone deteriorates (or weathers) when it is exposed to 

rain, wind, freezing and thawing, and so on, and although 

weathering is a natural process, increasing air pollution may 

be accelerating normal weathering processes. Acid precipitation, formed for the most part from the reaction of sulfur 

oxides and nitrogen oxides with various oxidizing agents, 

has been recognized as a widespread environmental problem (Likens and others, 1979; Babich and others, 1980; 

Armbruster and others, 1983; Franks, 1983). The marked 

deterioration of some stone buildings, monuments, and 

statues has been attributed to the effects of acid rain 

(Pearce, 1985; Peterson, 1985). For example, Skoulikidis 

(1982) suggested that the degradation of the Acropolis has 

accelerated over the last 20 to 25 years, coincident with 

increased industrialization and the use of high sulfur fuels. 

Concern about this rapid deterioration has prompted many 

studies that have attempted to determine the extent and 

causes of damage (Esbert and others, 1981; Guidobaldi, 

1981; B utlin and others, 1985; Lal, 1985) and that seek 

ways of preserving or protecting stone that is particularly susceptible (Gauri, 1978; Accardo and others, 1981; 

Castro, 1981; Skoulikidis and Beloyannis, 1981). 

Introduction 
In the United States, the National Acid Precipitation 

Assessment Program (NAPAP) is funding studies that 

address the problem of the effects of acid deposition on 

stone. Prior studies have been confined to either laboratory 

experiments or to observations and comparisons of buildings over a period of years. Although both approaches 

provide useful information, they also have limitations. 

Laboratory studies provide a controlled situation for the 

observation and manipulation of reactants but are limited by 

time constraints and by the difficulty of exactly duplicating 

the mixture of pollutants and conditions in the urban 

environment. Surveys of buildings and retrospective examination of photographs to study deterioration lack specific 

information about the pollution conditions affecting the 

stone and may lack information about the initial characteristics of the stone. We are conducting an exposed stone 

study under the auspices of the NAPAP (Task Group VII, 

Effects on Materials and Cultural Resources) that combines 

features of both laboratory and retrospective studies of stone 

weathering. In this study, dimension (building) stone samples have been placed at five exposure sites in the Eastern 

United States where atmospheric and environmental conditions are carefully monitored (National Acid Precipitation 

Assessment Program, 1984; Sherwood and Doe, 1984). 

The stone samples are studied on a yearly or quarterly basis 

to relate changes in the stones to the monitored atmospheric 

and environmental conditions (for example, Ross and others, 1989). 

Granite, limestone, sandstone, and marble are some 

of the more commonly used stones in buildings and monuments. For this study, two factors were important in 

selecting the stone to be tested. The test stone must be 

representative of the stone that has been used in buildings 

and monuments and may be at risk from acid deposition 

effects, and it must show some deterioration effects within 

the 10-year time constraints of the study. Carbonate stone 

will show weathering effects more rapidly than granite, 

which is composed primarily of silicate minerals (Winkler, 

1973). Therefore, although granite is the most widely used 

dimension stone in buildings, monuments, and bridges, we 

limited our choices of potential test stone to limestone, 

marble, and carbonate-cemented sandstone. Limestone is 

the second most widely used dimension stone (Sherwood 

and Doe, 1984). Marble is less commonly used as a 

building stone than limestone, granite, and sandstone, but it 

has been used in many monuments and buildings of 

historical or cultural value. Although carbonate sandstone is 

very susceptible to weathering, representative material is 

difficult to locate because, when sandstone was used in 

buildings, mostly local sources of sandstone were used. 

Thus, two stone types, limestone and marble, were selected 

for the exposure studies. The Salem Limestone from Indiana and the Shelburne Marble from Vermont have been 

used in many buildings, and both were available from active 

quarries that also provided stone for a number of buildings 

built over the past few decades in the Eastern and Midwestern United States. Because the Salem Limestone provided 

53 percent of the total limestone dimension stone used in the 

United States between 1880 and 1980 (D' Agostino and 

Atelsek, 1984, unpub. U.S. Geological Survey administrative report), it was selected as the limestone test sample 

(Ross and Knab, 1984). The Shelburne Marble was selected 

as the marble test stone (Ross, 1985), because, although 

Georgia and Vermont have produced comparable dollar 

amounts of marble for use in buildings, the Shelburne 

Marble from Vermont has been used in the Northeastern 

United States, the region where acid rain is more of a 

concern. 

Samples of the unexposed limestone and marble must 

be carefully characterized so that changes in the stone after 

exposure can be identified. This paper provides the initial 

mineralogical characterization of the marble and limestone 

used in the exposure program. The parent mineral phases 

that are in a rock reflect the environment and chemistry 

around the stone during lithification, and new phases may 

be produced in a significantly different environment during 

weathering. The phases behave in an ordered, predictable 

way based on their chemical composition and thermodynamic stabilities. Thus, the composition, arrangement, and 

kinds of minerals that compose the stone will influence how 

it responds to the environment; it is these features that are 

the focus of this report. 

THE EXPERIMENT 

Four sites in the Eastern United States (Newcomb, 

N.Y.; Chester, N.J.; Washington, D.C.; and Research 

Triangle Park, N.C.) were initially selected for the stone 

exposure studies, and 2 years later a fifth site (Steubenville, 

Ohio) was added. Sites were selected, in part, on the basis 

of the type of environmental monitoring equipment already 

present, the geographic location, the average yearly so2 

levels, and the availability of space for the sample racks. 

The sites are part of the NAPAP weather and pollution 

monitoring network, and in addition to the stone samples 

discussed here, the sites are used for exposure studies of 

metals and exterior paints. Air quality, meteorology, and 

rain chemistry parameters are monitored at each site and 

recorded in a standard computer format used by the Environmental Protection Agency. Some of the conditions that 

are monitored are atmospheric gas concentration, rain 

amount and chemistry, particulate amount and chemistry, 

relative humidity, temperature, and wind speed and direction. A full description of the sites and the types of 

environmental monitoring employed at the sites is given by 

Sherwood and Doe (1984), Flinn and others (1985), and 

Reddy and others ( 1986). Studies of the stone samples 

placed at these sites are being conducted by a group of 

researchers, who are employing a range of techniques. The 

2 Mineralogical Characterization of the Shelburne Marble and the Salem Limestone-Test Stones Used to Study the Effects of Acid Rain 
Figure 1A. Block of Salem Limestone at the quarry before 

cutting. Dimensions are 31fzX4X9 ft. 

studies include observations and measurements of changes 

in mineralogy, chemistry, surface roughness, and the runoff 

chemistry of the rainwater (Sherwood, 1984). 

Two large blocks of limestone and marble (figs. 1A 

and 2A, respectively) were obtained for the exposure study 

from active quarries that have provided stone for many 

major buildings. A block of Salem Limestone, 31/zX4X9 ft, 

was obtained from the Independent quarry near Bloomington, Ind., and a block of Shelburne Marble, 31/zX61/zX61/z 

ft, was obtained from the Danby quarry near Danby, Vt. 

The selection and procurement of the blocks are described 

by Ross and Knab (1984) and Ross (1985). Both blocks 

were cut into 12- x 24-inch slabs at mills near the quarries 

(Ross and Knab, 1984; Ross, 1985), and the slabs were 

numbered as shown in figures 1B and 2B. Most of the 

studies are being conducted on 2-inch-thick slabs or on 

briquettes cut from the slabs, but some of the limestone and 

marble slabs were cut 4 inches thick for some of the 

specialized tests that required thickness greater than 2 

inches (Ross and Knab, 1984). In all, 208 2-inch-thick slabs 

Figure 2A. Block of Shelburne Marble at the quarry before 

cutting. Dimensions are 31fzX61fzX61fz ft. 

Top Surface 

2~ "-------::'-:':----r' 't--------:e::-:-L ~ -i CL 

13 at 

r---~~ ~~=-~ ~ 

4 inches 

8 _i__ 

f..- 24 inches--+-1 I+ 24 inches----.., 

Figure 18. Diagram of the block, showing labeling of the 

slabs. U, upper; L, lower. 

of limestone and 252 2-inch-thick slabs of marble were 

made (figs. 1B and 2B). The 2-inch-thick slabs were 

finished on one 12- x 24-inch face so that the surface would 

resemble the surface commonly used for the stone in 

buildings; the saw cut on the opposite face was not finished. 

Thus, the limestone samples have a smooth planar finish on 

the top surface, and the marble samples have an 80 grit 

finish on the top surface. Some slabs were used for the 

rainwater runoff studies at the test sites. Other slabs were 

cut into briquettes that measure 3 x 3 5/s X 2 inches (marble) 

or 2 I5/J6 x 31/4 x 2 inches (limestone) and used in mineralogy, chemistry, and surface roughness studies. 

Slabs to be used for the runoff study and for the 

briquettes were selected to represent the average stone. 

Because the limestone is fairly homogeneous in overall 

appearance, slabs were selected from the middle of the 

block (layers G, H, and I; fig. 1B); the specific slabs 

Figure 28. Diagram of the block, showing labeling of the 

slabs. 

The Experiment 3 
Figure 3. Salem Limestone briquettes in sample rack. Briquettes are approximately 3 inches wide. Note that each 

briquette is held in place by one screw at the top edge and two dowels at the bottom edge; the bottom surface of the 

briquette rests on two plexiglass rails. The briquettes on the left of the photograph are used for mineralogy studies; the 

two briquettes on the right that have rounded corners are used in weight loss experiments. 

designated for the mineralogical studies are GL5, HL5, and 

IL5. The marble is less homogeneous in appearance, and so 

slabs were selected that contained few of the dark inclusion 

streaks. The mineralogy samples were made from the 

H14, E26, C16, 036, N15, and A33 slabs (fig. 2B). 

The briquettes are held in polymethyl metacrylate 

(plexiglass) open racks and rest on plexiglass rods that 

touch the lower surface in only two places (fig. 3). The 

racks hold 72 samples, and they are arranged side by side in 

the same relative position at all the sites (from left to right, 

limestone briquette rack, marble briquette rack, runoff 

slabs; fig. 4). The samples are positioned so that they face 

south and are tilted so that the upper surface is at a 30° angle 

from the horizontal. This arrangement was used for stability 

and to conform with the ASTM standard for test materials. 

The briquettes thus provide two analogies to surfaces on 

buildings. The upper surfaces of the briquettes are boldly 

exposed and represent those parts of buildings that may be 

washed by precipitation and thus are exposed to all wet and 

dry deposition. The lower surfaces of the briquettes are 

sheltered from direct rainfall and thus represent areas that 

are not directly washed by precipitation but may experience 

both dry deposition and dripping or collection of rainwater. 

Samples for all studies were installed at the sites on 

the following dates-North Carolina-May 25, 1984; New 

Jersey-June 5, 1984; New York-June 19, 1984; Washington, D.C.-August 11, 1984; and Ohio-July 17, 1986. The 

mineralogy samples are withdrawn at yearly intervals for 

examination and study. Briquettes used for the mineralogy 

studies were selected randomly, and the position for each 

sample in the rack was also determined randomly (National 

Park Service and Argonne National Laboratory, 1988). To 

minimize variation among the samples because of exposure 

position, the limestone and marble samples for a specified 

year occupy the same slot in their respective racks. For 

example, the first-year limestone sample is in slot 142, and 

the first-year marble sample is in slot 242; the first digit of 

the slot number indicates the limestone and marble rack, 

respectively. In addition, the samples for a specified year 

are in the same slot position at all five sites. Table 1 lists the 

sample numbers of the mineralogy briquettes at each of the 

sites, by year of withdrawal. The mineralogy samples are 

4 Mineralogical Characterization of the Shelburne Marble and the Salem Limestone-Test Stones Used to Study the Effects of Acid Rain 
Figure 4. Briquette sample racks at the Washington, D.C., site. Salem Limestone briquettes are in the foreground, 

Shelburne Marble briquettes are in the center, and the slabs used for runoff experiments are in the upper right of the 

photograph. The racks are slanted at 30° to the horizontal and face south. 

Table 1. Sample numbers, slot numbers, and year of withdrawal of briquettes of the Salem Limestone and Shelburne 

Marble used for mineralogy studies 

Year1 Year 2 Year 3 Year 4 Year 5 Year 6 Year 7 Year 8 Year 9 Year10 

Slot no. 142 153 133 118 146 158 112 154 137 125 

Site Salem Limestone 

N.Y ....... HL5-10 IL5-02 GL5-18 HL5-15 IL5-07 GL5-23 HL5-03 IL5-18 GL5-09 HL5-08 

N.J ........ HL5-06 IL5-23 GL5-14 HL5-11 IL5-03 GL5-19 HL5-24 IL5-14 GL5-06 HL5-21 

D.C ....... HL5-14 IL5-06 GL5-22 HL5-19 IL5-11 GL5-03 HL5-07 IL5-22 GL5-16 HL5-17 

N.C ....... HL5-02 IL5-19 GL5-10 HL5-05 IL5-24 GL5-15 HL5-20 IL5-10 GL5-02 HL5-16 

Ohio1 •.. ••. IL8-17 HL2-07 GL3-01 HL2-15 

Year1 Year 2 Year 3 Year 4 YearS Year 6 Year 7 Year 8 Year 9 Year10 

Slot no. 242 253 233 218 246 258 212 254 237 225 

Site Shelburne Marble 

N.Y ....... G36-20 N15-02 C16-23 N15-09 A33-10 C16-22 N15-15 A33-18 C16-18 Nl5-18 

N.J ........ G36-16 N15-23 C16-04 N15-06 A33-01 C16-20 N15-11 A33-23 C16-08 N15-22 

D.C . ...... G36-18 N15-14 C16-19 N15-12 A33-02 C16-06 N15-21 A33-07 C16-14 N15-19 

N.C ...... . H14-22 E26-19 C16-10 H14-14 E26-20 C16-12 H14-05 E26-04 C16-16 H14-D6 

Ohio1 . -..•.• G34-23 K13-17 G22-09 G24-11 

1

0nly four samples were put out at the Ohio site because this site was installed later than the other four, and the experiments were scheduled to end in 1990. 

The Experiment 5 
7 4 

10 

3 

9 1 

5 2 8 

6 

Year Slot no. Year Slot no. 

142 6 158 

2 153 7 1 1 2 

3 133 8 154 

4 1 1 8 9 137 

5 146 10 125 

Figure 5. Briquette rack showing the positions of the 

mineralogy briquettes by year of withdrawal. Samples 

were installed at New York, New jersey, Washington, 

D.C., and North Carolina in 1984, and so year 1 withdrawals at these sites were made in 1985. Positions were 

determined by a random process; Shelburne Marble and 

Salem Limestone briquettes occupy the same position in 

their respective racks. Limestone briquette slots are numbered 101-172; marble briquette slots are numbered 

201-272. 

removed on the installation anniversary from predetermined 

random locations (fig. 5). 

The ultimate goal of the mineralogical studies in the 

exposure program is to look for changes in the mineralogy 

of the stone and to determine whether those changes are due 

to the environmental conditions at the exposure sites. Thus, 

two questions have guided this study of the mineralogy of 

the unexposed stone: What are the reactants, and what 

characteristics or features of the minerals may be significant 

to the weathering of the stone? Knowledge of the stone's 

mineralogical characteristics and geologic history and studies of stone durability done by others provide some indication of the types of changes that may occur when the stone 

is exposed in a polluted environment. 

SELECTION OF THE STUDY STONE 

Shelburne Marble 

The Shelburne Marble, quarried in western Vermont 

and known by the trade name of Vermont marble, was 

selected as a test stone because it has been used in many 

monuments and historic buildings (table 2), particularly in 

the Eastern and Northeastern United States, where acid rain 

has long been recognized as a problem. The quarry that 

supplied the stone for the exposure study also supplied stone 

for the Jefferson Memorial, the Rayburn Building, and the 

French Embassy in Washington, D.C. (table 2). 

Shelburne Marble forms layers that contain different 

kinds and amounts of inclusions. The inclusions give the 

marble distinctive colors and striking patterns and may vary 

significantly from one layer to the next. Six broad groups of 

colors and patterns identified by Bain (1933) (white with 

gray dolomite mottling, white, white with greenish veining, 

gray and blue gray, .fine textured black, and red) reflect 

some of the differences in the layers and illustrate the 

diverse appearance of the Shelburne Marble. The appearance of the stone and the types of inclusions that it contains 

influence the uses to which a specific marble can be 

applied. Thus, the marble-producing companies have given 

commercial or trade names (for example, Royal, Imperial, 

Danby, and Dorset B) to marble layers within the Shelburne 

Marble; the names relate to the color characteristics of the 

marble. Many names have been used for the various layers. 

Although the names given to the marbles were used for 

many years, new names were sometimes given if a quarry 

changed hands; these name changes make tracing the usage 

of specific marbles difficult. The Royal marble from the 

Danby quarry was selected for the exposure study 

Table 2. Notable buildings constructed of Vermont 

marble 

[-, date unknown] 

Building 

The New Y ark City Library .. . 

The Federal Reserve Bank .... . 

Buildings of the Harvard Medical School. 

The John Hay Memorial 

Library. 

Memorial Continental Hall 

(Daughters of the American 

Revolution). 

The Red Cross Building ...... . 

The Supreme Court ... . ... . .. . 

The Jefferson Memorial ...... . 

The Rayburn Building .. .. ... . 

The French Embassy ...... . .. . 

The Art Association Building .. 

Location Date built 

New Y ark City 1911 

Philadelphia, Pa. 

Boston, Mass. -1912 

Providence , R.I. -1912 

Washington, D.C. 1909 

do. 1917 

do. 1936 

do. 1943 

do. 1965 

do. 1984 

Montreal, Canada -1912 

6 Mineralogical Characterization of the Shelburne Marble and the Salem Limestone-Test Stones Used to Study the Effects of Acid Rain 
Table 3. Notable buildings constructed of Indiana limestone 

[-, date unknown] 

Building 

The Empire State Building ... . 

Rockefeller Center ........... . 

The Metropolitan Museum of 

Art. 

The National Archives ....... . 

The Pentagon ............... . 

The Department of Interior ... . 

The National Cathedral ....... . 

The Indiana Capitol Building .. 

The University of Chicago ... . 

The Academy of Science ..... . 

Location 

New York City 

do. 

do. 

Washington, D.C. 

do. 

do. 

do. 

Indianapolis, Ind. 

Chicago, Ill. 

do. 

Date built 

1931 

1931 

1938 

1941 

1937 

1907 

(started) 

1878 

~1890 

~1890 

because it is similar in appearance and physical characteristics to the marble used in many of the buildings listed in 

table 2 (Ross, 1985). 

Salem Limestone 

The Salem Limestone, known by the trade name of 

Indiana limestone, has been used extensively in the construction of government and private buildings in the Eastern 

and Midwestern United States. Prior to the appearance of 

portland cement around 1900, limestone was the cheapest 

durable building material that was homogeneous in color 

and texture (Rooney, 1970). The dimension (building) 

stone facies of the Salem is uniformly textured, is a good 

freestone (meaning that it can be easily carved in any 

direction), and has little preferential splitting (Patton and 

Carr, 1982). By 1896, Salem Limestone had been used in 

the construction of buildings and as trim to complement 

other stones in 25 States (Hopkins and Siebenthal, 1896). 

Some of the notable buildings constructed of Indiana 

limestone are listed in table 3. Because of its widespread 

and continued use and because of its availability, the Salem 

Limestone was selected as the limestone for the acid 

deposition exposure studies. 

Dimension limestone that is selected for use in a 

building is specified by its color and grade. The color of the 

Salem Limestone varies, but it is classified as buff, gray, or 

variegated (a mixture of buff and gray). Grades are determined by the sizes of the pores and grains that form the 

texture of the stone. The texture is assessed by visual 

examination when the stone is graded. Three grades, rustic, 

standard, and select, are commonly used. Two other 

grades, gothic and statuary, also have been quarried but 

rarely are used. Of the three commonly used grades, rustic 

is the coarsest grained, and select is the finest grained and 

the most homogeneous in appearance. Although it is difficult to quantify the limits of the three grades, grain size 

decreases from the rustic through the standard to the select 

grade, and the pore sizes within each grade are typically 

more than 2 mm in the rustic, less than 2 mm in the 

standard, and less than 1 mm in the select (Rooney, 1970). 

The Salem Limestone block obtained from the Independent 

quarry near Bloomington, Ind. (Ross and Knab, 1984), is 

classified as a select buff stone. 

GEOLOGIC DESCRIPTION 

Shelburne Marble 

The Shelburne is of Early Ordovician age and is a low 

grade, regionally metamorphosed marble that forms part ~f 

the marble belt in western Vermont. The Shelburne IS 

interbedded with and overlain by schist. The complexly 

folded marble beds lie along the Middlebury synclinorium. 

The marble beds are bounded on the east by the Green 

Mountains, where low-angle thrust faults dip to the east, 

and are bounded on the west by the Adirondack Mountains, 

where thrust faults dip to the west along the northern portion 

of the marble belt and normal faults dip to the east along the 

southern portion. The Shelburne varies from sedimentary 

limestone near the Canadian border to the coarse-grained 

marble that is quarried in Danby, Vt. The Danby quarry lies 

in the southernmost of three main structural units that form 

the marble belt (Bain, 1934). The southernmost structural 

unit extends from Manchester to Middlebury and is characterized by medium- to coarse-grained marbles in complex 

flowage and fold structures. The two structural units to t~e 

north have experienced less tectonic and metamorphic 

activity than the southernmost unit. The central structural 

region of the marble belt lies between Middlebury and 

Milton and is characterized by fine-textured stone in simple, 

open folds lying between thrust faults. The northern structural unit, in the vicinity of Plattsburg, N.Y., and Isle la 

Motte, Canada, is a faulted area of unmetamorphosed 

sediments. 

The Danby quarry in Vermont is the source of the test 

stone used for this study, and it is also the only producing 

quarry in the Shelburne Marble. The gently plunging (8°) 

synclinal structure at the Danby quarry has enabled 

improvements to be made in quarrying techniques and thus 

allowed the quarry to be a contender in the world market 

(Meade, 1980), while other Vermont marble quarries have 

closed. 

The nature of the folding in the marble beds is a 

significant factor in assessing the commercial value of a 

particular layer of marble. As the marble beds were folded, 

the calcite became plastic, and elongation and thinning of 

the beds along the limbs of the folds and thickening of the 

beds at the ends of the folds resulted (Dale, 1912, 1914). 

Locally, a marble layer may thin to inches, and at other 

places it may thicken to more than 300ft (Bain, 1959). It is 

from the thickened beds that large, useable blocks of marble 

can be removed, and they are thus more likely to be of 

commercial value than marble taken from thin layers. 

Geologic Description 7 
Salem Limestone 

The Salem is Late Mississippian in age and has an 

outcrop area in south-central Indiana that is nearly 160 mi 

long (Donahue, 1967). Stratigraphically, it is above the 

Harrodsburg Limestone and below the Saint Louis Limestone. The Salem lies horizontal or slopes westward at very 

low angles (Loughlin, 1929), and it occurs in outcrop as 

massive rounded ledges that are gray in color and coarsely 

textured (Rooney, 1970). In some places, the Salem is 

nearly 100ft thick, but where dimension stone is quarried it 

is commonly 40 to 60ft thick (Smith, 1966). Early quarries 

in the Salem Limestone were located along or adjacent to 

stream valleys (Udden, 1909). The quarries today are 

located where there are thick, homogeneous lenses of 

material suitable for dimension stone (Patton and Carr, 

1982). The lenses or pods of suitable dimension stone are 

irregularly scattered; in some places, less than a mile from 

a thick lens, the dimension stone facies may thin or be 

interrupted (Patton and Carr, 1982). The principle production of dimension stone from the Salem Limestone is in the 

central third of its outcrop area, between the White River 

and the East Fork White River in Monroe and Lawrence 

Counties (Patton and Carr, 1982). 

The Salem Limestone comprises three lithologies: ( 1) 

a well-sorted, medium- to coarse-grained, massive calcarenite; (2) a poorly sorted calcarenite that ranges in grain 

size, sorting, and porosity; and (3) an impure carbonate that 

contains varying amounts of quartz and carbonaceous material (Smith, 1970). The ideal dimension stone from the 

Salem is massive, even textured, medium grained, and 

bryozoan rich but has few echinoderm plates and few 

specimens of the foraminifer Endothyra (Smith, 1966). 

Thus, of the three lithologies described, the first is the one 

that is used for dimension stone. 

The building stone facies of the Salem is light gray to 

bluish gray but is oxidized to a buff color in massive 

sections and along bedding planes and joints. Crossbeds are 

common microscopically and in outcrop; they are characteristic of the Salem Limestone and are well displayed in the 

weathered stone. Most crossbeds are less than 1 ft high, but 

they may be between 1 and 3 ft (Patton and Carr, 1982). 

The stone has a granular texture and a range of grain sizes 

from fine ( < 1 mm) through medium ( 1-3 mm) to coarse 

(> 3 mm), and it is well sorted (Loughlin, 1929). The 

porous and permeable nature of the limestone makes it an 

important reservoir for oil in the Illinois basin (Patton and 

Carr, 1982). 

The Salem Limestone has long been discussed in the 

geologic literature because of its distinctive dwarf fauna, 

which was first described by Hall (1858). Much has been 

written about the fossil constituents in an effort to distinguish whether the small sizes were due to stunting or 

selective sorting (Donahue, 1967). The foraminifer Endothyra baileyi is used as a guide fossil to identify the Salem 

in outcrop and in subsurface samples (Smith, 1970; Patton 

and Carr, 1982). Although the Salem has been called an 

oolitic limestone, true oolites are rare (coatings on fossil 

fragments are usually much less than 20 percent of the 

diameter (Patton and Carr, 1982)), as are structureless 

pellets. Both mechanically rounded fossil debris and abundant spheroidal specimens of Endothyra baileyi give the 

stone an oolitic aspect that may have given rise to the 

misnomer (Rooney, 1970; Smith, 1970). 

For many years the name used for the Salem Limestone in Indiana has been a matter of controversy (Smith, 

1970); however, for the last 30 years the name Salem 

Limestone has been consistently used by geologists. Some 

of the names that have been used and later discarded include 

Bedford stone, Bedford oolitic limestone, and Spergen 

limestone (Loughlin, 1929; Smith, 1970). The Salem Limestone also has names that are used in the dimension stone 

trade, such as Indiana limestone, Indiana oolitic limestone, 

Bedford stone, and Bedford oolitic limestone (Udden, 

1909). Some of these trade names are still in use today, 

although the most common name is Indiana limestone. 

MINERALOGICAL DESCRIPTION 

A necessary assumption that underlies the stone 

exposure program experiment is that the characteristics of 

the stones are known prior to exposure, particularly those 

characteristics that may influence the weathering behavior 

of the stone. Because stone is composed of various constituents (minerals and (or) fossils), it may respond inhomogeneously to liquid and gaseous weathering agents, such as 

H20, H+, S04 =, S02 , and so on. The mineral compositions, shapes, sizes, and associations all may contribute to 

the stone's resistance to deterioration. Thus, to provide a 

baseline for our study, we have examined freshly quarried 

samples from the blocks of Shelburne Marble and Salem 

Limestone that have been placed at the NAPAP stone 

exposure sites. 

The focus of the mineralogical characterization has 

been to identify the kinds and compositions of the mineral 

constituents, as well as their relative abundances, distributions, and associations. Characteristics related to the mineralogy, the bulk composition, the porosity, and some 

physical measurements, also were determined. The methods used and results of the mineralogical characterization 

are discussed below. The bulk compositions were obtained 

by submitting samples of the marble and limestone for 

whole rock analysis. One average sample of marble was 

analyzed from the middle of the block (slab H1-3), and four 

samples of limestone were analyzed, one from the top 

(AU3), one from the bottom (NU3), and two from the 

middle (GU3, HU3) of the block. The major and trace 

elements determined from whole rock analysis of the 

marble and limestone are shown in tables 4-6. As can be 

8 Mineralogical Characterization of the Shelburne Marble and the Salem Limestone-Test Stones Used to Study the Effects of Acid Rain 
Table 4. Whole rock analysis of the H1-3 

slab, Shelburne Marble 

[Analyses made by J.R. Lindsay (U.S. Geological 

Survey). Major elements determined by X-ray fluorescence; trace elements determined by direct 

reader direct current arc spectrometry. LOI. loss on 

ignition] 

Major elements (weight percent) 

Si02 ••••••••• 0.40 

Al20 3 •••••••• .20 

Fe20 3 •••••••. <.05 

MgO......... .52 

CaO......... 55.50 

Na20........ <.10 

K20......... .09 

Ti02 ......... .02 

P20 5 ......... <.03 

MnO......... <.01 

LOI.......... 43.20 

Total . . . . . . 99.93 

Trace elements (ppm) 

Mn ...... 234 La ...... 56 

As ·····. <100 Li ....... <10 

Au ...... <9.5 Nb ...... 162 

B . . . . . .. <9.5 Ni ....... 14 

Ba ...... 22 Pb ...... 38 

Be . ... . . . 99 Sb ...... <100 

Bi ....... <10 Sc ....... <10 

Cd ...... <2 Se ....... <200 

Ce . ..... 218 Sn 0. 0 • •• <8.4 

Co ...... 13 Sr ....... 302 

Cr ....... 19 Te .. .. . . <49 

Cu ...... 6.4 v ....... 38 

Ga ...... <9.7 y ....... 13 

Hg ...... <500 Zn ...... 648 

Zr ....... 51 

seen from tables 4, 5, and 7, the whole rock compositions 

of the Shelburne Marble and the Salem Limestone are 

similar to the compositions of typical Vermont marble and 

Indiana limestone. Porosity measurements on the marble 

and limestone samples are shown in table 8. The total 

porosities of the marble ( ~o. 7 5 percent) and of the limestone ( ~ 18.6 percent) are typical for these rock types (table 

8). Physical tests were made on samples of the Salem 

Limestone block by the Indiana Geological Survey (table 

9), but no similar tests were made on samples of the 

Shelburne Marble block. Similar physical tests were made 

on commercial marbles (Kessler, 1919) and limestones 

(Kessler and Sligh, 1927) to establish their value for use in 

masonry structures. Table 10 summarizes results from some 

of the tests made by Kessler (1919) and Kessler and Sligh 

( 1927) for a Vermont marble and an Indiana limestone that 

were taken from quarries near Danby, Vt., and Bedford, 

Ind., and that are similar to the Shelburne Marble and 

Salem Limestone samples of this study. The compression 

and shear strength measurements on the Salem samples 

Table 5. Whole rock analysis of the Salem Limestone 

[Rapid rock analysis of major elements by Homer Smith (U.S. Geological 

Survey). Emission spectrographic analysis of trace elements by A.F. 

Dorrzapf, Jr., and C.J. Skeen (U.S. Geological Survey)] 

Sample AU3 GU3 HU3 NU3 

Major elements (weight percent) 

Si02 ............... 0.44 0.52 0.48 0.52 

Al20 3 .............. .19 .48 .18 .17 

Fe20 3 ••.•••••.••••• .10 .18 .13 .12 

FeO ··············. .02 <.01 <.01 <.01 

MgO ............... .44 .48 .47 .47 

CaO ............... 56.2 55.3 55.4 55.5 

Na20 .............. .06 .05 .05 .06 

K20 ............... .22 .13 .12 .15 

H2o+ .............. .17 .42 .40 .31 

H2o- .............. <.01 .05 <.01 .07 

Ti02 .......••...... .01 .01 .01 .01 

P20s ............... .01 .01 .03 .03 

MnO ............... <.01 <.01 .02 .02 

C02 ··············· 43.2 43.1 42.7 43.5 

Total ............ 101.15 100.73 99.99 100.93 

Trace elements (ppm) 

Ag ................. 0.11 <0.10 0.11 <0.10 

Ba ................. 6.0 3.0 3.2 3.2 

Co ................. 1.7 1.6 1.3 1.5 

Cr ................. 3.7 3.0 6.0 1.6 

Cu ................. 1.1 <1.0 <1.0 <1.0 

Dy ................. <22 22 <22 <22 

Mn ................ 150 150 140 150 

Mo ................ 2.9 3.6 2.9 3.0 

Ni ................. 3.8 3.5 3.2 2.5 

Sc ................. 3.5 3.6 3.1 3.8 

Sr ................. 500 550 540 510 

v .................. 6.2 5.8 4.5 6.9 

Y .................. 3.8 3.1 3.7 4.1 

Zr ................. 6.8 3.9 5.8 5.2 

from the test block are much lower than the same measurements made by Kessler and Sligh (1927). A similar comparison made by the Indiana Geological Survey (written 

commun., March 28, 1986) between test Salem Limestone 

samples and typical Salem Limestone samples showed that 

the measurements differed significantly only in shear 

strength; samples from our test block had a lesser shear 

strength than that of typical Salem Limestone. 

Methods Used 

For the initial mineralogical characterization, polished thin sections were used to identify minerals and to 

determine the minerals' composition, distribution, association, and relative abundances. Polished sections of the 

Hl-3 slab (fig. 2B) of the Shelburne Marble were chosen to 

represent the diversity of the random inclusions in the stone. 

Polished sections of the Salem Limestone represent the top 

(AU3), bottom (NU3), and middle (GU3, HU3, LU6) 

Mineralogical Description 9 
Table 6. Sulfur in Salem Limestone 

[Analyses by P.P. Hearn, R.G. Johnson, and Homer Smith (U.S. 

Geological Survey)] 

Insoluble residue 

(weight percent) 

left after dissolvAU3 GU3 HU3 NU3 

ing rock in 5 percent HCl. 0.71 0.89 0.83 0.79 

Total sulfur from 

sulfides (ppm) 

contained in insoluble residue. 70 170 100 100 

Total sulfur from 

barite (ppm) contained in insoluble 

residue. 

Total sulfur as soluble sulfate (ppm) 

from the 5 percent 

6 

HCl solution. < 1 

6 2 

<1 <1 <1 

portions of the test block (fig. 1B). The sections were cut 

parallel to the bedding. Optical microscopy, modal analysis, scanning electron microscopy, and electron microprobe 

analysis were used in the mineralogical characterization. 

Modal analysis was used to determine the abundances 

of the individual minerals or fossils. For the marble, this 

information indicates the abundance of inclusions relative to 

calcite, and for the limestone, it indicates the abundance of 

fossils relative to matrix calcite. The results for the marble 

Table 7. Whole rock analyses of typical 

Vermont marble and Indiana limestone, 

in weight percent 

[Representative Vermont marble and Indiana limestone samples were measured by Kessler (1919; 

reference no. 10, Danby marble from Danby, Vt.) 

and Kessler and Sligh (1927; reference no. 46, 

Standard Buff limestone from near Bedford, Ind.). 

These examples were selected for comparison 

because of their similarity and proximity to test 

stones of this study. LOI, loss on ignition; insol. 

insoluble in HCl; orgnc, organic matter] 

Vermont marble 

CaO ..... . 

MgO .... .. 

Fe20 3 ••... 

Al20 3 ••..• 

so3 ••..... 

LOI. .... .. 

insol ..... . 

55.30 

.41 

.03 

.10 

trace 

43.72 

. 76 

Indiana limestone 

CaO .... .. 

MgO .... .. 

Fe20 3 ••••. 

Al20 3 ••... 

S03 .••.... 

Na20 ..... 

Si02 •..... 

TotalS ... . 

LOI. .... .. 

54.60 

.68 

.05 

.75 

.05 

.12 

.24 

.85 

43.57 

orgnc . . . . . trace 

Table 8. Porosity, in cumulative percent, of the Shelburne 

Marble and the Salem Limestone 

[Measurements by G.R. Olhoeft (U.S. Geological Survey)] 

Shelburne Marble Salem Limestone 

K13-01 G22-07 HL2-20 GL3-07 

Water accessible ..... 0.332 0.221 17.466 17.398 

Helium porosity ...... .374 .258 17.828 17.689 

Total porosity ........ .807 .731 18.651 18.748 

were combined into groups of mineral types (carbonates, 

layer silicates, framework silicates, and nonsilicates), and 

the results for the limestone were grouped by fossp types 

(echinoderms, bryozoans, other fossils-for example, 

Endothyra, ostracods, gastropods, and brachiopods) and 

calcite matrix. Miscellaneous categories were used in both 

point counts to account for points that were difficult to 

clearly distinguish. 

Quantitative chemical analyses of individual mineral 

phases and fossils were obtained by using an ARL-SEMQ 

electron microprobe. Standards similar to the unknowns 

were measured to check on analysis quality, and unknown 

analyses were judged to be acceptable for silicates, oxides, 

and sulfides if (1) the oxide total was 98 to 102 and (2) the 

cation stoichiometry was correct for the mineral analyzed. 

Several points were analyzed on each grain. Representative 

occurrences of a mineral were sought to determine if its 

composition varied with proximity to other mineral phases. 

Silicates and oxides were analyzed at 15 KV by using 

a beam current of0.1 ~J.a, 20 second counts, and a minimum 

(1-2 ~J.m) spot size. Bence and Albee (1968) correction 

procedures with modifications by Albee and Ray (1970) 

were used, and data were reduced on line (McGee, 1983). 

The elements that were analyzed varied for each mineral 

group. Water in layer silicates was calculated (Flohr, 1983) 

after the on-line data reduction. Sulfides were analyzed by 

using procedures similar to those used for silicates and 

oxides; however, a higher accelerating voltage of 25 KV 

was needed to measure zinc, copper, nickel, and cobalt. 

Analysis of carbonates required special analytical 

conditions because carbonates tend to be unstable under the 

operating conditions used for silicates and oxides. Thus, 

carbonates were analyzed by using 12 KV accelerating 

voltage, 0.05 ~J.a beam current, 20 second counts, and a 

spot size of ~0.2 mm. Data were reduced on line by using 

the MAGIC method of Colby (1968). C02 amounts were 

calculated off line for each of the carbonate analyses by 

using two assumptions: (1) the analysis total (with C02 

included) equals 100 and (2) C02 is the only oxide in the 

mineral that was not measured by the electron microprobe. 

Because the oxide totals and mineral stoichiometry of the 

C02 -free analyses could not be used directly to check the 

analysis quality (as they are with silicate and oxide analyses), modified checks were needed. By comparing the 

10 Mineralogical Characterization of the Shelburne Marble and the Salem Limestone-Test Stones Used to Study the Effects of Acid Rain 
Table 9. Physical measurements of the Salem Limestone 

[Measurements are averages of three determinations; ( ), standard deviation; -, measurement not made; measurements were made by the Indiana 

Geological Survey] 

Sample 

Hardness to Compression 

abrasion (lb/in2

) 

Modulus of 

rupture 

(lb/in2) 

Specific gravity 

Coefficient of 

absorption 

(percent) 

Shear strength 

(lb/in2

) 

ALl .......... 6.46 (0.03) 5,090 (1 ,600) 

GU2 ......... 6.65 ( .32) 4,540 ( 966) 

NL7 .......... 6.85 ( .10) 5,180 ( 330) 1,030 (36) 

2.21 (0.006) 

2.22 ( .006) 

2.23 ( .006) 

5.93 (0.05) 

5.92 ( .20) 

5.89 ( .04) 1,290 (15) 

Table 10. Physical measurements of typical Vermont marble and Indiana limestone 

[Representative Vermont marble and Indiana limestone samples were measured by Kessler (1919; reference no. 10, Danby marble from Danby, Vt.) and 

Kessler and Sligh (1927; reference no. 14, Select Buff limestone from Bedford, Ind.). These examples were selected because of their similarity and 

proximity to test stones of this study. Mbl, marble; Ls, limestone; Pp, perpendicular to bedding; pl, parallel to bedding; -, measurement not made. Frozen, 

tests made on samples that were frozen and thawed 30 times. Porosity is a calculated value; most values are averages of at least two tests] 

Compression Modulus 

Sample Wet of rupture Dry Frozen (lb/in2

) (lb/in2

) 

Mbl Pp ..... 10,558 9,944 8,599 1,524 

Mbl pl. ..... 10,691 10,306 8,734 1,481 

Ls Pp ..... 8,350 8,950 1,810 

Ls pl. ..... 9,000 9,299 1,505 

standard calcite and dolomite analyses (determined by wet 

chemical analysis) with the C02-free microprobe analyses, 

good C02- free totals for calcite (55-56 weight percent) and 

dolomite (52-53 weight percent) were determined. A check 

on the mineral stoichiometry of an analysis was made after 

C02 was calculated, and cation values were redetermined. 

A good carbonate analysis should have a sum for cations 

(Ca+Mg+Fe+Mn+Sr) of 1.0±0.2. 

Mineralogy of the Shelburne Marble 

The Shelburne Marble is composed predominantly of 

white calcite. Ten other minerals form heterogeneously 

distributed inclusions in the marble and, as they are commonly intergrown and some are dark in color, give the 

marble a characteristic streaked appearance (fig. 6). Whole 

rock analysis of a representative portion of the marble 

shows that CaO is the dominant component; all other oxides 

and element concentrations are below 1 weight percent 

(table 4). The minerals that compose the Shelburne are 

divided into four groups: carbonates (calcite, dolomite), 

layer silicates (phlogopite, muscovite, chlorite, talc), 

framework silicates (quartz, feldspar), and nonsilicates 

(rutile, pyrite, apatite). A common association is phlogopite 

+ dolomite ± rutile ± chlorite (fig. 7). Averaged modal 

abundances and modal abundances of the minerals within 

each sample are shown in table 11: carbonates= 97.3 

percent, layer silicates= 1. 8 percent, framework 

Specific Absorption Shear 

by weight by volume strength Porosity gravity (percent) (lb/in2

) 

2.71 0.102 0.276 0.48 

2.37 4.2 9.9 2,010 12.9 

2,000 

Figure 6. Slab of Shelburne Marble (dimensions 2X12X24 

inches), showing characteristic dark and light streak pattern caused by inclusions in the marble. 

Mineralogical Description 11 
Figure 7. Typical association of phlogopite and dolomite 

inclusions in the Shelburne Marble. Cc, calcite; Ph, phlogopite; Do, dolomite. 

silicates=0.1 percent, nonsilicates close to 0 percent, and 

pits and holes=O. 7 percent. Although talc, quartz, potassium feldspar, rutile, and pyrite were not encountered 

during point counting, all of these phases were found during 

petrographic study. Although random areas of the thin 

sections were counted to determine modal abundances, the 

sections were made especially to include portions of the 

dark inclusion streaks. Thus, the abundances determined by 

modal analysis should be regarded as approximate abundances. 

Most of the inclusions are relatively small grains 

(table 12). Mineral compositions do not vary much (table 

13) and are similar to the end member or ideal composition 

for that mineral. A description of each mineral in the 

Shelburne Marble is given below, and representative analyses of each phase are shown in table 14. 

Carbonates. -Although the Shelburne Marble is predominantly ( ~97 percent) calcite, it also contains dolomite 

( ~0.6 percent). The calcite is white in hand specimen and 

is unzoned and inclusion free in thin section. The calcite 

grains are equidimensional but vary in the largest dimension 

from 290 to 860 J.Lm; grain widths vary over relatively short 

distances, and within the scale of a thin section they 

commonly vary by 300 J.Lm. Grains are irregularly sliaped, 

have subangular to slightly curved edges, and are tightly 

interlocked. Calcite twinning is common, but much of it 

probably was caused by sample preparation. Compositionally, the calcite is fairly pure CaC03 and has an MgO 

content that averages 0.8 weight percent (tables 13 and 14). 

Dolomite is light to dark gray in hand specimen, but 

in thin section it has a speckled appearance that results from 

numerous tiny black inclusions. Dale (1912) identified one 

type of marble as graphitic calcite marble. The inclusions 

are probably graphite, but in this study they have not been 

positively identified because they are of submicron size and 

are not at the , surfaces of the grains. Dolomite grains are 

irregularly rounded in shape and range in diameter from 10 

to 290 J.Lm (table 12). They are commonly found in clusters 

with or without phlogopite, but solitary grains of dolomite 

surrounded by calcite grains are also present. The association of dolomite + phlogopite grains gives the marble its 

Table 11. Modal abundances in samples of the Shelburne Marble, in percent 

Samples 

H13-N-6 H13-N-7 H13-N-8 H13-N-9 H13-N-10 

Carbonates 

Calcite ............... 98.3 95.4 96.5 98.8 94.2 

Dolomite ............. 0 0 1.6 0 1.5 

Layer silicates 

Phlogopite ............ .2 3.3 .6 .2 2.9 

Muscovite ............ 0 .1 .1 .4 0 

Chlorite .............. .1 .7 .2 .1 .6 

Talc .................. 0 0 0 0 0 

Framework silicates 

Quartz ........... .. .. 0 0 0 0 0 

Sodium feldspar ....... .1 0 .3 0 0 

Potassium feldspar .. .. 0 0 0 0 0 

Nonsilicates 

Rutile ................ 0 0 0 0 0 

Pyrite ................ 0 0 0 0 0 

Apatite ............... 0 .1 0 0 0 

Pits, miscellaneous ...... .4 .3 .2 .3 .7 

Holes ................... .7 .2 .3 .3 .1 

12 Mineralogical Characterization of the Shelburne Marble and the Salem Limestone-Test Stones Used to Study the Effects of Acid Rain 
characteristic streaked appearance (figs. 6 and 7). The 

dolomite composition is very close to the ideal 

CaMg(C03h, although dolomite in the samples contains 

very small amounts of FeO ( ~0.3 weight percent) (tables 

13 and 14). 

Layer silicates.-Layer silicates (phlogopite, muscovite, chlorite, talc) are the second most abundant mineral 

group in the Shelburne Marble (0.3-4 percent; table 11). 

None of the: layer silicates has a large compositional range 

(fig. 8). Because the layer silicates form linear clusters of 

thin blades, they give the marble its distinctive wavy streak 

pattern. 

Phlogopite is by far the predominant layer silicate 

phase. In hand specimen it has a pale brown color and, with 

dolomite, is readily visible in the colored streaks of the 

marble. Optically, the phlogopite is only weakly pleochroic 

(very pale brown to white), and thin blades of phlogopite 

grains are intergrown together. Phlogopite + dolomite ± 

chlorite is a common association, but phlogopite also occurs 

as small isolated grains. Phlogopite blades range from 20 to 

nearly 600 J-Lm in length (table 12) but are commonly 150 to 

300 J-Lm long. Phlogopite is magnesium rich (Mg0=25.8-

28.0 weight percent) (tables 13 and 14) and contains minor 

amounts of FeO ( ~0.6 weight percent), Ti02 ( ~0.3 weight 

percent), and fluorine ( ~2.4 weight percent). 

Muscovite is relatively rare. It is small (10-100 J-Lm 

in length; table 12) and occurs as sparsely scattered colorless grains. Muscovite contains a small amount of MgO 

(2-3 weight percent) and very minor amounts of CaO ( ~0.4 

weight percent) and Ti02 (0.5-0.9 weight percent) (tables 

13 and 14) and is close to the ideal muscovite composition. 

Chlorite is nearly as rare as muscovite, but the grains 

are larger ( ~50-200 J-Lm long; table 12), and it is usually 

intergrown with phlogopite (or with phlogopite and dolomite). The grains are colorless in thin section. Compositionally, the chlorite belongs to the clinochlore group 

because it contains 32.3-33.3 weight percent MgO, only 

~ 1 weight percent FeO (tables 13 and 14), and ~5.8 silicon 

cations. 

Talc is rare but notable because the grains are large 

(400-530 J-Lm long; table 12). It is colorless in hand 

specimen and in thin section. The talc is in inclusion-rich 

areas, and it is most closely associated with quartz and 

dolomite. It is nearly ideal in composition (tables 13 and 14) 

and contains very minor amounts of Al20 3 (0. 2-0.4 weight 

percent), FeO ( ~0.3-0.4 weight percent), and fluorine 

(0.5-0.7 weight percent). 

Framework silicates. -Framework silicates in the 

Shelburne Marble include feldspar and quartz, which constitute up to 0.3 percent of the marble. Both feldspar and 

quartz are rounded, colorless, 30- to 150-J-Lm grains (table 

12). They are usually found as isolated grains, although 

they may be present also in inclusion-rich areas. Quartz is 

nearly pure Si02 (tables 13 and 14). Sodium feldspar is the 

primary feldspar in the Shelburne Marble, and it is commonly 50 to 100 J-Lm in diameter. A minor amount of small 

(30-40 J-Lm) potassium feldspar is present too. Both feldspars are very close to their respective ideal compositions 

(tables 13 and 14). 

Nonsilicates. -Rutile, pyrite, and apatite compose 

the nonsilicates in the Shelburne Marble. All are rounded, 

small grains; rutile and pyrite are similar in size (10-60 and 

10-40 J-Lm in diameter, respectively), but apatite is a little 

larger (30-100 J-Lm) (table 12). Rutile and apatite are 

colorless and best seen in thin section. Large grains of 

pyrite are visible in hand specimen, but they are rare. Pyrite 

is not framboidal in the unexposed marble; the surface 

texture of the pyrite is nearly indistinguishable from that of 

Table 12. Largest dimensions of mineral grains (~m) for the Shelburne Marble 

H13-N-6 

Carbonates 

Calcite ............... 700-860 

Dolomite ............. 

Layer silicates 

Phlogopite ........... . 

Muscovite . . . . . . . . . . . . 10-40 

Chlorite ............. . 

Talc ................. . 

Framework silicates 

Quartz . . . . . . . . . . . . . . . 40-100 

Sodium feldspar....... 40-75 

Potassium feldspar . . . . 30-40 

Nonsilicates 

Rutile ............... . 

Pyrite ............... . 

Apatite .............. . 

Samples 

H13-N-7 H13-N-8 

350-570 450-570 

20 10-90 

40-500 25-580 

20-100 20-30 

50-70 100-200 

50-150 15-75 

10-50 10-35 

10-40 

30 

H13-N-9 H13-N-10 

290-570 360-500 

60-290 20-180 

80-375 20-480 

60-100 

530 400 

150 50-70 

130 

60 40 

40-100 

Mineralogical Description 13 
.... 

~ 

~ 

:r 

~ Ill 

0 

OQ 

;:;· 

!:!.. 

n 

:r 

~ Ill 

!l 

~ 

;:::r 

a 

s· 

::I 

0 

:r -(D 

Vl 

:r 

(D 

a= 

5; 

::I 

(D 

~ Ill 

atO 

Ill 

::I 

c. 

-:r 

(D 

Vl 

Ill 

tO 

3 

r-

§f 

(D 

~ 

0 

::I 

(D 

I 

-1 

:! 

Vl 

0 

::I 

(D 

<ll 

s;: 

(D 

c. 

0 

Vl 

c 

c. 

-< 

:r 

(D 

m 

~ !l 

<ll 

0 

-

> 1"1 

a: 

;:11:1 

Ill 

:;-

Table 13. Compositional ranges of minerals in the Shelburne Marble, in weight percent 

[( ), number of grains analyzed] 

Oxide 

CaO ........ . 

MgO ........ . 

MnO ........ . 

FeO ........ . 

SrO ......... . 

co21 ....... . 

Oxide 

Si02 ......•.• 

Al20 3 ....... . 

Na20 ....... . 

CaO ........ . 

K20 ........ . 

BaO ........ . 

FeO ........ . 

MgO ........ . 

Carbonates 

Calcite 

(42) 

Minimum Maximum 

53.59-55.94 

.21-1.28 

0-.01 

0-.37 

0-.32 

43.29-44.97 

Dolomite 

(11) 

Minimum Maximum 

29.84-34.09 

18.37-21.72 

0--0 

.18-.65 

0-.25 

47.15-48.21 

Framework silicates 

Feldspar 

(28) 

Quartz 

(10) 

Minimum Maximum Minimum Maximum 

67.25-69.63 

19.28-20.35 

11.31-12.13 

.03-.60 

.03-.11 

0-.04 

0-.03 

0-.01 

98.07-101.50 

0-.05 

0-.04 

0-.05 

0-.03 

.06-.38 

0-.13 

0-.10 

1

Calculated value. 

Oxide 

Si02 ......... 

Al20 3 ........ 

K20 .. ....... 

CaO ......... 

MgO ....... .. 

FeO ......... 

BaO ......... 

Ti02 ......... 

Na20 ........ 

MnO ......... 

F .. ..... ..... 

H201 ........ 

Oxide 

Ti02 ........ . 

Cr20 3 ....... . 

Al20 3 ......•. 

FeO ........ . 

MgO ........ . 

MnO ........ . 

NiO ........ . 

CaO ........ . 

Si02 ••••••••. 

Phlogopite 

(34) 

Minimum Maximum 

41.67-44.57 

12.15-15.12 

9.69-10.90 

.03-.53 

25.76-27.97 

.52-.76 

0-.11 

.22-.42 

.04-.22 

0-.02 

2.06-2.83 

2.98-3.41 

Rutile 

(8) 

Minimum Maximum 

96.55-98.35 

0-.14 

0-.04 

0-.18 

0-.08 . 

0--0 

0-.02 

.21-2.01 

0-.08 

Layer silicates 

Muscovite 

(4) 

Minimum Maximum 

48.96--49.84 

30.20-33.56 

10.28-10.47 

.33-.49 

2.32-3.34 

.10-.12 

.11- .18 

.52-.88 

.11-.14 

0-.02 

.13-.17 

4.41-4.57 

Nonsilicates 

Element 

Fe ............. . 

s .............. . Cu ............. . 

Zn ...... . ...... . 

Co ............. . 

Ni ............. . 

Chlorite 

(5) 

Minimum Maximum 

30.41-31.37 

20.23-21.50 

0-.71 

.03-.19 

32.34-33.26 

.86-1.13 

0-.04 

0-.07 

0-.02 

0-.02 

.36-.49 

I 2.66-12.74 

Pyrite 

(5) 

Minimum Maximum 

45.30-45.76 

52.43-52.99 

0--0 

0--0 

.06-.20 

0--0 

Talc 

(3) 

Minimum Maximum 

62.05-63.44 

.16-.36 

0--0 

.09-.16 

30.70-31.54 

.29-.35 

0-.04 

.05-.07 

.05-.06 

0-.04 

.45-.66 

4.44-4.45 
Table 14. Representative mineral compositions in the Shelburne Marble, in weight percent 

Carbonates 

Oxide Calcite Dolomite 

CaO ...... 54.87 30.66 

MgO .... .. . 78 21.05 

MnO ...... 0 0 

FeO ...... . 05 .31 

SrO ....... .10 . 03 

co21 ..... 44.20 47.95 

Total ... 100.00 100.00 

Framework silicates 

Sodium Potassium 

Oxide feldspar feldspar 

Si02 ...... 68.08 65.02 

Al20 3 ..... 19.90 18.91 

Na20 ..... 11.76 .26 

CaO ...... .19 .16 

K20 ...... . 09 16.55 

BaO ...... 0 .16 

FeO ...... 0 0 

MgO ...... 0 0 

Total ... 100.02 101.06 

Ab ........ 98.62 2.30 

An ........ .89 .80 

Or ........ .49 96.89 

1

C02 calculated by difference and stoichiometry. 2

H20 calculated on the basis of site occupancies. 

Oxide 

Si02 ...... 

Al20 3 ..... 

K20 ...... 

CaO ...... 

MgO ...... 

FeO ...... 

BaO ...... 

Ti02 ...... 

Na20 ..... 

MnO ...... 

F ......... 

H202 ..... 

Total ... 

Quartz 

99.05 

0 

. 01 

. 13 

0 

. 04 

0 

0 

99.23 

the surrounding calcite in the secondary electron image (fig. 

9). Rutile , pyrite, and apatite may occur as isolated grains 

or may be associated with phlogopite in inclusion-rich areas 

(fig. 10). In one sample, rare sphene ( ~20 J-Lm) is associated 

with rutile ± quartz in an inclusion-rich area. The distribution of the nonsilicates is heterogeneous; pyrite grains are 

commonly localized in small areas. Rutile is the most 

widely distributed of the three phases, and apatite is a very 

minor inclusion. Rutile is nearly pure Ti02 (tables 13 and 

14), although it does contain some CaO ( ~ 1 . 2 weight 

percent), which may be due to the small grain size and 

overlap effects with calcite during analysis. Pyrite is homogeneous in composition (tables 13 and 14) and contains iron 

( ~45. 5 weight percent), sulfur (~52. 7 weight percent), and 

minor cobalt ( ~0.12 weight percent). 

Mineralogy of the Salem Limestone 

Layer silicates 

Phlogopite Muscovite Chlorite Talc 

42.60 49.07 30.54 62.52 

14.64 30.20 20.82 .20 

10.45 10.47 0 0 

.25 .33 .19 .09 

26.00 3.34 33.26 30.96 

.69 .12 1.09 .34 

0 .11 0 .02 

.35 .55 0 .05 

.05 .13 0 .05 

0 .01 0 .02 

2.14 .17 .39 .53 

3.29 4.41 12.73 4.44 

100.46 98.91 99.02 99.22 

Nonsilicates 

Oxide Rutile Element Pyrite 

Ti02 ...... 98.09 Fe ........ 45.42 

Cr20 3 .•••• .02 s ......... 52.83 

Al20 3 ..... . 04 Cu ........ 0 

FeO ...... . 07 Zn ...... .. 0 

MgO ...... . 07 Co ........ .13 

MnO ...... 0 Ni . .. . .... 0 

NiO ...... .02 Total . .. 98.38 

CaO ...... .59 

Si02 .... . . 0 

Total ... 98 .90 

MUSCOVITE t 

CHLORITE 

, PHLOGOPITE 

The Salem Limestone is a very pure calcium carbonate limestone. Whole rock analyses, fossil compositions, 

and the kinds and compositions of the minerals in the stone 

Figure 8. AI 20 3-K20-Mg0 ternary diagram that shows 

chemical compositions of layer silicate minerals in the 

Shelburne Marble. 

Mineralogical Description 15 
Figure 9. Pyrite and calcite on a fracture surface of unexposed Shelburne Marble. A, In the secondary electron image, 

surficial characteristics of pyrite are indistinguishable from those of the calcite (compare with B). 

reveal that the limestone contains little besides calcitecemented fossils. Whole rock analyses of four samples from 

the test block show that the limestone averages 55.6 percent 

CaO and that the CaO content varies only slightly throughout the block (table 5). The average MgO content is 0.47 

percent, and it too varies only slightly in the test block 

(table 5). The unexposed limestone also contains Si02 

(0.44-0.52 percent), Al20 3 ( ~0.18 percent with one exception), K20 (0.12-0.22 percent), and strontium (500-550 

ppm). Most of the sulfur measured in the unexposed stone 

is contributed by sulfides (70-170 ppm; table 6). 

The limestone is well sorted and even grained (fig. 

11); the average fossil size is 0.2 to 0.5 mm, but in some 

areas 0. 7-mm fragments are common. Whole fossils and 

fossil fragments are cemented by calcite, and mineral 

phases other than calcite are rare. Modal analysis of the 

samples indicates that the stone is composed of nearly equal 

amounts of echinoderm pieces and bryozoan fragments 

(29.9 percent and 27.2 percent, respectively; table 15). The 

calcite matrix is the next most abundant constituent (15.1 

percent), followed by miscellaneous fossils (11.8 percent), 

voids (10.0 percent), other fossils (3.9 percent), and pellets 

(2.0 percent). The miscellaneous fossils category includes 

fragments of fossils that were too small to positively 

identify but are most likely bryozoan fragments, echinoderms, small pellets, and algae pieces. The category "other 

fossils" includes Endothyra, ostracods, gastropods, and 

brachiopod pieces. Calcite was the only mineral phase 

encountered during point counting, but rare grains of 

quartz, feldspar, and hematite or magnetite were found 

during examination of the stone. The proportions of fossils 

found in these samples are similar to the results obtained by 

Smith (1962) in his study of more than 100 sections of 

Salem Limestone from various locations in Indiana. He 

found that most samples have a larger volume of fossil 

constituents than binding material and that bryozoans are 

16 Mineralogical Characterization of the Shelburne Marble and the Salem limestone-Test Stones Used to Study the Effects of Acid Rain 
Figure 9.-Continued. B, In the backscattered electron image of A, the pyrite appears white compared to the calcite. 

the most abundant fossil material, followed by echinoderms. Smith ( 1962) reported that miscellaneous fossils, 

bryozoans, and echinoderms are well mixed throughout the 

samples of Salem Limestone and concluded that the unclassifiable fossils are most likely bryozoans and echinoderms 

because these two fossils have the best representation in the 

Salem Limestone. 

Echinoderms.-Plates, spines, and columnal segments of echinoderms are present in the test block (fig. 12). 

The plates are the most abundant echinoderm piece, are 

generally square to elongate in shape, and measure from 

0.3x0.2 to 0.9x 1.5 mm. Plates that measure 0.3X0.5 and 

0.9x 1 mm are the most common, however. Oblique 

sections of echinoderm spine pieces (fig. 13) are elongate 

and measure approximately 1.5 X0.3 mm, although some 

measure up to 3.8X0.3 mm. Echinoderm columnal segments are readily recognizable but are not as abundant as 

the plates. The columnals range in size from 0. 3 to 1.4 mm 

in diameter. The echinoderm pieces are composed of calcite 

and do not differ in composition from the matrix calcite that 

surrounds them. Indeed, many of the echinoderm pieces are 

surrounded by large single grains of calcite that are in 

optical continuity with the fossil fragment. The echinoderm 

pieces predominately contain CaO, only small amounts of 

MgO (0.49-0.68 weight percent), and variable SrO 

(0.0-0.44 weight percent; tables 16-18). Echinoderm 

spines and columnals contain slightly less MgO than the 

echinoderm plates (table 18). Although the SrO contents of 

the various echinoderm pieces vary, there is no correlation 

between SrO content and type of fossil fragment. 

Bryozoans.-Bryozoans are most commonly found in 

the sample as fragments of stems, but occasionally portions 

of fenestra have been preserved (figs. 12 and 14). The 

bryozoan pieces are elongate in shape, and they range 

greatly in size. A common size is approximately l.Ox0.2 

mm, but pieces that are up to 1.4 mm long are not unusual. 

The fenestra that have survived are variable in degree of 

preservation and in size; pieces are about l.Ox 1.5 mm in 

Mineralogical Description 17 
Figure 10. Typical ass5ciation of pyrite and phlogopite in 

the Shelburne Marble. Cc, calcite; Ph, phlogopite; Py, 

pyrite. 

size, but one piece is 3.7x2.3 mm. Compositionally, the 

bryozoans are about 55 weight percent CaO, slightly more 

than 0.5 weight percent MgO, and slightly less than 0.5 

weight percent SrO (tables 16 and 17). Because of the 

abundance of bryozoans and because they could easily have 

fractured into pieces that would be difficult to identify with 

certainty, it is very likely that many of the pieces counted as 

miscellaneous fossils during modal analysis are actually 

small fragments of bryozoan stems. 

Other fossils.- The remaining fossils in the Salem 

Limestone form a minor (less than 5 percent) component of 

the fossil content, but they are notable because in most 

cases they are preserved as whole or nearly whole specimens. 

The foraminifer Endothyra has been widely used as 

an index fossil to identify the Salem. Endothyra is not 

Figure 11. Transmitted light image of fossil fragments in 

sample LU6D of the Salem Limestone. Note the homogeneous sizes of the fragments. Echinoderm plates (Ec) and 

bryozoan fragments (By) are abundant; Endothyra (E) and 

pellets (P) are also present. Scale bar=1 mm. 

particularly abundant in the test stone (1 percent of points 

counted), but because it is easy to identify, especially in 

field and laboratory studies, it has been useful to researchers 

(Smith, 1962). In the test stone, Endothyra individuals are 

quite uniform in size (0.3 mm in diameter) and appearance 

(fig. 11). Compositionally, Endothyra is nearly pure calcite, has only 0.5 weight percent MgO, and has less than 

0.1 weight percent of all other elements (table 17). 

Ostracods are preserved in the Salem as partial and 

whole specimens and are unusually striking in thin section 

(fig. 15). The inner part of the shells is usually empty but is 

sometimes lined with small calcite crystals. The ostracods 

are commonly elliptical in shape and are approximately 

0.6x 1.0 mm in size. It is likely that the ostracods contribTable 15. Modal abundances in samples of the Salem Limestone, in percent 

[No quartz or minerals other than calcite were found during point counting] 

Total 

AU3C AU 3D GU3C HU3D LU6D NU3C NU3D average 

Bryozoan .................... 27.3 27.4 19.4 32.3 27.8 28.9 27.1 27.2 

Echinoderm ................. 26.5 26.5 38.9 30.7 26.0 28.0 33.3 29.9 

Other fossils (3.9) 

Endothyra ................. .6 .2 2.0 .4 .7 .8 2.1 1.0 

Ostracod .................. .5 .8 2.8 .2 .4 .4 2.1 1.0 

Gastropod ......... ..... ... .8 .6 .7 0 .3 .7 .2 .5 

Brachiopod ......... ....... 1.0 2.3 2.5 .8 .7 .7 2.0 1.4 

Void ........................ 9.9 10.8 10.5 11.4 9.1 11.3 7.2 10.0 

Calcite matrix ............... 19.2 18.0 8.9 14.0 19.7 12.3 13.8 15.1 

Pellet ....................... .9 1.8 5.0 .7 1.2 .9 3.8 2.0 

Miscellaneous fossils ......... 13.3 11.7 9.3 9.5 14.3 16.1 8.5 11.8 

Total points ........... 1,169 1' 133 1,049 1,039 1,058 1,028 1,076 7,552 

18 Mineralogical Characterization of the Shelburne Marble and the Salem Limestone-Test Stones Used to Study the Effects of Acid Rain 
Figure 12. Echinoderm fragments and bryozoan pieces 

are typically mixed in the Salem Limestone, sample AU3D. 

Note echinoderm columna! (Ec) in lower left and partial 

bryozoan fenestra (By) in lower right. Scale bar=1 mm. 

ute to the inhomogeneous appearance of some of the lower 

grades of Salem Limestone (for example, perhaps forming 

the "glass spots" mentioned by Loughlin, 1929). The 

ostracods are similar compositionally to the other fossil 

constituents of the Salem Limestone (tables 16 and 17). 

Gastropods constitute about 0.5 percent of the limestone. They are preserved as whole or nearly whole specimens and are commonly filled with a very fine dark material 

that resembles mud (fig. 16). Gastropods in the samples 

contain so much of this very fine dark material and pitting 

(and occasional identifiable grains of quartz) that it was not 

possible to obtain any good analyses of the gastropods. The 

gastropods range in size from 0. 3 to 0. 7 mm in diameter. 

Matrix calcite. -Calcite cement fills spaces between 

fossil fragments and lines pore spaces in the Salem Limestone. Compared to the fossil fragments in polished sections, the matrix calcite is clear and unpitted. The matrix 

calcite either surrounds and is in optical continuity with 

echinoderm fragments or it occurs as rounded grains, ~20 

to 50 J..Lm in diameter, between fossil pieces. Compositionally, the matrix calcite is nearly pure (Ca0=54.84 to 55.92 

percent, MgO < 1 percent), and it does not differ much 

from the fossil compositions (tables 16 and 17). 

Other mineral phases.-Quartz and hematite are 

present in the Salem Limestone as small inclusions in fossil 

fragments, particularly in echinoderm columnals and bryozoan stem pieces (fig. 17A,B). Quartz grains are angular 

and range in size from 10 to 50 J..Lm commonly measuring 

10 to 20 J..Lm. Hematite is rounded and irregularly shaped, 

ranging in size from 10 to 100 J..Lm but commonly 10 to 20 

J..Lm. Identification of the hematite is tentative, because, 

although iron was detected by using energy dispersive 

analysis on the scanning electron microscope, good quanFigure 13. Oblique section of an echinoderm spine piece 

(Ec), sample AU3D, Salem Limestone. Scale bar=1 mm. 

titative analyses of the grains were not obtained. Small 

amounts of silicon in some hematite inclusions were 

detected (fig. 17C) and may indicate the presence of minute 

quartz grains within the pitted areas of the fossil fragments. 

Pitted areas of the fossil fragments were avoided during 

electron microprobe analysis because the poor sample 

surface always produced poor mineral analyses. Although 

minute mineral inclusions are not reflected in the overall 

composition of the stone (or the fossils), they may play a 

significant role in the weathering behavior of the fossil 

fragments in the limestone. 

Table 16. Range of fossil and mineral compositions in the 

Salem Limestone, in weight percent 

[( ), number of fragments or grains analyzed] 

Oxide 

CaO .......... . 

MgO ......... . 

MnO ......... . 

FeO .......... . 

SrO .......... . 

co2~ ......... . 

Oxide 

CaO .......... . 

MgO ......... . 

MnO ......... . 

FeO .......... . 

SrO .......... . 

co21··· ······· 

Bryozoan 

(6) 

Minimum Maximum 

54.00-55.52 

.29-.93 

0-.12 

.01-.22 

.12-.49 

43.76-44.66 

Ostracod 

(3) 

Minimum Maximum 

54.88-55.76 

.56-.98 

.02-.05 

.04-.08 

.03-.14 

43.59-44.00 

1

Calculated value. 

Echinoderm 

(11) 

Minimum Maximum 

54.60-55.43 

.36-.95 

.01-.08 

.02-.14 

0-.44 

43.52-44.61 

Matrix calcite 

(14) 

Minimum Maximum 

54.84-55.92 

.45-.88 

.03-.09 

.01-.11 

0-.25 

43.24-44.76 

Mineralogical Description 19 
Table 17. Representative analyses of fossil fragments and calcite in the Salem Limestone, in 

weight percent 

Oxide Bryozoan Echinoderm 

CaO ......... 54.98 55.41 

MgO ......... .62 .55 

MnO ......... .03 .05 

FeO ......... .15 .09 

SrO .......... .39 .16 

C02

1 ........ 43.84 43.75 

1 C02 calculated by difference and stoichiometry. 

Voids.-The Salem Limestone is a relatively porous 

material; voids constitute 10 percent of the rock volume 

(table 15). A more accurate measure of the proportion of 

voids in the stone is shown by the porosity measurements 

(table 8). The samples have a total porosity of ~ 18.7 

percent, slightly higher than the porosity measurement by 

Kessler and Sligh ( 1927), but within the range of porosities 

determined for all of the select buff limestones from Indiana 

(Kessler and Sligh, 1927, table 12). Connected pore space 

(water accessible porosity) constitutes 17.5 percent of the 

total porosity of our Salem Limestone samples (table 8), 

while only 0. 8 to 1.4 percent of the total porosity is 

contributed by isolated pores. The connected pore space 

may play a significant role in the stone's response to 

weathering because the connected pores may act as channels for the movement of liquid in the stone; rain may be 

readily transported into the stone along the interconnected 

pores. Incomplete filling by matrix between fossil fragments forms the connected pore space in the limestone and 

presents a large surface area where material may be dissolved or precipitated within the stone. 

STONE DURABILITY 

Building stone durability depends on factors that 

include natural defects in the stone, structure design, faulty 

selection or improper use of the stone, and macro- and 

microenvironmental conditions where the stone is used. 

Studies made in the late 1800's and early 1900's show that 

Ostracod Endothyra Matrix calcite 

54.88 55.39 55.18 

.98 .53 .68 

.02 .04 .05 

.06 .03 .10 

.06 .09 .07 

44.00 43.91 43.92 

geologists, architects, and others concerned with the building stone industry were aware of many of these factors (for 

example, Julien, 1884; Kessler, 1919; Kessler and Sligh, 

1927; Loughlin, 1929; Schaffer, 1932). In an early study of 

the relative durability of building stones in New York City, 

Julien (1884) noted certain characteristics of the stones 

(coarseness of grain size, presence of fossils or oolites), as 

well as architectural flaws (lack of drips, use of flat sills 

rather than sloped sills) that appeared to lead to accelerated 

deterioration of some stones. All stones used in buildings 

are exposed to physical and (or) chemical weathering agents 

that work on any inherent weaknesses in the stone. Physical 

weathering processes include rain, wind, ice, and organisms. 

Chemical weathering processes such as hydration, 

hydrolysis, oxidation, reduction, and exchange reactions 

(Reiche, 1950; Oilier, 1975) are likely to cause mineralogical changes. Chemical weathering processes are of a 

particular concern because the objective of the stone exposure program is to determine the contribution of acid 

precipitation to the weathering of building stones. Thus, it 

is expected that solution, hydrolysis, and cation exchange 

will be important processes in the deterioration of the 

stones. The interaction between physical and chemical 

weathering processes is significant, however, and cannot be 

ignored in a study of stone deterioration. 

The varied susceptibility of minerals to alteration in 

the weathering environment will influence how the stone 

responds to the environment. Because the Shelburne Marble 

and the Salem Limestone are composed so predominantly of 

Table 18. Echinoderm chemical analyses, in weight percent, by type of fragment 

in the Salem Limestone 

[( ), number of fragments analyzed] 

Oxide 

CaO ............. . 

MgO ............ . 

MnO ............ . 

FeO ............. . 

SrO ............. . 

C02

1 •••••••.••••. 

1

Calculated value. 

Columnal 

(3) 

Minimum Maximum 

54.93-55.43 

.36-.55 

.01-.06 

.07-.10 

.04-.41 

43.52-44.61 

Plate 

(7) 

Minimum Maximum 

54.60-55.38 

.46-.95 

.01-.08 

.02-.14 

0-.44 

43.71-44.48 

Spine 

(1) 

AU3D-2-1 

54.80 

.91 

.01 

.12 

.17 

43.99 

20 Mineralogical Characterization of the Shelburne Marble and the Salem limestone-Test Stones Used to Study the Effects of Acid Rain 
Figure 14. Large pieces of bryozoan fenestra (By) in the 

Salem Limestone. Sample AU3D, scale bar=1 mm. 

calcite, dissolution of calcite under acidic conditions will be 

a significant component of the weathering processes that act 

on the stones. However, the degree to which calcite 

dissolution is important in the overall durability of the 

stones is influenced by a number of other factors. Dolomite, 

the layer silicates, and possibly pyrite are also likely to play 

a significant role in the weathering of the marble as they 

react with water, pollutants, and one another in the marble. 

When determining the rates of weathering in minerals, 

crystal size, crystal shape, crystal perfection, and access of 

the weathering agent and removal of weathered products are 

important factors to consider, in addition to composition 

and structure (Ollier, 1975). 

The Shelburne Marble is medium to coarse grained 

and contains a variety of mineral inclusions that are heterogeneously distributed throughout the rock and are clustered together in linear streaks. On the basis of his examination of buildings in New York City, Julien (1884) 

estimated the life of coarse dolomitic marble to be 40 years, 

for fine dolomitic marble to be 60 to 80 years, and for fine 

marble to be 50 to 200 years. Dale (1912) recognized the 

significance of grain size and shape to stone durability. He 

suggested that, although fine-textured marbles present more 

surface area to rainwater, water can travel rapidly in a 

coarse-textured loosely compacted marble and thus readily 

weather the coarse marble. Bain (1941) also identified the 

width of intergranular openings in marble as a significant 

factor in the rate of marble weathering because of accessibility to water provided by the cracks. A similar accessibility to water is present around the grain boundaries of large 

flakes or crystals of silicate inclusions in marble (Dale, 

1912). Pore space and cracks are rare in the marble, and 

calcite grain boundaries are difficult to distinguish using 

scanning electron microscopy. Where calcite grains meet 

inclusions, the boundaries are more visible because of slight 

Figure 15. Ostracod (Os), echinoderm plates (Ec), and 

bryozoan fragments (By). Note matrix calcite (Cc) between 

echinoderm pieces in right half of photograph. Salem 

Limestone, sample GU3C, scale bar=1 mm. 

differences in texture and grain shapes. Although the 

Shelburne Marble is tightly compacted and not very porous, 

the movement of water along grain boundaries, especially 

where large silicate inclusions are present, can be significant. Lewin and Charola (1981) studied a dolomitic marble 

containing large platy or fibrous inclusions and concluded 

that it is particularly susceptible to the effects of freezing 

and thawing when the inclusions are present, resulting in a 

blistered and pitted appearance on the stone surface. It is 

likely that the inclusions will weather preferentially in the 

Shelburne Marble or that their presence will contribute to 

increased intergranular water in local areas. A preliminary 

examination of Shelburne Marble columns on the Jefferson 

Figure 16. Gastropod (Gs), echinoderm plates (Ec) and 

spines, and bryozoan fragments (By). Salem Limestone, 

sample NU3C, scale bar=1 mm. 

Stone Durability 21 
Figure 17 A. Backscattered electron image of a polished 

section of Salem Limestone. Bryozoan stem (By), echinoderm pieces (Ec), and matrix calcite (Cc). Matrix calcite is 

light gray and is between the larger fossil pieces. Note 

small round grains of calcite lining the pore (black) spaces. 

Note the pitting in the fossil fragments as compared to the 

matrix calcite. 

Memorial in Washington, D.C., has revealed pock marks 

and grooves that mimic the silicate inclusion pattern (fig. 

18); some of which still contain small flakes of mica. Thus 

due to the hydrologic properties of grain boundaries, the 

presence of inclusions may be more significant to the 

deterioration of the stone in buildings than the dissolution of 

the calcite. 

The Salem Limestone has a homogeneous composition and a uniform grain size. Such homogeneity may cause 

the stone to weather more uniformly than the marble and 

eliminate the problems of preferential deterioration. However, although the limestone is mineralogically homogeneous and has matrix and fossil constituents composed of 

calcite, observation of older buildings shows that with time, 

the matrix erodes away preferentially, leaving the fossils 

standing in relief. Similar preferential weathering of fossiliferous limestone has been noted in laboratory experiments 

of weathering, as well (Loughlin, 1929). The fossils may be 

slightly different compositionally from the matrix and thus 

more resistant. The analyses of the fossils and matrix in our 

limestone samples show minor variations of some elements, 

particularly magnesium and strontium (table 17). However, 

the amounts are small, and the variations in composition are 

irregular; no fossil type is consistently higher in minor 

amounts of an element than another fossil type or than the 

matrix. The calcite in the fossil fragments has a pitted 

appearance in polished section compared with the calcite 

that forms the matrix; the pitting indicates that the fossils 

were slightly more resistant to the grinding and polishing 

used in making the sections. Such resistance may be similar 

to the resistance the fossils show when exposed to weathFigure 178. Close up of the pitting in the bryozoan stem 

in A. Calcite (Cc) is light gray, quartz (Q) is darker gray, 

hematite (H) is white, fine black areas are pitting, and 

large continuous black areas are pore spaces. 

ering conditions. Some fossil fragments, particularly echinoderm columnals and bryozoan stems, contain very small 

quartz grains and (or) very small hematite(?) grains that also 

may cause those fossils to be slightly more resistant to 

weathering. Loughlin (1929) cited an example of silicified 

coral shells in a limestone building in New York City that 

protrude as much as I!J6 of an inch above the building 

surface after 40 years of exposure. Carbonaceous material 

within the fossils also may make the fossils more resistant to 

dissolution than the surrounding calcite matrix. 

Porosity is another important characteristic of limestone that may lead to accelerated or preferential weathering. Limestone is much more porous than marble, thus 

giving weathering agents access to more surface area and 

increasing the likelihood that matrix calcite will dissolve 

Fe 

Si 

c 

0 10.24 Kev 

Figure 17C. Energy dispersive spectra of bright white 

inclusion in B, showing that it is composed mostly of iron. 

A small calcium peak is probably due to overlap with 

calcite; the silica peak may be an impurity or may signify 

that there is minor quartz. 

22 Mineralogical Characterization of the Shelburne Marble and the Salem Limestone-Test Stones Used to Study the Effects of Acid Rain 
Figure 18. Grooves in a column of the jefferson Memorial, Washington , D.C., mimic the dark inclusion pattern 

in the Shelburne Marble and may indicate preferential 

weathering of inclusions or weathering along inclusionmatrix boundaries in the marble. The column is approximately 3 ft in diameter. 

preferentially to the fossil fragments. The matrix calcite fills 

the spaces between the fossil fragments, the same areas that 

form the connected pore space. In addition to providing 

easy access for water, the pore space in the limestone also 

provides places where salts can precipitate within the stone 

(Ross and others, 1989). The pressure of growing salts and 

the pressure from alternate freezing and thawing of ice in 

cracks may lead to the spalling of portions of stone from 

buildings (Lewin, 1982; Amoroso and Fassina, 1983). 

SUMMARY 

The Salem Limestone and the Shelburne Marble are 

representative of limestones and marbles commonly used in 

buildings and monuments. Both stones are composed pre-v 

dominantly of calcite. The Salem Limestone is homogeneous in composition and mineralogic characteristics 

throughout the test block. The Shelburne Marble has 

compositionally homogeneous mineral phases, but the distribution of those phases within the test block is random. 

The mineralogy and physical characteristics of the Shelburne Marble and Salem Limestone test blocks described in 

this study provide a baseline for future studies of the 

weathering behavior of these stones. It is particularly 

important to note that the two test stones that were chosen 

are relatively homogeneous in their characteristics, so that 

changes that are found in the stones after their exposure at 

the test sites can be attributed to their exposure experiences 

and not to individual differences in the samples. Because 

the Shelburne Marble and the Salem Limestone are representative ,of typical commercial marbles and limestones, 

they are likely to be useful in a consortium study of the 

effects of acid precipitation on these two types of building 

stones. 

ACKNOWLEDGMENTS 

This research is included within and was funded by 

the National Acid Precipitation Assessment Program. 

REFERENCES CITED 

Accardo, G., Cassano, R., Rossi-Doria, P., Sammuri, P., and 

Tabasso, M., 1981, Screening of products and methods for 

the consolidation of marble, in Rossi-Manaresi, Raffaella, 

ed., The conservation of stone, II, pt. B, Treatment, Proceedings of the International Symposium, Bologna, October 

27- 30, 1981: Bologna, Italy, Centro Per la Conservazione 

delle Sculture All'Aperto, p. 721- 735. 

Albee, A.L., and Ray, Lily, 1970, Correction factors for electron 

probe microanalysis of silicates, oxides, carbonates, phosphates, and sulfates: Analytical Chemistry, v. 42, no. 12, p. 

1408- 1414. 

Amoroso, G.G., and Fassina, Vasco, 1983, Materials science 

monographs, no. 11, Stone decay and conservation: New 

York, Elsevier, 453 p. 

Armbruster, F.E., Brown, W.M., and Yokelson, Doris, 1983, A 

perspective on current acid rain issues: Croton-on-Hudson, 

New York, Hudson Institute, 146 p. 

Babich, Harvey, Davis, D.L., and Stotzky, Guenther, 1980, Acid 

precipitation: Causes and consequences: Environment, v. 22, 

no. 4, p. 6- 13, 40-41. 

Bain, G.W., 1933, The Vermont marble belt, 16th International 

Geologic Congress Guidebook 1, Eastern New York and 

Western New England: Washington, D.C., U.S. Government 

Printing Office, p. 75- 80. 

---1934, Calcite marble: Economic Geology, v. 29, no. 2, 

p. 121-139. 

---1941, Geological, chemical and physical problems in the 

marble industry: Transactions of the American Institute of 

Mining and Metallurgical Engineers, v. 144 (Mining Geology), p. 324- 339. 

---1959, Trip D: Geology of the marble deposits near Rutland, in Zen, E-an, ed., New England Intercollegiate Geological Conference, 51st Annual Meeting, Rutland, Vt., 

References Cited 23 
1959, Stratigraphy and structure of west-central Vermont and 

adjacent New York, p. 35-41. 

Bence, A. E., and Albee, A.L., 1968, Empirical correction factors 

for the electron microanalysis of silicates and oxides: Journal 

of Geology, v. 76, no. 4, p. 382-403. 

Butlin, R.N., Cooke, R.U., Jaynes, S.M., and Sharp, A.S., 

1985, Research on limestone decay in the United Kingdom, 

Proceedings, Fifth International Congress on Deterioration 

and Conservation of Stone, Lausanne, September 25-27, 

1985, v. 1, pt. 3, Air pollution and weathering: Lausanne, 

Switzerland, Presses Polytechniques Romandes, p. 537-546. 

Castro, E. de, 1981, Quelques etudes sur 1' efficacite et la 

durabilite de deux traitements appliques a un calcaire [Several 

studies on the effectiveness and durability of two treatments 

applied to a limestone], in Rossi-Manaresi, Raffaella, ed., 

The conservation of stone, II, pt. B, Treatment, Proceedings 

of the International Symposium, Bologna, October 27-30, 

1981: Bologna, Italy, Centro Per la Conservazione delle 

Sculture All'Aperto, p. 633-643. 

Colby, J. W., 1968, Quantitative microprobe analysis of thin 

insulating films: Advances in X-ray analysis: New York, 

Plenum Press, v. 11, p. 287-305. 

Dale, T.N., 1912, The commercial marbles of western Vermont: 

U.S. Geological Survey Bulletin 521, 170 p. 

---1914, The commercial marbles of western Vermont, in 

Report of the State Geologist, Vermont (1913-1914): Burlington, Vermont, Vermont Geological Survey, p. 1-160. 

Donahue, J.D., 1967, Depositional environments of the Salem 

Limestone (Mississippian, Meramec) of south-central Indiana: New York, Columbia University, Ph.D. thesis, 109 p. 

Esbert, R.M., Ordaz, J., Alonso, F.J., and Alba, J.M., 1981, 

Petrographic and physical study of the building stones from 

Leon Cathedral (Spain), in Rossi-Manaresi, Raffaella, ed., 

The conservation of stone, II, pt. A, Deterioration, Proceedings of the International Symposium, Bologna, October 

27-30, 1981: Bologna, Italy, Centro Per la Conservazione 

delle Sculture All' Aperto, p. 285-298. 

Flinn, D.R., Cramer, S.D., and Carter, J.P., 1985, Field exposure 

study for determining the effects of acid deposition on the 

corrosion and deterioration of materials-Description of program and preliminary results: Durability of Building Materials, v. 3, p. 147-175. 

Flohr, M.J.K., 1983, BASIC programs for the calculation of 

cation site occupancies and plotting of mineral data with 

applications for evaluation of metamorphic mineral assemblages: U.S. Geological Survey Open-File Report 83-905, 

65 p. 

Franks, John, 1983, Acid rain: Chemistry in Britain, v. 19, no. 6, 

p. 504-509. 

Gauri, K.L., 1978, The preservation of stone: Scientific American, v. 238, no. 6, p. 126-136. 

Guidobaldi, F., 1981, Acid rain and corrosion of marble-An 

experimental approach, in Rossi-Manaresi, Raffaella, ed., 

The conservation of stone, II, pt. A, Deterioration, Proceedings of the International Symposium, Bologna, October 

27-30, 1981: Bologna, Italy, Centro Perla Conservazione 

delle Sculture All' Aperto, p. 483-497. 

Hall, J., 1858, Descriptions of new species of fossils from the 

Carboniferous limestone of Indiana and Illinois: Albany 

Institute Transactions, v. 4, p. 1-36. 

Hopkins, T.C., and Siebenthal, C.E., 1896, The Bedford oolitic 

limestone of Indiana: Indiana Geological Survey Annual 

Report 21 , p. 289-427. 

Julien, A.A., 1884, Report on the building stones of the United 

States, and statistics of the quarry industry for 1880: lOth 

Census of the United States, v. 10, p. 364-393. 

Kessler, D.W., 1919, Physical and chemical tests on the commercial marbles of the United States: Technologic Papers of the 

Bureau of Standards, no. 123, 54 p. 

Kessler, D.W., and Sligh, W.H., 1927, Physical properties of the 

principal commercial limestones used for building construction in the United States: Technologic Papers of the Bureau of 

Standards, no. 349, 93 p. 

Lal, B.B., 1985, Weathering and disintegration of stone monuments, Proceedings, Fifth International Congress on Deterioration and Conservation of Stone, Lausanne, September 

25-27, 1985, v. 1, pt. 2, Physical and chemical weathering: 

Lausanne, Switzerland, Presses Polytechniques Romandes, 

p. 213-222. 

Lewin, S.Z., 1982, The mechanism of masonry decay through 

crystallization, in Conservation of historic stone buildings 

and monuments: Washington, D.C., National Academy 

Press, p. 120-144. 

Lewin, S.Z., and Charola, A.E., 1981, Stone decay due to foreign 

inclusions, in Rossi-Manaresi, Raffaella, ed., The conservation of stone, II, pt. A, Deterioration, Proceedings of the 

International Symposium, Bologna, October 27-30, 1981: 

Bologna, Italy, Centro Per la Conservazione delle Sculture 

All' Aperto, p. 205-217. 

Likens, G.E., Wright, R.F., Galloway, J.N., and Butler, T.J., 

1979, Acid rain: Scientific American, v. 241, no. 4, 

p. 43-51. 

Loughlin, G.F., 1929, Indiana oolitic limestone: Relation of its 

natural features to its commercial grading: U.S. Geological 

Survey Bulletin 811, p. 113-202. 

McGee, J.J., 1983, $ANBA-A rapid, combined data acquisition 

and correction program for the SEMQ electron microprobe: 

U.S. Geological Survey Open-File Report 83-817, 45 p. 

Meade, L.P., 1980, The Vermont marble belt and the economics 

of current operations: Bulletin of the New York State 

Museum, v. 436, p. 54-56. 

National Acid Precipitation Assessment Program, 1984, Interagency task force on acid precipitation, 1984 annual report to 

the President and Congress: Washington, D.C., National 

Precipitation Assessment Program, 102 p. 

National Park Service and Argonne National Laboratory, 1988, 

Acid rain site management plan for dimension stone: Washington, D.C., v. 2, unpaginated. 

Oilier, C.D., 1975, Weathering: London, Longman Group Limited, 304 p. 

Patton, J.B., and Carr, D.D., 1982, The Salem Limestone in the 

Indiana building-stone district: Department of Natural 

Resources Geological Survey Occasional Paper 38, 31 p. 

Pearce, Fred, 1985, Acid eats into Britain's stone heritage: New 

Scientist, v. 107, no. 1475, September 26, 1985, p. 26-27. 

Peterson, Ivars, 1985, A material loss: Science News, v. 128, no. 

10, p. 154-156. 

Reddy, M.M., Sherwood, S.I., and Doe, B.R., 1986, Limestone 

and marble dissolution by acid rain-An onsite weathering 

experiment, in Baboian, Robert, ed., Materials degradation 

24 Mineralogical Characterization of the Shelburne Marble and the Salem Limestone-Test Stones Used to Study the Effects of Acid Rain 
caused by acid rain: Washington, D.C., American Chemical 

Society, ACS Symposium Series 318, p. 226-238. 

Reiche, Parry, 1950, A survey of weathering processes and 

products: University of New Mexico Publications in Geology, no. 3, 95 p. 

Rooney, L.F., 1970, Dimension limestone resources of Indiana: 

Department of Natural Resources, Indiana Geological Survey 

Bulletin 42-C, 29 p. 

Ross, Malcolm, 1985, Description, selection, and procurement of 

Shelburne Marble samples used to study effects of acid rain: 

U.S. Geological Survey Open-File Report 85-594, 15 p. 

Ross, Malcolm, and Knab, Larry, 1984, Selection, procurement, 

and description of Salem Limestone samples used to study 

effects of acid rain: Washington, D.C., National Bureau of 

Standards, NBSIR 84-2905, 17 p. 

Ross, Malcolm, McGee, E.S., and Ross, D.R., 1989, Chemical 

and mineralogical effects of acid deposition on Shelburne 

Marble and Salem Limestone test samples placed at four 

NAPAP weather-monitoring sites: American Mineralogist, v. 

74, nos. 3 and 4, p. 367-383. 

Schaffer, R.J., 1932, The weathering of natural building stones: 

London, Department of Scientific and Industrial Research 

Building Research, His Majesty's Stationery Office, Special 

Report no. 18, 149 p. 

Sherwood, S.I., 1984, The National Park Service research program on the effects of air pollution on cultural properties: 

Preprint from Proceedings, 77th Annual Meeting of the Air 

Pollution Control Association, June 24-29, 1984, 84-83.1, 

p. 1-15. 

Sherwood, S. I. , and Doe, B. R. , 1984, Acid rain stone test sites: 

Eos, Transactions, American Geophysical Union, v. 65, p. 

1210. 

Skoulikidis, T.N., 1982, Atmospheric corrosion of concrete 

reinforcements, limestones, and marbles, in Ailor, W.H., 

ed., Atmospheric corrosion: New York, Wiley Interscience, 

p. 807-825. 

Skoulikidis, T.N., and Beloyannis, N., 1981, Inversion de la 

sulfatation du marbre; reconversion en CaC03 du gypse 

forn1e sur les surfaces des monuments et des statues [Reversal 

of the sulphation of marble; reconversion to CaC03 of 

gypsum formed on the surfaces of monuments and statues], in 

Rossi-Manaresi, Raffaella, ed., The conservation of stone, 

II, pt. A, Deterioration, Proceedings of the International 

Symposium, Bologna, October 27-30, 1981: Bologna, Italy, 

Centro Per la Conservazione delle Sculture All'Aperto, p. 

545-558. 

Smith, N .M., 1962, Applied sedimentology of the Salem Limestone: Indiana University, Ph.D. thesis, 126 p. 

---1966, Sedimentology of the Salem Limestone in Indiana: 

Ohio Journal of Science, v. 66, no. 2, p. 168-179. 

---1970, Salem Limestone, in Shaver, R.H., and others, 

Compendium of rock-unit stratigraphy in Indiana: Indiana 

Geological Survey Bulletin 43, p. 152-155. 

Udden, J.A., 1909, The oolitic limestone industry in Bedford and 

Bloomington, Indiana: U.S. Geological Survey Bulletin 430, 

p. 335-345. 

Winkler, E.M., 1973, Stone: Properties, durability in man's 

environment: New York, Springer-Verlag, 230 p. 

References Cited 25 



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