January 1985
                           PROPERTY J
                            • DIVISICs
                                OF
EFFECTS OF ACZD DEPOSITION  08  THE  PROPERTIES
         OF PORTLAND CEMENT CONCRETE
             STATE-OF-KNOVLEDGE
  ATMOSPHERIC SCIENCES RESEARCH LABORATORY
     OFFICE OF RESEARCH AND DEVELOPMENT
    U.S. ENVIRONMENTAL PROTECTION AGENCY
RESEARCH TRIANGLE PARK, NORTH CAROLINA 27711

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    EFFECTS OF ACID DEPOSITION  ON  THE  PROPERTIES
             OF PORTLAND CEMENT  CONCRETE
                 STATE-OF-KNOWLEDGE
           R. P. Webster  and L.  E. Kukacka
           Brookhaven National Laboratory
                  Upton,  NY  11973
                  DW899307010-01-0
                   Project Officer

                   John W. Spence
Emissions Measurement an.d Characterization Division
      Atmospheric Sciences Research Laboratory
          Research Triangle Park, NC  27711
      ATMOSPHERIC SCIENCES RESEARCH LABORATORY
         OFFICE OF RESEARCH AND DEVELOPMENT
        U.S. ENVIRONMENTAL PROTECTION AGENCY
    RESEARCH TRIANGLE PARK, NORTH CAROLINA 27711

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                            NOTICE
     The information in this document has been funded wholly
by the United States Environmental Protection Agency under
Interagency Agreement DW899307010-01-0 to Brookhaven National
Laboratory.  It has been subject to the Agency's peer and
administrative review, and it has been approved for publica-
tion as an EPA document.  Mention of trade names or commercial
products does not constitute endorsement or recommendation  for
use.
                               ii ,

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                           ABSTRACT

     Presented are  the results  of  a  program  conducted to
determine the state-of-the-art  knowledge  pertaining to the
effects of acid deposition on the  properties  of  portland cement
concrete structures.  Information  was  collected  from a comput-
erized literature survey, interviews,  and  replies  to mail and
telephone inquiries addressed to cement and  concrete research-
ers and to governmental agencies and private  firms  active in
the maintenance and restoration of concrete  structures.   In
general, the study  revealed very little qualitative or quanti-
tative information  on the effects  of acid  deposition on  PCC
structures.   The rate of deterioration of  reinforced PCC struc-
tures in polluted areas, however,  appears  to  be  increasing, and
available information makes it  readily apparent  that acids and
acid waters significantly affect the durability  of  concrete,
and that SC>2» NOX>  and HC1 accelerate  the  corrosion of
reinforcing steel.
                              iii

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                           CONTENTS

Abstract	ill
Abbreviations and Symbols	   vi
  1.  Introduction 	    1
          Background 	    I
          Program Objectives 	    1
          Program Summary  	    2
  2.  Conclusions and Recommendations   	  .....    6
  3.  State-of-the-Art Review   	    8
          Background 	  .....    8
          Literature Survey. ........  	    8
          a. General Summary 	    8
          b. Resistance of Concrete  to  Chemical Attack  .  .   11
             Effects of Acids	11
             Effects of Carbon Dioxide  	   15
             Effects of Sulfur Dioxide  	   17
             Effects of Nitrogen Oxides   	   20
          Mail and Telephone Inquiries	20
          Summary	22
References   	24
Appendices	29
  A.  Summaries of Selected References  	   29
  B.  Individuals and Organizations  Surveyed  	   35
  C.  Letter of Inquiry	37

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               LIST OF ABBREVIATIONS  AND  SYMBOLS
ABBREVIATIONS
PCC

SYMBOLS

C3A
CaC03
Ca(OH)2
CaS04
C1,C1-
G02
H2S03
H2S04
HC1
HN02
HN03
NH3
N03,N03~
NOX
S02
S03 ,S03-2
S04,S04-2
sox
Portland cement concrete
tricalcium aluminate
calcium carbonate
calcium hydroxide, i.e.  lime
calcium sulfate, i.e. gypsum
chlorine, or chloride
carbon dioxide
sulfurous acid
sulfuric acid
hydrochloric acid
nitrous acid
nitric acid
ammonia
nitrate
nitrogen oxides
sulfur dioxide
sulfi te
sulfate
sulfur oxides
                               vi

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                            SECTION  1
                          INTRODUCTION

BACKGROUND
     Over the last 25 years, an  increasing  amount of evidence
has been gathered indicating that acid  deposition,  resulting
from the emission of oxides of  sulfur and nitrogen  into the
atmosphere, has a significantly  adverse  effect upon man's en-
vironment including  the acidification of lakes,  rivers and
groundwaters, acidification and  demineralization of soils, re-
duction of forest productivity,  damage  to crops, and deterio-
ration of building materials.(*"''  Although much of this
evidence pertains to the  effects of acid deposition on the
natural environment, i.e.  lakes, rivers,  forests and crops, it
is becoming increasingly  clear  that acid deposition has a sig-
nificant impact also on the durability  of building  materials
such as metals, masonry,  bui.lding stone,  and concrete.  Since
concrete is the most widely used construction material in the
United States, any comprehensive assessment of the  economic
impact of acid deposition  on materials  should include consider-
ation of portland cement  concrete (PCC)  and steel reinforced
PCC.  To this end, Brookhaven National  Laboratory (BNL) has
carried out a program as  part of the National Acid  Precipita-
tion Assessment Program (NAPAP)  Task Force  Project  G3-1.05,
sponsored by the Environmental Protection Agency/Atmospheric
Sciences Research Laboratory (EPA/ASRL),  entitled "Effects of
Acid Deposition on the Properties of Reinforced  Portland Cement
Concrete Structures."

PROGRAM OBJECTIVES
     The specific objectives of  the BNL  program  were (a) to
determine the state-of-the-art-knowledge  pertaining to the
effects of acid deposition  on the properties of  portland

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cement concrete (FCC), and (b) if  the  results  indicated  a need
for quantitative data, to develop  recommendations  for  an exper-
imental test program  to be submitted for Task  Group  G  approval
and implementation.

PROGRAM SUMMARY
     This report presents a summary of  the  state-of-knowledge
pertaining to the effects of acid  deposition on  the  properties
of portland cement concrete.  Information for  this  review was
obtained from a computerized literature survey,  interviews,  and
replies to mail and telephone inquiries addressed  to cement  and
concrete researchers  and  to governmental agencies  and  private
firms active in the maintenance and restoration  of  concrete
structures.
     In general, the  computerized  literature survey  indicated
that an abundance of  literature on acid precipitation  is avail-
able, but most of it  deals with the chemistry  of acid  precipi-
tation and its effects on the natural  environment.   Literature
dealing with the effects  on buildings  and building  materials
does exist, however,  very little  of it  deals with  the  effects
on cement or concrete.  The information that was found
regarding the effects of  acid deposition on buildings  and
building materials, however, indicates  that the  increasing
acidity of precipitation  enhances  normal weathering  and  corro-
sion processes.  In addition, private  communications indicated
that a rapidly increasing number  of reinforced concrete  struc-
tures in cities are showing deterioration which  the  respondents
attributed to S02, NOX, and HC1.
     Because the literature on  the effects  of  acid deposition
on PCC is limited, the large amount of  literature  dealing with
the corrosive effects of  acids, acid waters, and  sulfates on
concrete was reviewed in  an attempt to  estimate  the  effects  of
acid deposition on PCC.

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     This review indicated  that  acid  solutions generally attack
concrete in a combination of  four  ways:  (a)  by dissolving both
hydrated and unhydrated  cement compounds  present in the cement
paste, (b) by dissolving calcareous aggregates present in the
composite, (c) through physical  stresses  induced by sulfate and
nitrate salts crystallized  within  the  pore  structure,  and (d)
by salt-induced corrosion of  the  reinforcing steel.
     The first two forms of attack involve  the same mechanism:
the leaching away of water-soluble salts  formed by reaction of
the acid with the calcium compounds present  in the cement paste
and aggregate.  This is  one of the major  mechanisms of the
deterioration of many ancient statues,  monuments, and  buildings
made with calcareous building stone in  and  near industrialized
areas of Europe.
     The latter two forms of  attack involve  the development of
stresses within the pores of  the  cement paste or aggregate
which eventually cause the  concrete to  crack or spall.  These
stresses result from the crystallization  of  salts that have
accumulated beneath the  surface  of the  concrete or from salt-
induced corrosion of the reinforcing  steel.
     In addition to the  forms of  deterioration identified
above, the cracking and  spalling  of concrete due to acid-
induced corrosion can also  lead  to and  accelerate other forms
of deterioration, most notably freeze-thaw  deterioration.
     The literature review  concentrated on  the effects of three
specific pollutants; carbon dioxide,  sulfur  dioxide,  and nitro-
gen oxides.
     Carbon dioxide was  found to  affect concrete in two ways;
through carbonation of the  concrete surface  and carbonic acid
attack.  The carbonation of the  concrete  surface results in a
decrease of the pH value of the  cement  paste which eventually
leads to the corrosion of the reinforcing steel near the

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surface.  Carbonic acid attack primarily  results  in  the  leach-
ing of calcium hydroxide from the  surface and  interior  of  the
concrete.
     Sulfur dioxide, when dry, has  little or no  effect  on  dry
concrete.  It does, however, combine with water  and  oxygen to
form sulfurous and sulfuric acid,  both  of which  will attack
concrete.  Sulfuric acid attacks concrete (a)  by  converting
calcium carbonate  to gypsum, which  is subsequently  leached
away, and (b) by reacting with calcium  compounds  to  form salts
which crystallize, producing enormous stresses within the  pores
of the cement paste which eventually lead to spalling and
cracking.  The latter form of attack is commonly  known  as  sul-
fate attack.
     Very little information was available  regarding the ef-
fects of nitrogen  oxides on concrete.   They do,  however, react
with water or, as  ammonia, with oxygen  to form nitrous  and
nitric acid.  Nitric acid is not as strong  as  sulfuric  acid,
however, it is destructive enough  to bring  about  extensive
deterioration even in highly diluted solutions,  primarily
through the transformation of calcium hydroxide  into highly
soluble calcium nitrate.
     None of  the individuals and organizations responding  to
the mail and  telephone  inquiries was aware  of  any documented
information dealing specifically with the effects of acid
deposition on PCC  structures, or of any research  that had  been
or was being  done  in this area.  Comments on  the  need for  such
research work were varied: some respondents thought  it  was
needed because the large volume of  concrete structures  in  the
United States could present a potentially large  problem;
others thought the need for such research was  open  to question
because they  considered other mechanisms  of deterioration  to
be more important.

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     The study revealed very  little qualitative  or  quantitative
information on the effects of acid deposition on PCC  structures.
The rate of deterioration of  reinforced PCC  structures  in  pol-
luted areas, however, appears to be increasing,  and available
information makes it readily  apparent  that acids and  acid
waters significantly affect the durability of concrete,  and
that S02» NOX, and HC1 accelerate the  corrosion  of  reinforcing
s tee 1.

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                           SECTION  2
                CONCLUSIONS AND RECOMMENDATIONS

     The results of the literature  survey,  private  discussions,
and the responses to mail and  telephone  inquiries  have  indica-
ted that very little qualitative  or quantitative  information is
available dealing specifically with the  effects  of  acid deposi-
tion on PCC structures, but there is a considerable amount of
information available  indicating  that acids  and  acid waters
have a significant effect on the  durability  of  concrete.   This
effect may not be sudden or dramatic, but  it is  a  cause for
concern.
     It has been well  documented  that high  levels  of pollutants
(S02, N0x> etc«) have  greatly  accelerated  the  deterioration of
many of the ancient statues, monuments,  and  buildings made
using calcareous building stone in  and near  the  industrialized
areas of Europe.  Evidence is  now beginning  to  indicate that
rapidly increasing numbers of  reinforced concrete  structures
are also showing increased rates  of deterioration  which are
attributed by some to  be due to exposure to  high  levels of S02»
NOX, and HC1.
     On the basis of this evidence, it is  recommended that an
experimental test program, consisting of both  laboratory and
field tests, be developed and  implemented  to quantitatively
measure the effects of acid deposition on  PCC  structures.   It
is, however, recommended that  a preliminary  series  of acceler-
ated laboratory tests  be carried  out before  a  full-scale field
evaluation program is  instituted.   The objectives  of the labor-
atory test program should be to identify the magnitude  of  the
problem and to attempt to differentiate  between  the effects of
wet deposition, dry deposition, and normal  weathering.   Para-
meters to be studied in the test  program should  include:

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     wet deposition    - various  simulated  acid  rain mixtures
                         to differentiate between  the effects
                         of 804,  ^03, and the  normal background
                         components of  rain.
                       - simulated acid  rain mixtures of
                         varying  pH values.
     dry deposition    - various  levels  of  S(>2 and  NOX.
                       - various  relative humidities.
     normal weathering - freeze-thaw  cycles.
     Test methods used in  the evaluation should  include;  (a)
tests to evaluate changes  in the  physical and  mechanical
properties of the specimens, (b)  chemical analyses  to determine
the depth and rate of penetration of  the aggressive solutions,
and (c) tests to monitor and control  the treatment  solutions
and to analyze them for materials being  leached  from the test
specimens.

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                           SECTION 3
                    STATE-OF-THE-ART REVIEW

BACKGROUND
     Information pertaining to the effects of  acid  deposition
on the properties of portland cement concrete  was obtained  (a)
from a computerized literature survey, and (b)  from mail  and
telephone inquiries, and meetings with cement  and concrete
researchers, and from government agencies and  private  firms
active in the maintenance and restoration of concrete  struc-
tures.
     The information collected in these  surveys  was used  to
determine:  (a) if data exist regarding  problems associated
with the effects of acid deposition on PCC, and  what the  econo-
mic impact of these problems may be, (b) if any  research  work
has been or is being done to investigate the effects associated
with acid deposition, and (c) if there is a need for experimen-
tal work to be done in this area.  Results of  each  survey are
summarized below.

LITERATURE SURVEY
General Summary
     In the computerized literature survey, ten  data bases,
listed in Table 1, were searched for information on acids,
acid deposition, and portland cement concrete.   A  total  of  132
papers and reports were collected and  reviewed.  In general,
this literature dealt with one of four subject areas;  (a) the
chemistry of acid precipitation, (b) the effects of acid  depo-
sition on the natural environment, (c) the effects  of  acid
deposition on buildings and building materials,  and (d)  the
effects of acids and acid waters on concrete.   The  survey

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   Table 1. DATA BASES USED IN COMPUTERIZED  LITERATURE  SEARCH
    Data Base
                          Supplier
Dates Covered
CA SEARCH

CAB ABSTRACTS


COMPENDEX

DOE ENERGY



ENVIROLINE

ENVIRONMENTAL
  BIBLIOGRAPHY

NTIS
PAIS
  INTERNATIONAL

POLLUTION
  ABSTRACTS

SCISEARCH
                  Chemical Abstracts Service

                  Commonwealth Agricultural
                    Bureau

                  Engineering Info., Inc.

                  Office of Scientific and
                    Technical Information
                    (OSTI)

                  Environmental Info., Inc.

                  Environmental Studies Inst.
                  National Technical Info.
                    Service

                  Public Affairs Information
                    Service, Inc.

                  Cambridge Scientific
                    Abstracts

                  ISI Inc.
   1980-81

1972-1983/Dec.


1970-1983/Aug.

1974-1984/Mar.



1970-1984/Mar.

1974-1983/Oct.


1964-1983/Iss25


1976-1984/Apr.


1970-1983/Dec.


1981-1984/Mar.
Keywords:  acid rain, acid precipitation, acid  deposition,
           cement, portland cement, concrete, buildings,
           structures, deterioration, building  materials
revealed an abundance of literature on acid  precipitation,  but

most of it deals with the chemistry and  effects  on  the  natural

environment.  Some of the papers  include  general  statements

indicating that the increasing acidity of precipitation enhan-

ces the weathering and corrosion  of materials  and buildings,
but nothing any more speci f ic .
                                   )
                                      por  example, Trumbule
and Tedeschl(12) state: "Acid rain also  is believed  to  cause

damage to buildings and other manmade  structures.  One  estimate

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places damage to structures in the eastern  third  of  the  United
States from acid rain at $2 billion per year  in 1978  dollars."
They do not, however, cite any supporting data or  damage
functions describing the deterioration.  Martin'^) also  makes
a similar statement.
     The literature also indicates that while it  is  felt,  by
some, that acid precipitation does have an  adverse effect  on
the performance of building materials, no work apparently  is
being done to investigate these effects.  Ashton  and
Sereda^1^) report that:  "Monitoring of the concentration  of
pollutants in the atmosphere and  in rain is done  by  various
government agencies in many countries, but  little  effort is
directed to the study of their effect  on building  materials,
particularly that of acidic components in rainwater."
     Of the articles reviewed, ~20% dealt with the effects of
acid deposition on buildings and  building materials,  and most
of those dealt with its effects on natural  building  stones
(marble, limestone, sandstone) and metals (steel,  iron,  alumi-
num). (14-27)  Only references 4,  5, and 23-27 dealt  directly
with the effects of acid deposition on cement or  concrete.
Each of these is summarized in Appendix A.
     Because the literature on the effects  of acid deposition
on PCC is limited, the large amount of literature  dealing  with
the corrosive effects of acids, acid waters,  and  sulfates  on
concre te( 28-54) wag use
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Resistance of Concrete  to  Chemical  Attack

Effects of Acids -
     Since concrete, chemically,  is a  basic  material,  having a
pH of about 13, it  is subject  to  attack  by  acids.   Woods(37)
reports that concrete is not very resistant  to  strong  solutions
of sulfuric, sulfurous, hydrochloric,  nitric,  hydrobromic,  or
hydrofluoric acids, and is  destroyed by  prolonged  contact with
any of these, though not necessarily at  the  same  rate.   Weaker
solutions (<1%) attack  concrete at  a slower  rate,  but  in some
cases the severity  of the  attack  can be  very significant.
Woods further states that  for  all practical  purposes,  an acid-
ity of pH 5.5 to 6  may  be  considered the limit  of  tolerance of
high quality concrete in contact  with  any  of these acids,
although the pH value is not invariably  a  good  criterion of the
aggressiveness of acids.   The  chemical composition of  the acid
is at least as important as pH  in influencing  the  rate  a.t which
concrete is attacked.
     Galloway^1) reports that  the relative  contribution of
H2S04, HN03, and HC1 to the acidity of precipitation is
difficult to determine  because  the  acids are not  present as
such in solution but rather as  dissociated  ions.   However,
using the absolute  concentration  of 804, NC>3 and  Cl it  is
possible to determine their relative contribution.  Likens  and
Bormann^2) and Glass et al^3)  report that  precipitation
data for the northeastern  United  States  indicate  that  60 to 70%
of the acidity in acid  precipitation is  due  to  sulfuric acid,
30 to 40% to nitric acid,  and ~5% to hydrochloric  acid.  For
this reason, the following  discussion  of the effects of acids
on concrete will focus  on  effects of sulfuric  acid.
     In general, acid solutions attack concrete  in any  combi-
nation of four ways: (a) by dissolving both  hydrated and
                               11

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unhydrated cement compounds, (b) by  dissolving  calcareous
aggregates present in the mix, (c) through  physical  stresses
induced by the deposition of soluble  sulfate  and  nitrate salts
and the subsequent formation of new  solid phases  within the
pore structure, and (d) by  salt-induced  corrosion of the
reinforcing steel.
     The first two forms of attack involve  the  same  mechanism:
the leaching away of water-soluble salts  formed by reaction of
the acid with the calcium compounds  in  the  cement paste and
aggregate.  When calcareous materials are attacked by sulfuric
acid, the sulfate radicals  in  the acid  react  with the calcium
carbonate (CaCOj) to produce calcium  sulfate  (CaSO^) , or
gypsum.  Since gypsum is much  more soluble  in water  than cal-
cium carbonate, it is readily  washed  away.  This  process even-
tually results in the complete destruction  and  removal of  any
calcareous material exposed to attack.   Brown(31)f reports
that this is the type of damage observed  on the walls and  floor
of the lock chamber of  the  Holt Lock  and  Dam  near Tuscaloosa,
Alabama, after they were subjected to prolonged contact with
waters having a pH of about 4.2.  The damage  consisted of  a
large number of areas where the limestone coarse  aggregate was
removed from the surface of the concrete  to depths of 0.64 to
1.27 cm (1/4 to 1/2 in.).  The evidence,  collected by the  Corps
of Engineers, indicated that the removal  of the aggregate  was
due to the dissolution  of the  exposed aggregate particles  by
acid or acids in the river  water as  pollution from local strip
mines.  While the source of the acid  may  be different, this
type of deterioration has also been  documented  to be one of the
major mechanisms of the damage occurring  to many  of  the ancient
statues, monuments, and buildings made  with calcareous building
stone in and near industrialized areas  of Europe.(4-6,14-17,
21-23)
                               12

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     Acid attacks  cement  paste  the sane way: it reacts with  the
calcium compounds  in  the  paste,  such as calcium hydroxide and
calcium carbonate,  producing  soluble salts that are easily
leached away.  Gradually,  the acid also attacks the hydrated
minerals in the cement  paste, again producing soluble salts.
The leaching process  results  in  the gradual loss of cement
paste from the surface  of  the concrete and eventual exposure of
the aggregate.  In  addition,  Tremper(30)  reports that the
leaching process is not limited  to the surface of the concrete,
but also extends into the  concrete.  He states that as calcium
carbonate is removed  from  the surface, calcium hydroxide (lime)
diffuses from the  interior to the  surface and is precipitated
as calcium carbonate.   When  calcium hydroxide is thus precipi-
tated, the water held in  the  pores of the concrete becomes un-
saturated and more  calcium hydroxide is taken into solution.
There is thus a continuous travel  of calcium hydroxide from  the
interior to the surface,  resulting in a general loss of lime
throughout the body of  the concrete.  In  its early stages, this
form of attack is  characterized  by a slight etching of the sur-
face, and, in later stages by severe pitting and scaling,
followed by'a gradual decrease  in  strength.
     The third form of  attack is  a secondary effect of the
first two forms.  The reaction  of  acids with the various cal-
cium compounds present  in  the cement paste or aggregate leaves
a residue of soluble  salts, which  accumulates on or just
beneath the surface. The  salts  at  the surface are leached away
by rainwater, the  salts accumulated beneath the surface can
crystallize with the  absorption  of water, which increases their
volume.  This results in  the  development  of enormous stresses
within the pores of the cement  paste or aggregate, which can
eventually lead to  blistering and  spalling of the surface.  In
addition, some of  the sulfates  formed, such as gypsum, react
                               13

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with the hydra ted tricalcium aluminate  in  the  cement paste to
produce ettringite (3CaO'A1203•3CaS04'31H20) ,  which also
occupies a large volume  and, thus,  can  also  cause  cracking.

     The accumulation of salts beneath  the  surface can also
lead to the formation of crusts  in  protected areas that are
shielded from washing by rainwater.  These  impermeable crusts
can hold water and salts within  their pore  structure,  causing
the concrete or stone to spall off  in layers rather than
gradually eroding.
     Regarding this  type of deterioration,  Fishert4) reports:
"Many scientists think  that acid  deposition  damages buildings
more through the physical stresses  than through  the chemical
reactions it brings  on."
     The accumulation of salts within the  concrete pore struc-
ture can also lead to the corrosion of  reinforcing steel,  the
fourth form of deterioration identified above.   This corrosion
is accompanied by an increase  in  the volume  of the steel,  which
eventually causes the concrete  to  crack and  spall.  In discuss-
ing the atomospheric corrosion of  concrete  reinforcements,
Skoulikidis(25) notes:  "The increase of atmospheric pollution
intensifies the corrosion tendency  of the  reinforcements in  the
atmosphere.  The cracking of the  concrete  was  observed more
frequently with an increase of  the  atmospheric pollution (SC>2,
C02» NH3 , NQX, etc.) and the acceleration  of  the corrosion by
the formation of a more  conductive  environment,  that also
chemically attacks the  metals."
     In addition to  the  forms  of  attack already  discussed,
cracking and spalling of concrete  due to acid-induced corrosion
can also lead to and accelerate  other forms  of attack having
other causes, most notably  freeze-thaw  deterioration.
                                14

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           found that concrete which  normally  withstood
attack due to freeze-thaw cycling was  subject  to  attack after
exposure to acid solutions.

Effects of Carbon Dioxide -
     Concrete is known to be affected  by  the  take-up  of C<>2
from ambient air, i.e. carbonation.<37»39-42)  tfoods<37)
states:  "The reaction between atmospheric  carbon dioxide and
dense hardened concrete is very  slow,  and even after  a  consid-
erable number of years, may affect  only a thin layer  nearest
the exposed surfaces.  A principal  product  of  the reaction is
calcium carbonate, the presence  of  which  may  enhance  the early
resistance of concrete to attack by some  chemicals  in solution,
such as sulfates.  In practice,  however,  any  beneficial effect
that may exist appears to be of  relatively  small  moment."
     The harmful effect of carbonation arises  when  the  carbon-
ated layer created on the surface of  reinforced concrete over
the years reaches the steel reinforcement.  The alkaline pro-
tective layer is then considerably  less alkaline, and the
steel bars may start  to rust.  Sentler'3?)  has determined the
thickness of concrete cover required  to protect the  reinforcing
steel from corrosion as a function  of  the water/cement  (w/c)
ratio.  He finds that for a 50-yr life the  concrete  cover
needed for w/c » 0.4 or 0.8 is 12 or  45 mm  (0.47  or  1.77 in.),
respectively, for a failure probability of  0.05;  and  13 or 51
mm (0.51 or 2.01 in.) for a failure probability of  0.01. These
values are for the carbonation effect  only, without  cracks in
the concrete; if other factors affecting  degradation  are taken
into account, the required thickness  of the cover will  be
greater.
     Carbon dioxide will also react with water to form  carbonic
acid.  There are, however, conflicting data regarding the rate
at which carbonic acid will attack  concrete.
                               15

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     Bertacchi(32) reported,  for  standard  portland  cement
concrete, a weight loss of 287 g/kg  of  concrete  and compressive
and flexural strength reductions  of  -90% after a 7-yr  exposure
to distilled water into which CO2 was  continuously  bubbled and
which was replaced periodically as  the  dissolved lime  content
increased so that its pH varied from ~4 to 5.5.   Tremper'30)
reported reductions  in compressive  strength of 5 to 127. for
portland cement concrete subjected  to  carbonic acid solutions
of pH 6.9 to 6.1, respectively, for  8  months.
     On the other hand, Greschuchna'43)  reports  that a car-
bonic acid solution  saturated at  760 Torr  (14.7  psi) and 25°C
(77°P) has a pH of 3.7, and  that  for pH >3 the corrosion rate
should be hardly greater than that  due  to  leaching  by  pure
water, i.e. the acid effect  becomes  negligible.   There is also
evidence, however, that carbonic  acid  attack is  enhanced by the
presence of suIfates(^*)t
     Tremper'^O) developed a damage  function to  describe the
deterioration observed in his work.  The damage  function, which
is expressed as
                       log L - K-log T,
where L * the percentage of  the original lime  lost  from the
          concre te
      T * the time in days for which the concrete has  been
          exposed
      K » a constant which varies with the pH  of the solution
          to which the concrete is  exposed and  the  surface to
          volume ratio of the concrete
predicts the rate of detrioration due  to acid  attack based upon
the loss of lime from concrete.   Based upon the  results of a
series of laboratory tests,  Tremper  concluded  that  for purposes
of computation  the mechanical failure  of average portland
cement concrete will occur when 50%  of the original lime
                                16

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content has been  removed.   Values  for K are developed based
upon the results  of  the  laboratory tests,  however, Tremper had
to make several assumptions  during the development of these
values, thereby limiting  the  accuracy of the damage function.
Tremper does point out,  however,  that:  "It should be borne in
mind that the results  (using  this  damage function) cannot, in
any event, be expected  to  be  more  than relative measures since
factors other than corrosion  will  generally have their effect
in determining actual  life."   He  also points out that he does
not believe that  data  on  the  quality  of concretes are suffi-
ciently developed to warrent  applying (the damage function) in
more than a general way.
                published  a  series  of  equations for
calculating the depth  of  the  corroded  zone  for concrete spec-
imens exposed to carbonic  acid  attack  as  a  function of the
physical and mechanical properties  of  corroded and noncorroded
specimens, i.e. density, volume,  mass,  modulus of elasticity,
and strength.  The equations,  however,  do not take into consid-
eration such factors as the  composition of  the concrete or the
degree of attack to which  it  is  subjected.   In addition, the
wide variation in  test results,  obtained  from laboratory tests
performed to varify the theoretically  derived equations, limit
their applicability.

Effects of Sulfur Dioxide  -
     Sulfur dioxide, when  dry,  has  little or no effect on dry
PCC.  It does, however, combine  with water  to form sulfurous
acid (^303), which gradually  reacts with oxygen to form sul-
furic acid (t^SC^), both of which will  attack concre te . ( 37 )
Most of the damage to  materials  from SOX  is  attributed to
highly reactive sulfuric acid  formed either  in the atmosphere
or on the surface of materials.   Damage to  limestone products,
                               17

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concrete, and marble have been observed  in  those  areas experi-
encing relatively high levels of 802  over a  prolonged
period.<27>
     As previously discussed, sulfuric acid  attacks  concrete
(a) by converting calcium carbonate  to gypsum,  which is subse-
quently leached away, and (b) by reacting with  calcium com-
pounds to form salts which crystallize,  producing enormous
stresses within the pores of the cement  paste which  eventually
lead to spalling and cracking.  The  latter  form of attack is
commonly known as sulfate attack.  Both  mechanisms of deterior-
ation were identified by Hansen et al(35) in their work
regarding the corrosion of concrete  due  to  sulfuric  acid
attack, in which they conclude that  exposure to sulfuric acid
can progress from a straight corrosive attack  to  a combination
of corrosion and sulfate attack.
     The effects of sulfate attack on portland  cement concrete
have been well documented.<28»29»37•38,45-47,50-54)  Kuenning
(29) describes the mechanism of sulfate  attack  as follows:
"The destructive action of sulfates  on concrete is primarily
the result of their reaction with either CjA err the  C3A hydra-
tion products to form the high-sulfate form  of  calcium sulfo-
aluminate (ettringite).  The crystalline reaction product is of
larger volume than the original aluminate constituent, and
expansion results.  The concrete or  mortar  increases in
strength at first, because of the increase  in  solid  matter,
even though it is changing chemically.   As  the  process contin-
ues the concrete or mortar expands,  cracks,  becomes  progres-
sively weaker, and finally disintegrates."
     Jambor'^'' has published a damage function describing
sulfate attack in terms of the percent of 803  bound  in hardened
cement paste, which he reports as being  the  prime cause of sul-
fate corrosion.  The damage function  (DC) which is expressed as
                               18

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      DC - (0.11s0.45)(0<143t0.33)(0>204e0'145c3M

takes into consideration  the  concentration of the acting sul-
fate solution  (S),  the  period  of  time  of its action (t), and
the tricalcium aluminate  (C^A)  content of the portland cement
used.  The damage function was  developed on the basis of exper-
imental test results which demonstrated the effects, with time,
of sodium sulfate solutions, with  varying 804 concentrations,
on the dynamic modulus  of  elasticity,  compressive and flexural
strength, volumetric and  mass  changes, and changes in the bound
    content of portland cement  mortar  specimens.
     Jambor has, apparently,  been  able  to relate the changes
observed in the physical  and  mechanical  properties of the spec-
imens to changes in  the bound 803  content.   These data, how-
ever, were not given  in the paper.   The  data presented relate
bound 803 content  to  sulfate  concentration,  C3A content, and
time of testing.   It  is these data  upon  which the damage func-
tion was based.  As Jambor  points  out,  the  damage function is
limited in that it does not take  into  account temperature
effects, influence of  the  cement  content in  the mortars and
concrete, total porosity  of the composite material,  as well as
the influence of the  cross- sec tion  size  of  the structure.  It
does, however, serve  to give  a first approximation.
     Even though the  mechanisms are not  fully understood, it
has been fairly well  established  that  802 accelerates the cor-
rosion of carbon stee 1 . (18-20 , 55-57 ) xh£s results in the
creation of a layer  of rust,  i.e.  iron  oxides, on the surface
of the steel, which occupies  more  than  twice the volume of the
iron from which it was produced.   In addition, Haynie and
Upham(19) report that  iron  oxides  catalyze  the oxidation of
802 to 803 as well as  react with  802 to  form sulfates.  Both
                                19

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conditions, i.e. the expansion  of  reinforcing  steel  due to
corrosion and sulfate attack, have  been  shown  to  cause the
deterioration of PCC.

Effects of Nitrogen Oxides -
     Very little information  is  presently  available  in the
literature regarding the effects  of nitrogen oxides  (NOX)  on
PCC.  Gauri^23) reports  that  nitrogen  dioxide  produced
primarily during combustion processes  by the oxidation of
atmospheric nitrogen is  the main  cause of  the  acidity of preci-
pitation in the Los Angeles Basin  where  N03* is  more than  twice
as concentrated as SO^"2.  H0
-------
deposition.  The individuals  and  organizations contacted are
listed in Appendix B;  14 of  them  replied  to the inquiries. The
letter used in the survey  appears  in  Appendix C.
     None of the individuals  replying was  aware of any documen-
ted information dealing specifically  with  the effects of acid
deposition on PCC structures,  although a  few mentioned that
there is some information  about  the effects of acids and acid
waters, as well as about the  effects  of acid deposition on
building stone structures.   No one was aware of any research
that has been or is presently  being done  in this  area.
     The question regarding  the  need  for  experimental work got
varied replies.  Some  thought  that the need for research in
this area was open to  question because other mechanisms of
deterioration, such as freeze-thaw cycling and chloride-induced
corrosion of reinforcing steel by  deicing  salts,  were more
important.  Others thought the need was pressing  because the
large volume of concrete structures in the United States could
present a potentially  large  problem.   In  fact, Mr. 6. W. DePuy
of the Bureau of Reclamation  stated that  the Bureau is cur-
rently in the process  of formulating  a program to determine
which of its projects  are  in  areas with high levels of acid
precipitation so that  it can  evaluate the  need for addressing
the problem of deterioration  due  to acid  precipitation.
     Discussions at the Third  International Conference on the
Durability of Building Materials and  Components held in Espoo,
Finland, August 1984,  disclosed  that  at least one research
effort on the effects  of pollutants on reinforced PCC is in
progress.  The Building Research Institute in Japan is doing
chamber studies with S02 and  CC>2 at two relative  humidities,
50% and 90%, but has not yet  published any results. The goal of
this work is to develop models for predicting deterioration
rates, and to use the  results  in establishing design criteria
for the extension of service  life.
                               21

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     Information from private communications  indicated  that a
rapidly increasing number of reinforced  concrete  structures in
cities are showing deterioration attributed  to  the  presence of
high concentrations of S02» Nox» an<* **C1  in  the atmosphere.
The mechanism appears to be similar  to chloride attack  of  rein-
forced concrete bridge decks.  For example,  in  areas  of South-
east Asia, highly polluted with SC>2  and  NOX,  cracking in at
least 200 buildings was noted after ~*2 yr, and  severe corrosion
occured within 5 yr (e.g. Prof. H. 0. W.  Kim, National  Univer-
sity of Singapore, personal communication, 1984).   In New  York
City, highrise multiple dwellings built  in the  1950s  are show-
ing similar distress.  A staff member of  one  engineering firm
states:  "The deterioration on bridge decks  due to  corrosion is
now being observed in concrete structural members.   Corrosion
of vertical members may take longer  because  of  gravity  drain-
age, but if the materials and conditions  are  similar, corrosion
will take place no matter the angle."

SUMMARY
     The literature survey, private  discussions,  and  responses
to mail and telephone inquiries have revealed very  little
qualitative or quantitative information  on the  effects  of  acid
deposition on PCC structures.  The rate  of deterioration of
reinforced PCC structures in polluted areas  appears to  be
increasing, and available data make  it readily  apparent that
acids and acid waters significantly  affect the  durability  of
concrete.  The immediate effects of  acid  deposition on  PCC may
not be sudden or dramatic, but the available  evidence suggests
that there is cause for concern.  When steel  reinforcement is
used, as it normally  is, the potential for problems is  much
greater because acid  rain or pollutants  eventually  reach the
steel via the capillary porosity in  the  cement  phase  or through
                               22

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cracks and then will initiate corrosion  of  the  steel,  which
subsequently results in cracking and  spalling of  the  concrete.
Dry deposition is anticipated to produce  much greater  effects
than acid rain, or wet deposition, because  it results  in  much
more concentrated forms of attack.  Synergistic  effects  that
accelerate the deterioration are also  presumed  to  occur.
                              23

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                           REFERENCES
 1.   Galloway,  J.  N.   Acid Precipitation:  Spatial and Temporal
     Trends.   Acid Rain, Proceedings of a Symposium Sponsored
     by ASCE,  April 2-6, 1979, 1-20.

 2.   Likens,  G.  E., and F. H.  Bormann.  Acid Rain:  A Serious
     Regional  Environmental Problem.  Science, 184(4142), 1974,
     1176-9.

 3.   Glass, N.  R., et al.  Effects of Acid Precipitation in
     North America.  Environmental International, 4, 1980,
     443-52.

 4.   Fisher,  T.   When the Rain Comes.  Prog. Arch., 7, 1983,
     99-105.

 5.   Stanwood,  L.   Acid Rain,  A Cloudy Issue.  The Construction
     Specifier,  Nov.  1983, 74-9.

 6.   Gauri, K.  L.   Effects of  Acid Rain on Structures.  In:
     Proceedings of a Session  Held at the National Convention,
     ASCE, Boston, MA, April 2, 1979, 70-91.

 7.   Cowling,  E. B.  Acid Precipitation in Historical Perspec-
     tive.  Environ.  Sci. Technol., 16(2), 1982, 110A-123A.

 8.   Martin,  H.  C.  Acid Rain: Impacts on the Natural and Human
     Environment.   Materials Performance, 21(1), Jan. 1982,
     36-9.

 9.   Likens,  G.  E.  Acid Precipitation.  Chem. and Engr. News,
     54(48),  Nov.  22, 1976, 29-44.

10.   Cogbill,  C. V.,  and G. E. Likens.  Acid Precipitation in
     the Northeastern United States.  Water Resources Research,
     10(6), Dec. 1974, 1133-7.

11.   Berry, M.  A., and J. D. Bachmann.  Developing Regulatory
     Programs  for the Control  of Acid Precipitation.  Water,
     Air, and Soil Pollution,  8(1), 1977, 95-103.

12.   Trumbule,  R.  E., and M. Tedeschi.  Acid Rain Information:
     Knee Deep and Rising.  Science   Technology Libraries,
     4(2), Winter 1983, 27-41.

13.   Ashton,  H.  E., and P. J.  Sereda.  Environment, Micro-
     environment and Durability of Building Materials.  Dura-
     bility of Building Materials, 1, 1982, 49-66.
                              24

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14.  Dornberg, J.  The Plaster of Paris Cathedral.  Pan Am
     Clipper, July 1982, 18-22 and 77-9.

15.  Fassina, V.  A Survey on Air Pollution and Deterioration
     of Stonework in Venice.  Atmospheric Environment, 12,
     1978, 2205-11.

16.  Gauri, K. L. and G. C. Holden, Jr.  Pollutant Effects  on
     Stone Monuments.  Environ. Sci. and Technol. 15(4), April
     1981, 386-90.

17.  Longinelli, A. and M. Bartelloni.  Atmospheric Pollution
     in Venice, Italy, As Indicated By Isotopic Analyses.
     Water, Air, and Soil Pollution, (10) 1978, 335-41.

18.  Kucera, V.  Effects of Sulfur Dioxide and Acid Precipita-
     tion on Metals and Anti-Rust Painted Steel.  Ambio, 5(5,6)
     1976, 243-8.

19.  Haynie, F. H. and J. B. Upham.  Effects of Atmospheric
     Pollutants on Corrosion Behavior of Steels.  Materials
     Protection and Performance, 10(11) 1971, 18-21.

20.  Ericsson, R. and T. Sydberger. , Influence of S02»
     Periodical Wetting and Corrosion Products on the
     Atmospheric Corrosion of Steel.  Werkstoffe und Korrosion,
     31, 1980, 455-63.

21.  Schreiber, H.  Air Pollution Effects on Materials.  Report
     for Panel 3 ("Environmental Impact") of the NATO/CCMS
     Pilot Study on Air Pollution Control Strategies and Impact
     Modelling, 1982.

22.  Von Ward, P., ed. Impact of Air Pollutants on Materials.
     A Report of Panel 3 ("Environmental Impact") of the NATO/
     CCMS Pilot Study on Air Pollution Control Strategies and
     Impact Modelling, 1982.

23.  Gauri, K. L.,  Deterioration of Architectural Structures
     and Monuments.  Polluted Rain (Environmental Science
     Research), 17; 1980, 125-45.

24.  Dijkstra, G.  Effects of Air Pollution on the Materials in
     the Netherlands.  Report for Panel 3 ("Environmental
     Impact") of the NATO/CCMS Pilot Study on Air Pollution
     Control Strategies and Impact Modelling, 1982.
                              25

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25.  Skoulikidis, T. N.  Atmospheric Corrosion of Concrete
     Reinforcements, Limestones, and Marbles.  Atmospheric
     Corrosion of Concrete Reinforcements and Their Protection,
     date unknown, 807-25.

26.  Skoulikidis, T. N.  Effect of Primary and Secondary Air
     Pollutants and Acid Depositions on (Ancient and Modern)
     Buildings and Monuments.  In:  Proceedings of Symposium
     and Acid Deposition, A Challenge for Europe, Proceedings
     Preliminary Edition, Sept. 1983, 193-226.

27.  Gillette, D. G.  Sulfur Dioxide and Material Damage.  J.
     Air Pollution Control Assoc., 25(12), Dec. 1975, 1238-43.

28.  Biczok, I.  Concrete Corrosion, Concrete Protection.
     Akademia Kiado, Budapest, 1972.

29.  Kuenning, W. H.  Resistance of Portland Cement Mortar to
     Chemical Attack - A Progress Report.  Highway Research
     Record, (113), 1966, 43-87.

30.  Tremper, B.  The Effect of Acid Waters on Concrete.  ACI
     Journal, 28(1), Sept. 1931, 1-32.

31.  Brown, F. R.  Examination of Surface Concrete from Lock
     Chamber, Holt Lock and Dam near Tuscaloosa, Alabama.
     U.S. Army Corps of Engineers Report, October 6, 1977.

32.  Bertacchi, P.  Deterioration of Concrete Caused by
     Carbonic Acid.  In:  RILEM Symposium, Durability of Con-
     crete-1969, Final Report, Part II, Academia Prague, 1970,
     C159-C168.

33.  M/odecki, J.  Testing the Resistance of Mortars and Con-
     cretes to Acid and Carbonic Acid Attack by Stationary
     Accelerated Method and by Flow Method.  In:  RILEM Sympo-
     sium, Durability of Concrete-1969, Preliminary Report,
     Part II, Academia Prague, 1970, C221-C240.

34.  Prudil, S.  Effect of Combined Actions of Acid and Frost
     on Corrosion of Concrete.  In:  RILEM Symposium, Durabi-
     lity of Concrete-1969, Preliminary Report, Part I, Aca-
     demia Prague, 1970, A59-A68.

35.  Hansen, W. C., et al.  Corrosion of Concrete by Sulfuric
     Acid.  ASTM Bulletin, 231, July 1958, 85-8.

36.  Wong, S. G.  Life Expectancy of Concrete Attacked by Acid.
     Paper for CE 697D, Purdue Univ., 1978.
                              26

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37.  Woods, H.  Durability of Concrete Construction.  ACI
     Monograph Mo. 4, 1968.

38.  Czernin, W.  Cement Chemistry and Physics For Engineers.
     Chemical Publishing Co., New York, NY, 1962.

39.  Sentler, L.  Stochastic Characterization of Carbonation  of
     Concrete.  In:  Proc. Third International Conference  on
     the Durability of Building Materials and Components,
     Espoo, Finland, Vol. 3, Aug. 12-15, 1984, 569-80.

40.  Verbeck, G.  Carbonation of Hydrated Portland Cement.
     ASTM STP-205, 1958, 17-36.

41.  Leber, I. and F. A. Blakey.  Some Effects of Carbon
     Dioxide in Mortars and Concrete.  Journ. Amer. Cone.
     Institute, 53-16, Sept. 1956, 295-308.

42.  Smolczyk, H. G.  New Aspects About Carbonation of  Concrete.
     RILEM Symposium on Durability of Concrete-1969, Preliminary
     Report, Part II, Academia Prague, 1970, D59-D75.

43.  Greschuchna, R.  Concrete Corrosion and Chemical
     Equilibrium.  In:  RILEM Symposium, Durability of
     Concrete-1969, Final Report, Part II, Academia Prague,
     1970, C189-C191.

44.  Idorn, G. M.  Durability of Concrete Structures in
     Denmark. Ph.D. Thesis, Technical University of Denmark,
     1967.

45.  Brown, P. W.  An Evaluation of the Sulfate Resistance of
     Cements in a Controlled Environment.  Cement and Concrete
     Research, 11, 1981, 719-27.

46.  Heller, L., and M. Ben-Yair.  Effect of Sulphate Solutions
     on Normal and Sulphate-Resisting Portland Cement.  J. App.
     Chem., 14, Jan. 1964, 20-30.

47.  Jambor, J.  Possibilities for More Precise Evaluation of
     the Resistance of Concrete to an Aggressive Medium.  Dura-
     bility of Building Materials and Components, ASTM  STP-691,
     1980, 301-12.

48.  Lea, F. M.  The Chemistry of Cement and Concrete.  3rd
     Edition, Arnold Publishers, 1970.

49.  Friede, H.  Depth of the Corroded Zone in Concrete Exposed
     to Carbonic Acid.  Durability of Building Materials and
     Components, ASTM STP-691, 1980, 355-63.
                              27

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50.  Reading, T. J.  Combating Sulfate Attack in Corps of
     Engineers Concrete Construction.  Durability of Concrete,
     ACI SP-47, 1975, 343-66.

51.  Mehta, P. K. and M. Polivka.  Sulfate Resistance of Expan-
     sive Cement Concretes.  Durability of Concrete, ACI SP-47,
     1975, 367-79.

52.  Ludwig, V.  Durability of Cement Mortars and Concretes.
     Durability of Building Materials and Components, ASTM
     STP-691, 1980, 269-81.

53.  Klieger, P.  Durability Studies at the Portland Cement
     Association.  Durability of Building Materials and Compo-
     nents, ASTM STP-691, 1980, 282-300.

54   Mehta, P. K.  Performance Tests for Sulfate Resistance  and
     Alkali-Silica Reactivity of Hydraulic Cements.  Durability
     of Building Materials and Components, ASTM STP-691, 336-45.

55.  Haynie, F. H. and J. B. Upham.  Correlation Between Corro-
     sion Behavior of Steel and Atmospheric Pollution Data.
     Corrosion in Natural Environments, ASTM STP-558, 1974,
     33-51.

56.  Mikhailovskii, Y. N. and A. P. San'ko.  Statistical Esti-
     mation of the Influence of Fluctuations in the Atmospheric
     Sulfur Dioxide Concentration on the Rates of Corrosion  of
     Metals.  Protection of Metals, 15(4), 1979, 342-5.

57.  Ma'tsushima, I. and T. Ueno.  On the Protective Nature of
     Atmospheric Rust on Low-Alloy Steel.  Corrosion Science,
     11(3), 1979, 129-40.
                              28

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                           APPENDIX  A
               SUMMARIES  OF  SELECTED REFERENCES

Reference 4.  Fisher, T.   When  the  Rain Comes.   Prog. Arch.
              (7), 1983,  99-105.
     This paper presents  a general  discussion of the effects
of acid deposition on building  materials.   It is designed to
give architects a basic understanding of the mechanisms in-
volved in the acid-induced deterioration of buildings.  The
author thinks that once architects  understand the problem they
can greatly reduce the effects  of acid deposition through
proper detailing and material  selection.  He makes the follow-
ing comments on the deterioration of concrete and other build-
ing materials.
     The effects of acid  rain  on  buildings range from minor
surface discoloration to  possible destruction of structural
members.
     Much of the acid-related  damage to structures comes not
from acidic precipitation  but  from  sulfur  dioxide and nitrogen
oxide gases directly deposited  on and absorbed  by building
materials, i.e. "dry deposition."   These dry compounds react
with dew or other moisture on  a building to form strong acids
that attack the building  material on which they are  deposited.
     The effects of acid  deposition depend not  only  upon the
type of material but on its  grain size, porosity, location on
the building, and relationship  to other materials.  Portland
cement, which contains tricalcium aluminate, is susceptible to
attack by sulfates or sulfuric  acid.   Silicate  materials such
as concrete can produce a  soft, colorless  material called
kaolin as atmospheric acids  accelerate their hydration.
                               29

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     Fisher states: "Many scientists  think  that  acid  deposition
damages buildings more through  the physical  stresses  it  induces
than through the chemical reactions  it  brings  on."  The  acids
leave a residue of soluble sulfate and  nitrate salts,  which
accumulate on or just beneath the surface of  the  material  and
then crystallize with the absorption  of water, exerting  enor-
mous stresses within the material.  These salts  create an  addi-
tional problem in reinforced concrete,  i.e.  salt-induced corro-
sion of the reinforcing steel,  which  increases the  internal
stresses developed within the concrete.
     The paper goes on to discuss methods for  reducing the
effects of acid deposition on building  materials.

Reference 5.   Stanwood, L.  Acid Rain, A Cloudy  Issue.   The
               Construction Specifier,  Nov.  1983, 74-9.

     The paper presents a general discussion  of  the  threat
posed by acid rain to building  materials  such  as  stone,  con-
crete, metals, and paints and coatings.   It  indicates  that
materials such as stone and concrete, which  contain  calcium
carbonate and related compounds, are  particularly susceptible
to deterioration in an acid environment.
     Sulfur compounds in acid rain react  with  calcium  carbonate
to form calcium sulfate, or gypsum, which is  about  30  times
more soluble in water than calcium carbonate  and  can  be  rapidly
washed away.  Furthermore, the  gypsum forming  within  the base
material can weaken it and at the same  time  provide  a  course
for more damaging moisture to penetrate  the  structure.
     Stanwood refers to an interview  with Paul Klieger,  chair-
man of ACl's committee on durability.   Klieger thinks  that acid
rain "is an exceedingly minor problem"  with  concrete  and that
"all you would get is a slight  etching  of  the  surface,"  and
                               30

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his committee has not deemed  acid  rain  a  problem needing exten-
sive study.  Stanwood points  out,  however,  that this statement
applies to concrete, not  to  the  possible  corrosion of metals
used in reinforcing a concrete structure,  or to the effects of
acid-laden water on sewer pipes  and  other  related structures.

Reference 23.   Gauri, K. L.  Deterioration of Architectural
                Structures and Monuments.   Polluted Rain
                (Environmental Science  Research), 17, 1980,
                125-45.

     The major objective  of  this paper  is  to present the
effects of increased atmospheric toxicity  on common materials,
such as natural building  stones, brick, concrete, mortar,  and
terra-cotta, so that attempts will be made  to reduce it.
     Gauri states that:   "Natural  stone,  concrete, and mortar
are the common materials  exposed at  the facade of architectural
structures.  Carbonate and silicate  minerals are the essential
constituents of these materials.   These minerals are suscepti-
ble to attack by atmospheric  CC>2 .  The  weathering of these
minerals has increased at an  alarming rate  in the industrial
countries due to NOj and 302  emanations."
     "The S(>2 attack has  produced  sulfate  crusts on ancient
buildings.  The continuing reactivity behind these crusts  has
resulted in the removal of stone in  layers  obliterating the
original sculptural details  and  causing serious damage to  the
s true tures."
     "Most ancient buildings  and monuments  contain flores-
cences.  Evaporation of water at the  surface tends to accumulate
the florescences in subsurface regions  of  the stone; their
migration is facilitated by  increased ionic concentration
resulting from atmospheric pollution.   Repeated dissolution and
                               31

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crystallization of the florescences  in  subsurface  regions  and
the accelerated oxidation of reinforcing metals  generate
stresses which disintegrate the  stone."
     Gauri points out that deterioration mechanisms  involve
more than just the reaction of the material with atmospheric
gases, the mechnical effects of  weathering  due  to  crystalliza-
tion and hydration of florescences,  freezing  of  water,  and the
expansion of reinforcement due to corrosion are  equally
important.

Reference 24.  Dijkstra, 6.  Effects  of Air Pollution on
               Materials in the  Netherlands.  Report Prepared
               for Panel 3 ("Environmental  Impact")  of  the
               NATO/CCMS Pilot Study  on Air Pollution Control
               Strategies and Impact  Modelling,  1982.

     The paper presents a brief  summary of  the  effects  of  air
pollutants, mainly sulfur oxides, on  materials  such  as  metals,
paints, textiles and building stones.   With reference to con-
crete, Dijkstra states: "Cement  contains calcium aluminate
which converts in the presence of S02  into  ettringite,  which by
the large volume change causes cracks  in concrete."

Reference 25.  Skoulikidis, T. N.  Atmospheric  Corrosion of
               Concrete Reinforcements, Limestones,  and
               Marbles.  Atmospheric  Corrosion  of  Concrete
               Reinforcements and Their Protection,  date
               unknown, 807-25.

     The paper reports the atmospheric  attack on,  and the  pro-
tection of, concrete reinforcement,  and the sulfation by atmo-
spheric S<>2 of limestones and marbles  used  in the  construction
of ancient monuments and statues.
                              32

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     In discussing  the corrosion  of  concrete  reinforcement, the
author states: "The increase of atmospheric  pollution intensi-
fies the corrosion  tendency of  the reinforcements  in the atmo-
sphere.  The cracking of concrete was  observed  more  frequently
with an increase of the atmospheric  pollution (SC>2,  C02, NH3,
NOX, etc.) and the  acceleration of the  corrosion  by  the for-
mation of a more conductive environment,  that also  chemically
attacks the metals."

Reference 26.  Skoulikidis, T. N.  Effect of  Primary and
               Secondary Air Pollutants and  Acid  Depositions
               on (Ancient and Modern)  Buildings  and Monu-
               ments.  In:  Proceedings of Symposium on Acid
               Deposition, A Challenge  for Europe,  Preliminary
               Edition, Sept. 1983,  193-226.

     The author discusses  the effects  of  atmospheric pollutants
on the accelerated  corrosion of zinc,  copper,  aluminum, lead,
and steel as bare metals and as reinforcement in  concrete, and
also the direct and indirect effects of S02»  N0X,  C02»  H2S04,
and HNC>3 on the deterioration of  calcites (such as  limestones)
and marble.  Regarding concrete the  author states:  "Air pollu-
tants accelerate the cracking of  concrete and consequently the
corrosion of rebars. SC>2 and 803  transform Ca(OH)£  of concrete
to CaS04  a
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     Most of the material damage associated  with  SO2  or other
pollutants is caused by long-term exposure.   Furthermore,  most
of the actual damage from sulfur compounds  is  due  to  the forma-
tion of sulfur acids, and 502 represents  the  best  proxy for the
presence of those sulfur compounds.
     Sulfur dioxide and its acid derivatives  are  known to
cause considerable damage to materials, attributed mostly  to
highly reactive t^SO^ formed either  in  the  atmosphere or on the
surface of materials.  In the absence of  adequate  moisture, the
amount of material damage caused by  SOX would  be  practically
nil.
     Damage to limestone products, concrete  and marble, has
been observed in areas experiencing  relatively high levels of
S02 over a prolonged period.
                               34

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                          APPENDIX B

            INDIVIDUALS AND ORGANIZATIONS SURVEYED
Dr. George Lauer
Environmental and Energy
  Systems Div.
Rockwell International Corp.
2421 West Hillcrest Dr.
Newbury Park, CA  91320

Dr. Richard G. Stein
The Stein Partnership
20 West 20th Street
New York, NY  10011

Mr. James T. Dikeou
Chairman, Am. Concrete Inst.
(ACI) Committee 124-Research
Quazite Corp.
5515  Gasmer
Houston TX  77035

Mr. Paul Klieger
Chairman, ACI Committee 201-
  Durability
Portland Cement Association
5420 Old Orchard Rd.
Skokie, IL  60077

Mr. Charles M. Dabney
Chairman, ACI Committee 303-
  Architectural Concrete
L. M. Scofield Co.
6533 Bandini Blvd.
Los Angeles, CA  90040

Mr. Lawrence F. Kahn
Chairman, ACI Committee 364-
  Rehabilitation
Georgia Inst. of Technology
School of Civil Engineering
Atlanta, GA  30332
Mr. Mark B. Hogan
Chairman, ACI Committee 531-
  Concrete Masonry Structures
Natl. Concrete Masonry Assoc.
P.O. Box 781
Herndon, VA  22070

Mr. James E. McDonald
Chairman, ACI Committee 546-
  Repair of Concrete
Waterways Exper. Station
P.O. Box 631
Vicksburg, MS  39180

Dr. Charles Duncan Pomeroy
Cement and Concrete Assoc.
Wexham Springs
Slough SL3 6PL  349620
ENGLAND

Mr. G. W. DePuy
Bureau of Reclamation
P.O. Box 25007/Code 1512
Denver, CO  80225

Dr. Peter J. Sereda
Div. of Building Research
National Research Council
Ottawa, Ontario FC1A OR6
CANADA

Professor Povindar K. Mehta
Dept. of Civil Engineering
Univ. of California
Berkeley, CA  94720

Dr. V. M. Malhotra
CANMET/EMR
405 Rochester St.
Ottawa, Ontario  209660
CANADA  K1A OG1
                              35

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Dr. Geoffrey Frohnsdorff
Chief, Building Materials Div,
National Bureau of Standards
Building 226, Room B-368
Washington, DC  20234

Mr. Larry W. Masters
Building Materials Div.
National Bureau of Standards
Building 226, Room B-343
Washington, DC  20234

Dr. James R. Wright
RILEM President
National Bureau of Standards
Building 225, Room B-119
Washington, DC  20234t

Centre for Research and Devel-
  opment in Masonry
No. 105, 4528 6A Street, N.E.
Calgary, Alberta  T2E 4B2
CANADA

Mr. Sol Caller
MCP Facilities Corp.
P.O. Box 257
Glen Head, NY  11545
Mr. John M. Scanlon
Chief, Eng. Mechanics Div.
U.S. Army Corps of Engineers
Waterways Experiment Station
P.O. Box 631
Vicksburg, MS  39180

Dr. Gunnar Morten Idorn
G.M. Idorn Consult. Aps.
Tovesvej 14 B
2850 Naerum  299200
DENMARK

Dr. Delia M. Roy
Prof, of Materials Science
Pennsylvania State Univ.
Materials Research Laboratory
University Park, PA  16802

Mr. Howard Kanare
Portland Cement Association
5420 Old Orchard Rd.
Skokie, IL  60077

Dr. Vance Kennedy
U.S. Geological Survey
Water Resources Division
345 Middlefield Rd.
Menlo Park, CA  94025
                              36

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                          APPENDIX  C

                       LETTER OF  INQUIRY
                               April   ,  1984
Dear       :

     I am writing to you in hopes  that  you  may  be  able to
assist us in gathering information  for  a  research  program cur-
rently underway at Brookhaven National  Laboratory.

     We are presently involved  in  the preliminary  phase of a
research program funded by the  Environmental  Protection Agency
to investigate the effects of acid  deposition on  portland
cement concrete (PCC) structures.   As part  of this  program we
are conducting a survey to determine; (a)  if  any  information
exists regarding problems associated with  acid  deposition on
PCC, and what the economic impact  of  these  problems may be,
(b) if any research work has been,  or is  currently  being done
to investigate the problems associated  with acid  deposition,
and (c) if there is a need for  experimental work  to be done in
this area.

     While I realize that these  questions  are very  broad and
complex, any information that you  may be  able to  provide to us
will be greatly appreciated.

                                Sincerely,
                               Ronald  P.  Webster
                               Materials  Research  Engineer
RPW:jgm

cc:  L. E. Kukacka
                              37

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                                   TECHNICAL REPORT DATA
                            (Please read Instructions on the reverse before completing]
1. REPORT NO.
                             2.
                                                           3. RECIPIENT'S ACCESSION NO.
4. TITLE AND SUBTITLE
 EFFECTS OF ACID DEPOSITION  ON THE PROPERTIES OF
 PORTLAND CEMENT CONCRETE  STATE-OF-KNOWLEDGE
                                                           S. REPORT DATE
             6. PERFORMING ORGANIZATION CODE
7. AUTHOR(S)
 R.P.  Webster and L.E. Kukacka
             8. PERFORMING ORGANIZATION REPORT NO.
9. PERFORMING ORGANIZATION NAME AND ADDRESS
 Brookhaven National Laboratory
 Upton, NY  11973
             10. PROGRAM ELEMENT NO.
               CCYN1A-08/4063    (FY-85)
             11. CONTRACT/GRANT NO.


               DW 899307010-01-02
12. SPONSORING AGENCY NAME AND ADDRESS
  Atmospheric Sciences  Research Laboratory -  RTP,  NC
  Office of Research and  Development
  U.S. Environmental Protection Agency
  Research Triangle Park, N.C.  27711	
                                                            13. TYPE OF REPORT AND PERIOD COVERED
             14. SPONSORING AGENCY CODE


               EPA/600/09
19. SUPPLEMENTARY NOTES
16. ABSTRACT
       Presented are  the results of a program conducted to determine the state-
  of-the-art knowledge  pertaining to the effects of acid deposition on the pro-
  perties of portland cement concrete structures.  Information  was collected from
  a computerized literature survey, interviews, and replies  to  mail and telephone
  inquiries addressed to cement and concrete researchers and to governmental
  agencies and private  firms active in the  maintenance and restoration of concrete
  structures.  In  general, the study revealed very little qualitative or quanti-
  tative information  on the effects of acid deposition on PCC structures.  The
  rate of. deterioration of reinforced PCC  structures in polluted areas, however,
  appears to be increasing, and available  information makes  it readily apparent
  that acids and acid waters significantly affect the durability of concrete,
  and that SOa, NOX,  and HC1 accelerate  the corrosion of reinforcing steel.
17.
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EPA Form 2220-1 (R«v. 4-77)   PREVIOUS EDITION is OBSOLETE

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