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OCR for page 251
lv
An Evaluation of
Activated Carbon for
Drinking Water
Treatment
This chapter contains the findings of the Subcommittee on Adsorption of
the National Research Council's Safe Drinking Water Committee, which
studied the efficacy of granular activated carbon (GAC) and related
absorbents in the treatment of drinking water. Some attention is given to
an examination of the potential health effects related to the use of these
absorbents, but detailed toxicological and epidemiological implications
resulting from the presence of organic compounds in drinking water are
considered in separate chapters of Drinking Water and Health, Volume 3.
The development of standards for GAC and the economic aspects of its
use was not a part of this study.
The subcommittee defined "activated carbon" as a family of carbona-
ceous substances that are characterized primarily by their surface area,
pore size distribution, and sorptive and catalytic properties. Different
raw materials and manufacturing processes produce final products with
different adsorption characteristics.
The use of GAC under specified conditions was proposed by the U.S.
Environmental Protection Agency (EPA) as the option of choice for the
control of "synthetic organic chemicals" in drinking water. During the
subcommittee's study, the EPA held hearings and received written
comments regarding this treatment.
The subcommittee reviewed the pertinent literature and rigorously
assessed the scientific data base. Its scope of work included a review of
work on:
251
OCR for page 252
252 DRINKING WATER AND H"LTH
adsorption efficiency
· microbial activity on absorbents
· physiochemical interactions
· regeneration ofadsorbents
· analytical methods to monitor adsorption processes
The subcommittee considered the ability of absorbents to remove
organic compounds of concern to health and the possible products of the
adsorption process. A large and diverse segment of the scientific
literature, particularly that concerning recent European experience, was
scrutinized. Studies that met established criteria for quality assurance
and completeness of data were used as primary sources by the
subcommittee. Where possible, stress was placed on studies of chemicals
at nanogram to microgram per liter concentrations, which are typically
found in drinking water. The subcommittee was confronted by a
continual flow of new data and the need for postulation and interpreta-
tion. To ensure a thorough review of each topic, the data for each type of
adsorbent were considered and reported separately.
Carbon and other absorbents in various forms have been used for the
treatment of water and as detoxifying pharmaceutical agents in medicine
for many centuries. There has been an uninterrupted use of carbona-
ceous absorbents since biblical times (Old Testament, Num. 19:9;
Maimonides, 1 185) and there have been marked changes in the nature of
the adsorbent since that time (Kunin, 1974a,b).
During the twentieth century, GAC and powdered activated carbon
(PAC) have been used in the United States to control taste and odors in
drinking water (U.S. Environmental Protection Agency, 1978a). During
the past 20 yr, research on the use of absorbents to treat drinking water
has emphasized the removal of specific organics. The removal of organic
compounds from drinking water has been based primarily on the
measurement of organic matter as measured by carbon chloroform
extract (CCE), total organic carbon (TOC), or other group parameters.
However, it has long been recognized that these group parameters
provide only estimates of performance for target compounds. Studies
beginning with those of Middleton and Rosen (1956) began to identify
the specific organic compounds in drinking water and their removal by
the carbon adsorption.
Over 700 volatile organic compounds have been identified in drinking
water (U.S. Environnmental Protection Agency, 1978c). These com-
pounds make up only a small fraction of the total organic matter
(National Academy of Sciences, 1977~. Approximately 90% of the
volatile organic compounds that can be analyzed by gas chromatography
OCR for page 253
An Evaluation of Activated Carbon 253
have been analyzed, but this represents no more than logo by weight of
the total organic material. Only 5~o logo of the nonvolatile organic
compounds that comprise the remaining 90% of the total organic matter
have been identified.
The EPA (1978c) has categorized the organic compounds in drinking
water into five different classes. Each class has distinctly different
characteristics of concern to those involved in water treatment.
Class I: organic compounds that cause taste and odor and/or color
problems;
Class II: synthetic organic chemicals that are present in source waters
from upstream discharges or runoff;
Class III: organic compounds (precursors) that react with disinfec-
tants to produce "disinfection by-products";
Class IV: organic chemicals that are the disinfection by-products
themselves; and
Class V: natural (non-Class III) organic compounds of little direct
toxicological importance.
Today there are GAC beds in U.S. water treatment plants for removal
of Class I compounds. Consideration is being given to the use of GAC
for removal of Class II, III, and IV compounds as data become
available. Class V compounds are of interest because they may compete
for adsorption sites, thereby lessening the removal of other compounds.
This report identifies the compounds that may be removed and/or
added to drinking water by the adsorption process with its attendant
chemical and microbial processes. It focuses on recently published lists
of organic chemicals of concern to health (Interagency Regulatory
Liaison Group, 1978; National Academy of Sciences, 1977, 1979;
National Cancer Institute, 1978~.
Each section deals with complex subjects in which there are uncertain-
ties, inconclusive or incomplete data, and, thus, conflicting opinions. The
length of each section represents only the number of studies reviewed
and does not reflect the relative importance of the subjects.
ACTIVATED CARBON—A l:)EFINITION
"Activated carbon" comprises a family of substances, whose members
are characterized primarily by their sorptive and catalytic properties.
Different raw materials and manufacturing processes produce final
products with different characteristics.
OCR for page 254
254 DRINKING WATER AND H"LTH
Activated carbon can be made from a variety of carbonaceous
materials and processed to enhance its adsorptive properties. Some
common materials that are used to make activated carbon are bitumi-
nous coal, bones, coconut shells, lignite, peat, pecan shells, petroleum-
based residues, pulp mill black ash, sugar, wastewater treatment sludge,
and wood ~Veber, 1972~. As is true with any production process, the
quality of the final product is influenced by the starting material. In the
past, activated carbons that were used for industrial applications were
commonly produced from wood, peat, and other vegetable derivatives.
Today, lignite, natural coal, and coke are the most frequently used
sources of activated carbon due to their availability and attractive price.
The basic structural unit of activated carbon is closely approximated
by the structure of pure graphite with only slight differences. The
structure of activated carbon is quite disorganized compared with that of
graphite because of the random oxidation of graphite layers. The regular
array of carbon bonds in the surface of the crystallites is disrupted
during the activation process, yielding free valences that are very
reactive. The structure that develops is a function of the carbonization
and activation temperatures. During the carbonization process, several
aromatic nuclei with a structure similar to that of graphite are formed.
From X-ray spectrographs, these structures have been interpreted as
microcrystallites consisting of fused hexagonal rings of carbon atoms.
The diameter of the planes making up the microcrystalline is estimated to
be 150 A, and the distance between microcrystallites ranges from 20 ~ to
so A (Wolff, 1959~.
The presence of impurities and the method of preparation influences
the formation of interior vacancies in the microcrystalline. The ringed
structures at the edges of the planes are often heterocyclic, resulting from
the nature of either the starting material or the preparation process.
Heterocyclic groups would tend to affect both the distance of adjacent
planes and the sorptive properties of the carbon.
As a rule, the structure of the usual types of active carbon is
tridisperse, i.e., they contain micropores (effective radii of 18-20 A),
transitional pores (4~200 A), and macropores (50C~20,000 A). Accord-
ing to Dubinin (1966) only a few of the micropores lead directly to the
outer surface of the carbon particle. Most of the pore structures of the
particles are arranged in the following pattern: the macropores open
directly to the external surface of the particle; transitional pores branch
off from macropores; and micropores, in turn, branch on from the
transitional pores. The specific area of the micropores usually amounts
to at least 90% of the total surface area.
OCR for page 255
An Evaluation of Activated Carbon 255
THE WATER TREATMENT PROCESS
GAC is typically used in a water treatment plant after the coagulation
and sedimentation processes and, commonly, following preliminary
disinfection steps during which chemical reactions can occur. Moreover,
water is often disinfected before it passes through the GAC adsorbers in
order to prevent nuisance biological growths. In many instances, the
activated carbon functions as a granular filter medium for removing
particulates, although in a few cases in the United States and in most
instances in Europe the GAC absorbers are preceded by filters for
particulate removal.
Water is usually passed downward through packed beds of GAC. The
frequency of backwashing is dependent on the amount of particulates
being removed and the extent of microbial growth. Some intermixing of
the GAC granules takes place during this step, although this tendency is
countered by particle size stratification during backwash. While packed-
bed downflow absorbers in parallel are most commonly used, many
other flow patterns, such as operation in series, upflow packed bed, and
upflow expanded bed, may be used.
Regeneration of GAC is not generally practiced at water plants in the
United States as it is in Europe. If the objective of GAC use is to include
the removal of organic compounds in addition to those that cause taste
and odor, regeneration is likely to become more common in the United
States. The type of contactor selected for the GAC will be influenced by
the frequency of regeneration.
After treatment of a water supply with GAC, postdisinfection is
generally used to reduce the total number of bacteria, some of which
may be present because of the microbial growths in absorbers. Sufficient
disinfectant is usually applied to ensure a residual in the distribution
system to prevent contamination of the water.-Postdisinfection is used in
addition to predisinfection because aqueous oxidants that are used in
preliminary disinfection steps will generally be eliminated by reaction
with the GAC.
In certain instances, some synthetic resins may serge as replacements
for GAC or they may be used in conjunction with GAC to provide the
desired quality of water. The major difference between resins and GAC
is that the resins are regenerated by application of aqueous solutions of
acids, bases, and/or salts, or of nonaqueous solvents or steam, while
GAC is usually thermally regenerated. In general, resins usually require
a pretreatment step that is dependent upon the nature of the resins.
Powdered activated carbon (PAC) is now more commonly used in the
OCR for page 256
256 DRINKING WATER AND H"LTH
United States than is GAC. It generally added to control taste and odor
at points in the water treatment plant, ranging from the water supply
intake to just before the rapid sand filter. PAC is removed either in the
sedimentation basin or by the rapid sand filter. No attempt is made to
regenerate it during the water treatment. Whether PAC can be used to
remove organics other than those that cause offensive taste and odor
requires closer examination.
Various types of GAC and PAC are commercially available as a result
of variations in the raw materials and manufacturing processes. Because
the types of organic contaminants vary widely from location to location,
the best carbon for one application may not be the best in another.
Consequently, comparative testing for a particular water source is
mandatory.
The chemical compounds entering an adsorption water treatment
process consist of high-molecular-weight humic materials, lower-molecu-
lar-weight organic compounds of natural or industrial origin, and the
products of previous treatment such as chlorination or ozonization. A
portion of the chemicals can be removed by the clarification process
and/or sorbed by the adsorbent or any microbial floe within the
adsorbent bed. Some compounds may be nonabsorbable or only very
weakly adsorbable.
The chemical compounds leaving the adsorption treatment process
can be the same chemicals that entered the plant, or they may be
products of chemical reaction or microbial action within the system.
Organic compounds may appear in the effluent of an adsorption column
because available adsorption sites are saturated or because they are
displaced from the adsorption sites by other organics. Because adso~p-
tion is often reversible, adsorbed compounds may desorb and appear in
the effluent when the influent concentrations of those compounds
decrease. These phenomena may lead to the appearance of a larger
concentration of a compound in the effluent than is in the influent. Thus,
both the qualitative and quantitative variability of the mixture of
organics entering an adsorption process affect the quality of water that
can be produced by it.
GENERAL CONCLUSIONS AND RECOMMENDATIONS
Raw water sources and disinfected water supplies may contain organic
compounds that have been demonstrated to be carcinogenic or otherwise
OCR for page 257
An Evaluation of Activated Carbon 257
toxic in experimental animals or in epidemiological studies. Also present
are a large number of compounds that either have not been identified or
their effects on health have not been characterized. Properly operated
GAC systems can remove or effectively reduce the concentration of
many of the compounds described above. Less is known about synthetic
resins than about GAC, but it is known that they can be applied to
remove certain types of organic contaminants.
The information available as of this date on the treatment of water
with GAC provides no evidence that harmful health effects are produced
by the process under proper operating conditions. However, there are
incomplete studies on the possible production of such effects with virgin
or regenerated carbon through
· reactions that may be catalyzed by the GAC surface;
· reactions of disinfectants with GAC or compounds adsorbed on it;
· reactions mediated by microorganisms that are part of the process;
or
· by the growth of undesirable microorganisms on GAC.
Studies are also needed on the properties of regenerated activated
carbons and on the adsorption of additional contaminants with potential
health ejects. The frequency of GAC regeneration is determined by the
organic compounds in the water and their competitive interactions. The
types and concentrations of organic compounds may vary widely among
different locations and seasons of the year. Competitive interactions are
complex and presently cannot be predicted without data from laboratory
and/or pilot scale tests on the water to be treated.
While there is ample evidence for the effectiveness of GAC in
removing many organics of health concern, more data are needed in the
quantification of any harmful health effects related to the use of GAC.
This need, however, should not prevent the present use of GAC at
locations where analysis of the water supply clearly indicates the
existence of a potential health hazard greater than that which would
result from the use of GAC.
Clarification processes (coagulation, sedimentation, filtration) remove
significant amounts of some organics, especially some types of THM
precursors and relatively insoluble compounds that may be associated
with particulates. In some cases, the removal of THM precursors by
clarification may be sufficient to eliminate the need for an adsorption
process.
OCR for page 258
258 DRINKING WATER AND H"LTH
ADSORPTION EFFICIENCY OF GAC
The trace organic compounds that can be removed by GAC are usually
present at ,ug/liter quantities or less. The subcommittee considered the
GAC adsorption efficiency for individual compounds and the competi-
tive adsorption of mixtures. Since GAC is used in conjunction with other
water treatment processes, the effect of pretreatments for removing trace
organic compounds and their precursors were examined in depth. Hence,
the following questions were addressed:
1. How efficiently does GAC adsorb individual trace organic com-
pounds, particularly those of concern to health?
2. When processes such as coagulation, sedimentation, filtration,
aeration, disinfection, oxidation, and PAC adsorption precede GAC
adsorption, how is the efficiency of the GAC affected?
3. Can water that has been treated by GAC be disinfected more or
less easily than water that has not been treated by GAC?
4. What is the potential for electively using PAC to remove organics?
5. What reactions take place between oxidants that are applied as
predisinfectants and the activated carbon or the compounds that are
adsorbed on the activated carbon? Do these reactions result in
potentially hazardous compounds that would not be present if activated
carbon were not used?
6. To what extent does competitive adsorption between trace organics
with potential health ejects and the large concentrations of background
organics, generally characterized as humic substances, influence the
electiveness of GAC?
7. To what extent does competitive adsorption among similar concen-
trations of trace organics with potential health effects influence the
electiveness of GAC?
8. How significant is the effect of competitive adsorption when it is
compared to the eject of the reequilibration that is produced by the
variable nature of the composition and concentration of trace organics in
the feedwater to the GAC bed?
Removal of Selected Organic Compounds
Adsorption isotherms and small column studies that are performed in
the laboratory using GAC are useful tools that have been developed to
OCR for page 259
An Evaluation of Activated Carbon 259
describe how specific organic chemicals can be removed in large-scale
GAC applications. A considerable amount of adsorption research
describing the affinities of pure compounds for the activated carbon
surface has been reported in the literature during the last 15 years.
Improved analytical tools have made it possible both to detect the
organics at trace levels in the environment and to follow their removals
in adsorption studies in the laboratory. This section of the chapter
evaluates the efficiency of GAC adsorption of individual trace organic
compounds, particularly those with potential health ejects.
Removals of organic chemicals are discussed in the literature on the
basis of laboratory and pilot-scale studies and large-scale applications.
Laboratory studies are by far the most useful for describing specific
organic removals since environmental factors can be more carefully
controlled in them than in field evaluations. The problem of competitive
adsorption is significant when environmental samples are used in
experiments in which specific organic compounds are removed by
adsorption. A later section of this chapter addresses this problem
exclusively.
Adsorption data obtained in the laboratory are normally reported as
percent removed, adsorption isotherms, kinetics of adsorption, and the
results of small-scale column studies. In the following sections, these
data are reviewed and the utility of each method is evaluated.
Percent Removals
Giusti et al. (1974) made extensive use of percent reduction as a measure
of the effectiveness of activated carbon for removing organic chemicals.
They added 93 petrochemicals individually at one level to one type of
activated carbon and used the subsequent calculated percent reductions
to test several hypotheses concerning the removal of different classes of
organics by activated carbon.
There are several problems associated with using percent removal data
exclusively to describe how well a particular organic compound is
removed from water. The single value study results in a single point on
an isotherm. Unfortunately, this single point gives no indication of how
capacity varies with concentration, i.e., by the isotherm slope and shape.
To be truly representative, the amounts of adsorbed compound per gram
of carbon for individual organic compounds must be compared on an
equal equilibrium concentration basis, which is not possible if only a
single percent removal value is available.
OCR for page 260
260 DRINKING WATER AND H"LTH
Adsorption Isotherms
Adsorption isotherms are plots of the equilibrium relationship between
the amount of organic compound that is left in solution (equilibrium
concentration, Ce) and the amount of compound that is on the surface of
the activated carbon (surface concentration, qJ.
Few studies describe the adsorption isotherms of a wide variety of
organic compounds over several orders of magnitude. An EPA publica-
tion (U.S. Environmental Protection Agency, 1978c) tabulated refer-
ences on the removals of some 50 organic compounds by GAC. While
there are some useful data among the references cited in this work, a
large fraction of the reported data is fragmentary. Generally, informa-
tion is omitted, such as the number of data points used to define the
isotherm or the equilibrium concentration range over which the slope
and intercept of the linear isotherm are valid. Dobbs et al. (1978) have
made significant efforts to standardize the reporting of isotherm data.
Table IV- 1 lists a series of compounds for which detailed isotherms are
available. No attempt has been made to list all studies that have been
published. Instead, Table IV-1 presents a sample of available studies.
The compounds in the table represent a wide variety of organic
chemicals, including naturally occurring chemicals, industrial solvents,
and compounds that have been identified in surface waters and waste
streams in the United States. Dobbs et al. (1978) and Fochtman and
Dobbs (1980) have made some of the few efforts to, determine adsorption
capacities for many organic chemicals of toxicological concern. In the
future, the isotherm data base should be expanded much more rapidly to
include the compounds that are just now being identified as toxic or
potentially carcinogenic. There are significant difficulties in determining
isotherms for some of these organic compounds. A major difficulty is
that many compounds must be analyzed at concentrations that have
previously been near the limit of detectability.
Isotherm data for the organic compounds that are listed in Table IV-1
have become available only recently, and few attempts have been made
to analyze the data to determine whether general patterns exist. Figure
IV-1 plots selected isotherms for compounds from Table IV-1 over seven
orders of magnitude of equilibrium concentration (McGuire and Buffet,
1980~.
Although the isotherms in Figure IV-1 were determined by different
investigators using different techniques and different carbons, there is
surprising agreement between isotherms for the same compound.
Clearly, other aspects of the experimental conditions that affect the
positions of the isotherms include pH, ionic strength, and temperature.
OCR for page 261
An Evaluation of Activated Carbon 261
TABLEIV-} Some Orgaruc Compounds for Which Detailed, Wide-
Range Isotherms Have Been Determ~ned
acetonef
acetophenonea
acridine orangea
acridine yellowa
adeninea
adipic acida
anetholea
manisidinea
benzenea h
benzidineh
benzidine dihydrochloridea
benzoic acida
benzothiazolea
bromochloromethane'
bromodichloromethanea g
bromoforma,8
~bromophenol~
S-bromouracila
n-butanolb
(all) -n -butylphthalatea
carbon tetrachloridea g
chlorobenzenea
bis (2-chloroethyl) ethera
chlorodibromethanea
chloroforma g
1 -chloro-2-nitrobenzenea
p-chlorophenolC~f
5-chlorouracila
p-cresolf
cyclo he xan one a
cytosinea
3,3'-dichlorobenzidine h
dichloromethaneg
2,4-dichlorophenolC'
dimethylphenylcarbinol a
2,4-dinitrophenola C
dimethyl phthalatea
1,1'-diphenyl hydrazineh
1,4-dioxaneb
diphenylaminea
EDTAa
ethylbenzenea
ethylene chloridea
S-nuorouracila
geosmin'
guaninea
hexachlorobutadienea
hydroquinonea C
p-methoxyphenolC
4,4'-methylene-bis
(2 chloroaniline) h
methyl ethyl ketone b
2-methylisoborneole
naphthaleneh
c'-naphthola
,l3-naphthola
c'-naphthylaminea
,(~-naphthylamineh
p-nitroanilinea
nitrobenzenea
nitromethaneb
p-nitrophenOlb~c,4,i
N-nitrosodiphenylaminea
p-nonylphenola
parathionj
pentachlorophenola
phenOIa,c,i
phenyl mercuric acetatea
2-propanolf
propionitrilef
sodium benzene sulfonate~
styrenea
tetrachloroethylene g
1,2,3,4-tetrahydronapththalenea
thyminea
trichloroethyleneg
2,4,6 -trichlorophenol c
uracila
ureab
p-xylenea
aDobbsetal.,1978.
b McGuire, 1977.
c Zogorski, 1975.
Jain and Snoeyink, 1973.
' Snoeyink et al., 1977.
f Radke and Prausnitz, 1972a.
g Weber e' al., 1977.
h Fochtman and Dobbs, 1979.
Snoeyink et al., 1969.
Weber and Gould, 1966.
OCR for page 370
370 DRINKING WATER AND H"LTH
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An Evaluation of Activated Carbon 371
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Representative terms from entire chapter:
drinking water
