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OCR for page 135
lv
Solid Particles
in Suspension
INTRODUCTION
In addition to dissolved substances, drinking water typically contains
small amounts of very finely divided solid particles of several kinds.
These particles, ranging in size from colloidal dimensions to about 100
,um, are composed of inorganic and organic materials that are derived
from soils and rocks and from the debris of human activity with which
the raw water has come in contact. They include clays, acicular or fibrous
particles of asbestos minerals, and organic particles resulting from the
decomposition of plant and animal debris in the soil.
Little is known about the effects that these suspended solids may have
on the health of those who drink water that contains them. However,
there is widespread concern over the biological effects of the asbestos
mineral fibers that occur in water, since similar fibers are known to be
carcinogenic when air heavily laden with them is inhaled for many years.
In view of this concern that such fibers as occur in water may be injurious
to health, their occurrence, characterization, analysis, and biological
ejects are reviewed in some detail.
No evidence has yet been discovered that either of the other classes of
common particulate contaminants of drinking water-clays and organic
colloids has any direct effect on health. Nevertheless, it is possible that
both may indirectly affect the quality of drinking water because they can
adsorb a variety of toxic substances, bacteria, and viruses from solution
or suspension and bind them more or less strongly. By such means these
135
OCR for page 136
136 DRINKING WATER AND HEALTH
materials may serve to concentrate and transport some water pollutants
and protect them from removal by water treatment.
For this reason, the properties of clays and organic particulates are also
discussed, together with the tendency of chemicals, bacteria, and viruses
to become concentrated at the surfaces of such particles.
Removal of suspended particles from water is briefly reviewed,
together with the significance of measurements of turbidity as an index of
water quality.
CLAY PARTICLES AND THEIR INTERACTIONS
Clay is usually defined on a particle-size basis, the upper limit being 2,um
diameter. Soils and sediments in nature will therefore have vaporing
proportions of clay material containing clay-mineral components (usual-
ly the phyllosilicates), as well as nonclay-mineral material that may
include a variety of substances such as iron and aluminum oxides and
hydroxides, quartz, amorphous silica, carbonates, and feldspar. The clay
minerals themselves are classified in Table IV- 1 (Grim, 1968~.
Clays are ubiquitous in soils and sediments derived from soils. They
may be formed in soils during soil development through the weathering
of various minerals, or they can be inherited essentially without change
from the parent material upon which the soils are formed. Parent
material, climate, topography, and vegetation determine the kinds of
clays that are found. Hydrothermal activity may also lead to clay
formation. As erosion acts on the landscape, clays may be suspended in
water and carried until they are deposited by sedimentation. Most
sedimentary rocks contain more or less clay as, for example, shales
(almost exclusively clay), limestones, and sandstones.
A number of scientific techniques are useful for studying clays, but the
most useful for identification and indication of relative abundance is X-
ray diffraction. The diffraction properties of the various clay minerals, as
well as the methods of treatment and sample preparation, can be found in
publications of Grim (1968), Brown (1961), and Whittig (1965~. Infrared
spectroscopy is a valuable adjunct to X-ray diffraction in characterizing
clays, and this subject has recently been reviewed by Farmer (1975~.
Infrared spectroscopy is the most powerful method for study of organic-
clay interactions (Mortland, 1970; Theng, 1975~. Other techniques useful
in characterizing clays are electron microscopy (Gard, 1971), thermal
methods (Mackenzie, 1957), and chemical analysis (Weaver and Pollard,
1973~.
The layer-lattice clay minerals, in themselves, do not appear to have
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Solid Particles in Suspension 137
TABLE IV-1 Classification of the Clay Minerals (Grim, 1968)
I. Amorphous
Allophane group
II. Crystalline
A. Two-layer type (sheet structures composed of units of one layer of silica tetra-
hedrons and one layer of alumina octahedrons)
1. Equidimensional
Kaolinite group
Kaolinite, nacr~te
2. Elongate
Halloysite group
B. Three-layer types (sheet structures composed of two layers of silica tetrahedrons
and one central dioctahedral or tr~octahedral layer)
1. Expanding lattice
a. Equidimensional
Montmor~llonite group (smectite)
Vermiculite
Montmor~llonite, sauconite
b. Elongate
Montmor~llonite group
Nontronite, saponite, hector~te
2. Nonexpanding lattice
Illite group
Regular mixed-layer types (ordered stacking of alternate layers of different types)
Chlorite group
D. Chain-structure types (hornblende-like chains of silica tetrahedrons linked to-
"ether by octahedral groups of oxygens and hydroxyls containing Al and Mg
atoms)
Attapulgite
Sepiolite
Pal ygors kite
deleterious effects when ingested by humans. Some of them are, in fact,
constituents of pharmaceuticals such as kaopectate (kaolinite). Other
indications (some from folklore) suggest beneficial results from ingestion
of clays. The effect of ingestion of fibrous clay minerals of the chain-
structure types (e.g., attapulgite, palygorskite, sepiolite, sometimes called
"asbestos"), is still open to question and is the subject of extensive study
at the present time. If layer-lattice clay minerals have deleterious e~ects
on human health, they are probably indirect, through adsorption,
transport, and release of inorganic and organic toxicants, bacteria, and
viruses.
Several reports have shown that concentrations of many pollutants are
much higher in sediments of streams and lakes than in the waters with
which they are associated. Clays and organic particulates are the
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138 DRINKING WATER AND HEALTH
materials chiefly responsible for such concentrations. Since clays are
ubiquitous in many waters used as sources for human consumption, it is
to be expected they will appear as particulate matter in some drinking
waters and thus it is of interest to consider the kinds of interactions they
have with dissolved materials. Considerable knowledge exists regarding
the surface chemistry and adsorptive properties of clays, and thus, with
information on the nature of a solute, it is possible to have some idea of
their interaction. Clays are very adsorptive substances. The possibility
exists that clays could act as vehicles for transport of toxic compounds
through adsorption in one environment, followed by release of the toxic
material when the clay entered a different environment.
It has been well established that some pesticides applied to watersheds
can be adsorbed by soil components and subsequently removed into
water by erosional processes (Bailey et al., 1974; Nicholson, 1969;
Nicholson and Hill, 19701.
Inorganic Pollutants
This classification of pollutants would include metal cations and some
anions. Among the metal cations that have been found to be polluting
some water and soils are Pb, Cr. Cu. Zn, Co, Mn, Ni, Hg, and Cd, while
radioactive isotopes of Pu, Cs, and Sr, among others, over potential
threats as pollutants. On the other hand, anionic species such as
phosphates, arsenate, borate, and nitrates are considered pollutants in
some situations.
The interactions of metal cations with clays include adsorption by ion
exchange, precipitation as hydroxides or hydrous oxides on clay surfaces,
and adsorption as complex species. ObviouslY. OH and Eh are critical
1 J ' AL
factors In determining the nature of the interactions between clays and
some transition and heavy metal ions. Hodgson's review (1963) includes
some reference to earlier work on clay interactions with some of the
transition ions and heavy metals. Jenne (1968) has electively described
the various factors controlling the concentrations of transition cations in
waters and soils, while Jenne and Wahlberg (1968) and Tamura (1962),
among others, have considered the interaction of radionuclides with
clays. Holdridge (1966) has reported adsorption studies of heavy metal
cations on ball clay. With regard to phosphate, it is likely that its
interactions with calcium ion and amorphous hydroxides of Fe3+ and
A13+ and with allophane are more important than adsorption by clay
minerals in affecting its concentration in natural waters.
In addition to adsorption by simple ion exchange, much work indicates
the retention of transition and heavy metals at clay mineral surfaces via
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Solid Particles in Suspension 139
precipitation of insoluble compounds, notably hydroxy and oxidehy-
droxy polymers. The incorporation of A13+, Mg2+, and Fe3+ hydroxy
polymers within the interlamellar space of swelling clays to form chlorite-
like species is a well-known pedogenic process. It has also been shown
that these brucite-gibbsite-like materials may often be withdrawn if the
mineral is subjected to a different environment, usually one involving a
change in pH. Gupta and Malik (1969) have reported the incorporation
of Ni2+ in smectite to form a nickel-chlorite, while Blatter (1973) found
similar reactions of smectite with Hg2+ . Thus it seems that many of these
kinds of metal cations have the ability to form interlayer complexes in
swelling clays. It would seem likely that in natural systems where the
polluting species might be present in very low concentrations compared
with other interlayer-forming species such as A13+, they might be
incorporated within the gibbsite-like layer as it forms, in essentially
isomorphous substitution for A13+, although reports of this phenomenon
were not found. It would also appear that incorporation of a polluting
metal cation within the intergrade clay is no guarantee that it might not
again be released to the natural system when the clay, through erosion
and deposition, is placed in a different environment where the interlayer
material may be removed. This phenomenon has been shown for
vermiculite-chlorite intergrades that, upon erosion from an acidic soil, are
deposited in a calcareous freshwater lake or floodplain to form discrete
vermiculite, within relatively short periods of time (Frink, 1969; Lietzke
and Mortland, 1973~.
The clay mineral vermiculite has a special affinity for K+ ion,
the ion is initially adsorbed in the interlamellar regions of the mineral and
then trapped by collapse of the layer structure. The ion is thus removed
from direct interaction with the surrounding solution. This process is
called potassium fixation, but will occur with other ions of similar
diameter to more or less extent. Cations that might be considered
pollutants that undergo this reaction with vermiculite are Ba2+ and
radioactive Cs+ .
in which
The hydroxides and hydrous oxides of iron, manganese, and aluminum
are often components of the clay fraction of sediments and have
important e~ects on pollutant concentrations in natural waters. They
often exist as coatings on the surfaces of other minerals and thus may
exert chemical activity far out of proportion to their total concentrations.
Jenne (1968) suggests that they furnish the principal control on the
concentrations of heavy metals such as Co, Ni, Cu. and Zn through
adsorption processes. The principal factors a~ecting adsorption and
desorption of heavy metals from these kinds of particulates are pH, Eh,
concentration of the metal in question, concentration of competing
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140 DRINKING WATER AND HEALTH
metals, and the eRects of other adsorbents such as organic matter and
clay minerals.
Organic Pollutants
These materials encompass a wide range of compounds, including
pesticides, polychlorinated biphenyls, aromatic species of various kinds
arising from industrial activity, and fluorine compounds in aerosols.
Whether or not organic species adsorb or interact with clays depends
upon the structure and properties of the compound and the nature of the
clay and its exchangeable cations. Several mechanisms of interaction are
possible and have been described in a number of recent reviews
(Mortland, 1970; Bailey and White, 1970; Theng, 1974; and Rausell-
Colom and Serratosa, 1975~. Organic cations adsorb on clays by ordinary
ion exchange and are usually preferred over the inorganic ions by the
exchange complex because of their large size and high molecular weights.
Examples of organic compounds that are cationic and could be
considered pollutants if transported outside their areas of application are
the herbicides Paraquat and Diquat. These compounds are strong bases
and are completely ionized in water. Other organic compounds, while
neutral at the ambient pH of the solution phase, may become protonated
after adsorption at the clay surface. The surface acidity of clays has been
shown to be a considerably stronger proton donor system than pH
measurements of the water-clay system would indicate. Thus, organic
compounds containing basic nitrogen or carbony} groups may become
protonated, and therefore cationic, after adsorption at clay surfaces.
Another kind of organic-clay interaction is the coordination or ion-
dipole type. Compounds with nitrogen, oxygen, sulfur, or olefinic groups
have electron pairs that may be donated to electrophilic exchange cations
to form complexes on the clay surface. In natural systems, an important
consideration is the competitive eject of water for these adsorption sites.
That is, the energy of ligand formation of an organic molecule with an
exchange cation must be greater than the salvation energy of the cation in
order to displace water molecules and obtain direct organic-cation
coordination. In the laboratory these interactions are easily obtained by
dehydration; however, in natural systems the competition of water is a
major factor in determining whether or not these complexations occur.
Nevertheless, it is likely that this kind of interaction does occur with some
highly polar, electron-donating organic compounds. Another important
factor is the nature of the exchange cation. Thus, for example, transition
metal cations on the exchange complex, that have unfilled a'orbitals, will
interact strongly with electron-supplying groups of organic molecules.
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Solid Particles in Suspension 141
Still another kind of organic-clay interaction is hydrogen bonding. These
interactions can be classified into three types:
1. Hydrogen bonding between water molecules directly solvating
exchangeable cations and polar functional groups, such as carbonyl, on
organic molecules. The water molecules thus act as a "bridge" between
the cation and organic species.
2. Hydrogen bonding between functional groups such as alcoholic and
amino groups and oxygens of the silicate surfaces. Infrared spectroscopy
has indicated that these are relatively weak bonds, being within the lower
range of energies where hydrogen bonding is found.
3. Intermolecular hydrogen bonding between two organic species on
the clay curface. Other factors involved in clay-organic interactions
include physical forces and entropy effects.
With this general description of the interactions of organic species with
clays, it is now appropriate to mention some special clay-organic
properties that have relevance to organic pollutants. Many organic
compounds, including aromatics and particularly the halogenated types
such as DDT, chlorinated and brominated phenyls and biphenyls, are
adsorbed to little if any extent on clay surfaces from aqueous solution. In
the natural environment they are more likely to be adsorbed in organic
components of soils and sediments. These materials usually have limited
solubility in water, since they are hydrophobic. It is thus not surprising
that they are not attracted to the hydrophilic surfaces of clays. The above
discussion, however, suggests that, in natural systems, clay-organic
complexes may act as adsorbing media for some organic pollutants that
are not adsorbed at all by pure inorganic clays.
Another phenomenon that may take place when organic species are
adsorbed at clay surfaces is that of catalytic alteration. This has particular
relevance for organic pollutants since there is much interest in their fate
in the environment. Much work has been reported on catalytic reactions
on clays at high temperatures, but it is only recently that much attention
has been paid to catalysis by clays in conditions resembling the natural
environment. One mechanism by which clays can act as catalysts is via
their Bronsted acidity. Examples of this are the hydrolysis of esters
demonstrated by McAuli~e and Coleman (1955), the conversion of
atrazine to hydroxyatrazine by Russell et al. (1968), the decomposition of
alkylammonium ions by Chaussidon and Calvet (1965), and the
hydrolysis of nitrites to amides by Sanchez et al. (1972~. In many
decomposition reactions involving Bronsted acidity, carbonium ion
formation is undoubtedly involved. On the other hand, Lewis acid sites
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142 DRINKING WATER AND HEALTH
may exist in clays that also will catalyze many organic reactions. These
sites (electron acceptors) may be part of the basic structure of the mineral
itself as, for example, ferric iron within the octahedral layer or exposed
aluminum on the edges of the minerals. In addition, some cations on
exchange sites function in this capacity, particularly those of the
transition metal group. Solomon et al. (1968) have demonstrated catalytic
properties of Lewis sites located on edges of clay minerals. The activity of
some transition metal cations on exchange sites has also been amply
demonstrated as, for example, the decomposition of urea to ammonium
ion when complexed with Cu2+, Mn2+, or Ni2+ smectite. No such
reaction was noted for urea complexed with alkali metal or alkaline
earth-saturated clay (Mortland, 1966~. Aromatic molecules such as
benzene will complex via pi electrons with clay minerals saturated with
Cu2+, under mildly desiccating conditions. Under more vigorous
dehydrating conditions, a radical cation of benzene is formed that will
react with molecular benzene to give polymers containing phenyl groups
as well as fragmented benzene rings (Doner and Mortland, 1969~. Anisole
(methoxybenzene) will also form radical cations that react with molecular
anisole to give 4,4'-dimethoxybiphenyl (Fenn et al., 1973~. Other cationic
species with oxidizing abilities as great as Cu2+, such as Vo2+ and Fe3+,
were also found to produce radical cations from some aromatic species
with subsequent polymer formation (Pinnavaia et al., 1974~. These
reactions suggest the possibility that some pollutant species adsorbed on
clay surfaces may undergo similar reactions to form radical cations and
subsequently interact with themselves, or other organic compounds with
formation of different chemical derivatives. Thus, pollutant degradation
or alteration on clays by oxidation-reduction reactions involving ex-
changeable transition-metal cations may be a real possibility in nature.
In addition to the degradation of atrazine to hydroxyatrazine,
mentioned above, a number of other clay-catalyzed pesticide reactions
have been reported. For example, Fleck and Halter (1945) report the
conversion of DDT to DDE by kaolinite and smectite samples, preheated
to 400°K. Also, degradation of heptachlor by palygorskite has been
suggested by Malina et al. (1956~. The degradation of the organic
phosphate insecticide, ronnel, by clays heated to various temperatures
has been reported by Rosenfield and van Valkenburg (1965~. Organic
phosphate pesticides have been observed by Mortland and Raman (1967)
to be hydrolyzed in the presence of Cu2+-montmorillonite by a
coordination mechanism. The much weaker catalytic e~ects of Cu2+-
vermiculite, beidellite, and nontronite were attributed to reduced activity
of the copper on these minerals, as compared with montmorillonite, due
to charge location. While most of the degradation of pesticides in nature
OCR for page 143
Solid Particles in Suspension 143
has been attributed to biological agencies, the above discussion would
suggest that catalysis at mineral surfaces may also play a role.
Natural organic material in soils forms complexes with clays that exert
important influences on the physical, chemical, and biological properties
of the soil (Greenland, 1965, 1971~. Since the exact chemical and physical
nature of these organic materials is not known, the kinds of interaction
they have with clays are less well known than those of well-defined
organic compounds. However, some of the kinds of reactions described
above are probably involved. It is obvious that clays eroded from soil
surfaces into streams and lakes will probably be, to some degree,
complexed with organic matter.
Humic acids, a constituent of soil organic matter, may be strongly
adsorbed by clays, presumably by interaction with positive sites on the
edges of clay particles or with polyvalent cations on the cation exchange
complex acting as "bridges." Schnitzer and Kodama (1967) have shown
that fulvic acid (another constituent of soil organic matter) adsorption
depends on pH, and is greater under acid than alkaline conditions. This is
to be expected, since the fulvic acid would be relatively undissociated at
low pH but considerably more anionic at alkaline pH. Schnitzer and
Kodama (1972) showed that fulvic acid is very strongly bound to Cu2+ on
the exchange sites of montmorillonite through a coordination type of
reaction. In addition, they have shown such adsorption is typical for any
electrophilic cation on the exchange complex, particularly for ions of the
transition metal group.
Summary
Pollutant concentrations are higher in sediments than in the waters with
which they are associated. It should be recognized that the consequences
of pollutant adsorption by clays may be very important in natural
systems and may affect drinking water quality. Clay-pollutant complexes
may be mobilized by erosion from the landscape, or form when eroded
clay enters a stream containing a polluting species. If the complex
survives water treatment and enters the drinking water system, it would
then be available for ingestion by humans. In the adsorbed state on the
clay surface the pollutant is probably not toxic, but the possibility exists
that the pollutant might be released from the clay in the environment of
the alimentary tract and thus exert toxic effects. Whether or not such a
process might take place would depend on the complex in question, so
that no generalities are possible. Information is completely lacking in this
area, and thus research should be encouraged and supported.
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144 DRINKING WATER AND HEALTH
ASBESTOS: NOMENCLATURE, OCCURRENCE AND
REDISTRIBUTION IN WATER
Structure and Nomenclature
Asbestos is the name for a group of naturally occurring hydrated silicate
minerals possessing fibrous morphology and commercial utility. This
definition generally limits application of the term to the minerals
chrysotile, some members of the cummingtonite-grunerite series, crocido-
lite, anthophyllite, and some members of the tremolite-actinolite series.
Amosite is commonly used to refer to a cummingtonite-grunerite
asbestos mineral, but it is a discredited mineral name (Rabbit 1948;
Committee on Mineral Names, 1949~.
Mode of occurrence and fiber length are important determinants of
commercial value. Of the commercially mined and processed asbestos
minerals, chrysotile accounts for about 95%, the remainder being amosite
and crocidolite (May and Lewis, 1970~. Crocidolite is the fibrous
equivalent of riebeckite, and chrysotile belongs to the serpentine group of
minerals, which contains other nonfibrous members (Deer et al., 1970~.
Noncommercial deposits of asbestos minerals are also relatively com
mon.
The standard definitions of the Glossary of Geology (American
Geological Institute, 1972; second printing, 1973) are given below.
ASBESTOS: (a) a commercial term applied to a group of highly fibrous silicate
minerals that readily separate into long, thin, strong fibers of sufficient flexibility
to be woven, are heat resistant and chemically inert, and possess a high electric
insulation, and therefore are suitable for uses (as in yarn, cloth, paper, paint,
brake linings, tiles, insulation cement, fillers, and filters), where incombustible,
nonconducting, or chemically resistant material is required. (b) a mineral of the
asbestos group, principally chrysotile (best adapted for spinning) and certain
fibrous varieties of amphibole (ex. tremolite, actinolite, and crocidolite). (c) a term
strictly applied to the fibrous variety of actinolite. Syn: asbestos; amianthus;
earth flax; mountain leather.
ASBESTIFORM: Said of a mineral that is fibrous, i.e. that is like asbestos.
ACICULAR (Cryst): Said of a crystal that is needlelike in form. Of: fascicular,
sagenitic
FIBROUS: Said of the habit of a mineral, and of the mineral itself (e.g. asbestos),
that crystallizes in elongated thin, needle-like grains, or fibers.
The nomenclature used in this report conforms generally to these
definitions, subject only to the further qualifications that the term
asbestos will not be used in its most restrictive sense (c, above);
OCR for page 145
Solid Particles in Suspension 145
asbestiform will not be used; and the terms acicular and fibrous are to be
understood as discussed below.
The term asbestos has often been used in recent scientific literature to
describe individual fibrous or acicular particles of microscopic and
submicroscopic size. However, mineralogists and geologists have has-
tened to point out that the term should be used only as defined above, in
reference to the minerals in bulk. Ampian (1976) considers the terms
asbestos and asbestiform to be synonymous and that they then may only
be used to apply to the bulb fibrous forms occurring in nature.
Asbestiform is often used to define the morphology of a mineral that is
similar to asbestos, but does not necessarily occur in nature in a
commercial deposit; to avoid ambiguity, the term will not be used here.
The terms acicular and fibrous are used here to characterize any
mineral particle that has apparent crystal continuity, a length-to-width
aspect ratio of 3 or more and widths in the micrometer or submicrometer
range. Although the two terms are not strictly synonymous, the use here
of either one to describe a mineral particle should be taken to imply the
other, unless otherwise qualified.
Table IV-2 lists some of the naturally occurring minerals that can have,
but do not always have, an acicular morphology. To this list could be
added a number of synthetic fibers, although they are not naturally
occurring minerals. Many of the minerals in Table IV-2 are common
rock-forming minerals.
Properties of Asbestos Minerals
MINERALOGY
The asbestos minerals belong to the serpentine and amphibole groups,
and the amphiboles are further divided into those of the orthorhombic
crystal system (orthoamphiboles) and amphiboles of the monoclinic
crystal system (clinoamphiboles). Table IV-3 summarizes the basic
properties of the asbestos minerals.
Chrysotile is the asbestos mineral of the serpentine group. Its crystal
structure is a double sheet, comprising a layer of silica tetrahedra and a
layer of magnesia octahedra, arranged in a manner that is somewhat
analogous to the alumina octahedra silica tetrahedra layering of
kaolinite. The way in which the sheet structure is modified to develop a
fibrous morphology is, in detail, very complex; but in essence the
modification can be imagined as a buckling of the double sheet, due to
misfits, to form a hollow tube (Deer et al., 1966~. This central tube may or
may not be filled with electron-opaque material, and the appearance of its
OCR for page 194
194 DRINKING WATER AND HEALTH
Committee on Mineral Names. 1949. Am. Min. 34:339.
Cotterell, K., and P.F. Halt. 1972. An examination of crocidolites from North West Cape
and Transvaal Mines. Inst. Min. Metall. Trans. Sect. B. 81:169-171.
Cralley, LJ., R.G. Keenan, J.R. Lynch, and W.S. Lainhart. 1968. Source and identification
of respirable fibers. J. Am. Ind. Hyg. Assoc. 29:129-135.
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water. Nature 232:332-333.
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OCR for page 195
Solid Particles in Suspension 195
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204 DRINKING WATER AND H"LTH
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Representative terms from entire chapter:
humic acid
