The Science of the Total Enuironment,

47 (1985)
299-315
Elsevier Science Publishers
B.V., Amsterdam
-Printed
in The Netherlands

ALTERNATIVE

METHOOS

FOR CHLORINATION

F. Fiessinger,
Laboratoire

J.J.
Central

Rook and
Lyonnaise

J.P.
des

Ouguet
Eaux,

78230

Le

Pecq

299

(France)

ABSTRACT
Existing
disinfectants
are
oxidative
agents
which
all
present
effects
on
subsequent
treatment
processes.
None of them has decisive
over
chlorine,
althouqh
chlorine-dioxide
and
chloramines
might
at
preferable.
Optimum
treatment
practices
will
improve
the
removal
orecursors
before
final
disinfection
which
could
then
consist
in a liqht
addition.
A
in
water
treatmentphilosophy
of
radical
change
encompassing
physical
treatment
without
chemicals
such
as
membrane
solid
disinfectants
is presented.

negative
advantages
times
be
of
organic
chlorine
technology
filtration,

INTRODUCTION
Since

its

chlorine

has

broad
its

introduction
held

range
of

chlorine

is

the

only

is

also

used

periods

in

uncovered

organic

matter

the

led

Bruchet

to
et

Figure

is

present

1.

and

Some

of

these

et

known

a large

al.

1984,
like

to

be

able

to

in

the

of

part

or

warm

of

when
undesirable

(TOX)

and

analytical
et

1984b)

as

al.,

et

1983,

illustrated

several
(Simmon

more

techniques

(Christman

al.

toxic

the

Unfortunately,

dichloroacetonitrile,
mutagenic

readily.

during

formation

them
et

its

addition

ammonia

algae

modern

of

Ouguet

of
waters,

In

compounds

use

century,

treated

oxidize
of

halogenated

of

compounds

are

effectiveness.

basins.

results

this
because

in

cost

sedimentation

(THM).

Coleman

is

The

of

disinfectant

proliferation

total

i.e.

identification

chloroform

that

beginning

persistence

its

the

chlorination
;

a1.1984,

ketones,

agent

Trihalomethanes

the

and

controlling

the

reasonable

control

coagulation

in

as reliable

its

chemical
for

compounds

particularly

position

and

Chlorine

has

treatment

effectiveness,

application

halogenated

water

a predominant

biocidal

ease

into

in

chlorinated
al.

1977,

Bull

1980).
The

effects

Many

authors,

(see

Fig.2)

but

influence.
water,

of

water

(Kool,

Thus
variation

the

chlorination
1984)

nature
Cognet
of

,
of

on mutagenic
conclude

that

organics

(1984)
mutagenicity

and

found

activity

chlorination

that

during

during

one

0 1985

Elsevier

Science

Publishers

been

increases

have

chlorination
year

B.V.

was

studied.

mutagenicity

conditions

significative.

0048-9697/85/$03.30

have

chlorination

of
not

treated
statistically

a great
Seine

300

[ 78.8 7. MWc1000
\

VOLATILE5
NON VOLATILES

Diagram
of
Fig.
1.
of a reservoir
water

molecular
(Chalet,

weight
France)

distribution
and speciation

of

TOX after
prechlorination
of the volatile
fraction.

VOLUME OF WATER
i Ilterl

Fig.
2. Comparison
of mutagenic
activity
on Salmonella
TA'98(-'S9)
, before
(xl
and after
prechlorination/Dissoved
of a surface
water
(Moulle,
France)

thyphimurium
air

strain
flotation

301
Another
road

risk

is

transport

and

populated

areas.

of

chlorine,

liquid

situ

are

and

can
at

chlorine,

chlorine

be

toxicity

of

chlorine,

avoided

a 20

to

through

is

by-products

disinfection
ozone,

in

by

using

25 % increase

chlorine

gas

plants

located

sodium

hypochlorite

in

electrolysis

good

costs

might

be

chlorine

during
near

its

densely
instead

(Gomella,1980).

also

respect

to

their

summary

of

oxidant

caused
The

chloramines

permanganate,
(1981)

the

have

reconsidered.

dioxide,

peroxide,

disinfectant,

formation

to

Fiessinger

TABLE

risk

direct

liquid

be

In

applied.

DISINFECTANTS

Although

hydrogen

the
as

though
of

halogenated
water

to

storage

This

generation

ALTERNATIVE

related
its

summarized

possible

the

to

on

a less
and

properties

of

extend

in

ultraviolet
ions.

is

(1980)

disinfectants

with

An

shown

in

use

light,

Gomella

constituents.

surveys

of

drinking

disinfectants

several

water

these

risks

subject

silver

of

with

based

health

entire

alternative

halogens

reactivities

properties

main
and

other

potential

the

extended

table

1.

Comparison

of

Various

Disinfectants

c102

cl2

Iron
and manganese
Ammonia
THM formation
THM precursors
removal
Formation
of mutagens
or toxic
substances
Enhanced
biodegradability
Taste
removal
Disinfection

KMn04

03

+
it+
ttt

it

ttt

tt

t
+
t

tt++

tt++

+
tt

tt
ttt

t
t-

- no effect
+ little
effect
For

the

evaluation
it

process,(see

Fig.31

disinfection,

i.e.

of

must

the

be
either

before

formation

different

properties

distinguished
in
or

where

preoxidation,
after

potential

the

it
as

bulk

(THMFP)

of
has

been

?
?

t-

t
+

effect
very

and

effects

of

applied

in

organic
removed.

effective

is

an intermediate

the

H22

tt
ttt

disinfectant

trihalomethane

NH2C1

an

step
matter,

alternative

the

treatment
or

especially

in

postthe

302

Fig.

3.

Influence

Fig.
4.
process

Possible

of

iight

positions

on

residual

of

oxidation

Cl02

and

chlorite

treatments

in

concentration

surface

water

treatment

303
Preoxidation
Traditionally

preoxidation

process,

to

control

algal

covering

the

treatment

ensure

is

good

growth

hygienic

in

basins

performed,

at

the

conditions

flocculation

p:ovitled

throughout

basins.

that

beginning
the

Thus

ammonia

of

be

treatment

treatment

growth

would

the

can

removed

and

to

be

limited

by

in

subsequent

steps.

Permanganate.
manganese

The

and

at

the

is

relatively

application

destroys

taste

pretreatment

and

dosage
modest

disinfectant

and

distribution

system

of

odor

usually

(Singer

causing

et

the

It

why

is

manganese

oxidizes
can

of

Permanganate
of

reasons

pretreatment

reduction

a1.,1980).
residual

two

in
substances.

applied

possible
are

permanganate

reduce

iron,
THMFP
formation

not

effective

a very

precipitation

permanganate

is

but

chloroform

in

rarely

used

in

the
water

treatment.

Chlorine

dioxide.

pretreatment

are

products

is

chlorite

of

water

is

reported

skin

and

acids

reaction

use

of

chlorine

formation

dioxide

Acha,

be

the

negligible

(Rav
to

of

produces

1984).

The

dioxide

halogenated

polar

main

in
by-

compounds

inorganic

such

by-products

toxic.

promotion

with
short

of

chlorine

initiation

However,

inorganic

(Bull

and

disinfected

observed.
its

effect
However,

ketones

mouse

advantages

1982).

which

Using

great

algicidal

(Stevens

as aldehydes,

The

essays

chlorine

dioxide

term

toxicity

of

products

may

present

among

were

chlorine

mice

when

applied,
dioxide

a higher

no
and

risk

concentrates
effect

more

than

was

specifically

chlorine

or

ozone

19801.

Chlorite
been

(C102-)

found

to

uncertainties

have

chlorine

dioxide

mg/l

at
to

to
hand

necessitates
The
chlorine

such

health

many

the
costs
for
(Gomella,

in

authorities

low

level,

1984).

Cl02

to
is

In
the

that
applied
of

applying
1980).

chlorine

cause.

(Hoff,

in

basins

open

dioxide

dose

analytical

are

3 to

low

as 0.1
by-

concentrations
are

chlorine

Longley

not

4 times

,198l).

is
On the

of

1981)
than

yet

dioxide

photodecomposition

(Fiessinger,

of

inorganic

problems
of

1981,
the

as

these

by-products

efficiency

have
These

application

standards

the

mg/l)

1985).
the

maintain

and

chlorine

an excessive

allow

countries

Many

(100

(Komorita,
to

to

disinfective
of

application

some
order

reagents

which
The

concentrations
animals

reluctant
In

edicted.

high
in

countries.

been

be superior
when

(C103-)

methemoglobinemia

monitored

(Masschelein,

reported
other

have

be constantly

solved

chlorate

made
in

chlorites

products
have

and

produce

those

(see
for

Cl02

Fig.4).

304
Ozone.
removal

The

modify

the

increased

Reckhow
the

Singer

precursors
turbidity

humic

TOC

The

polymerizing

more

(Jekel,

1983).

synthetic

organic

hexamers

and

that

ozone

compounds

found

could

prcozonation

along

sized

TOX

removal

of

0.8

mg 03

effect.

may

using

present

a dichlorophenol

induced
improve

improved

below

micropollutants

ozonation

Doses
THM and

with

ratio's

a1.(1985a))

will

of

no further

waters

fig.6).

improved

in

had

lake

removal

particles

small

which

certain
(see

the

applied

and

that

polymers,

preozonated

case

of

reported

ratio

on

Duguet

improved

however,

significantly

however

was

of

of

for

this

to
The

coagulation

example
found

in

hampered

mineral

of

insoluble

TOX

liter

coated

possibilities.

that

is

polarity.

improvement

preozonation

preozonation

Increase

effect

interesting

that

Jekel
acid

such

direct

costs.

THM and

TOC per

when

same

its
effect

subsequent

was

The

flocculant

coagulation,.

by

dose,

shown
of

mg

agglomeration,

mg

on

have

in

to

of

A clear

pretreatment
5).

lead
primary

increase

1981).

Fig.

not
The

adsorbability

alum

saving

per

alum

caused

particle

(see

potentials

mg 03
in

oxidative

does

towards

(Kuehn,

by

(1984)

formation
1.2

favor

1981)

for

matter
TOC values.

molecules

increased

means

and

exceeding

per

a slighty

an expensive

the

turn

induced

by

organic

unchanged

processes

(Fiessinger,

be achieved

reduced

in

adsorption

removal
water

natural

nearly
of

will

and

Seine

by
nature

polarity

turbidity

of

reflected
chemical

filtration

was

preozonation

as is

polymerization

to

removal

in

coagulation

formation

of

organic

filtration.

As with

other

products
Especially

be

contact

can

be

dosage

be
it

biodegradation

complete

Fig.

ecology

of

experience

has

zooplankton

during

summer

of

mutagens

a1.,1984a)

8)

as

with
place

an

et

al.,

the
periods

will
filtered
(Rook,

as

waters
1983).

and

an

foul

the
contain

also

prolonged
of

organic

1983)

which

disadvantage.
leaves

carbon

which
is

by

Benedek,

water

may

water
It

the

A principle
operated

develop

treated

Ozonation
and

the

ozonation

Fig.7).

disinfection.

biologically

the

1980)

Hoof,1983).

as well
before

1985)

in
(Van

by-

(Mallevialle,

during

(see

advantage

post
in

plankton
that

Hoof

mutagenicity

biologically

higher

shown

acids

biodegradability,(Peel

interfere
taking

to

carbon

production

removed

may

(Van

induce

et

leads

carboxylic

activated

increase
(see

must
since

also
by

(Duguet

naturally

considered

material
plant
the

or

will

the

and

quantified

may
removed

diminish

time

matter

been

by-products

to

also

ketones

have

effectively

possible

ozonation

aldehydes,

aldehydes

Ozonation
can

oxidants,

mostly

This
treatment

disadvantage
filters
filters.
heavy

is

of
that

Practical
loads

of

305

II

WATER [ NO 031

CLARIFIED

WATER (1 PPM 031

-____

FILTEREG

WATER [NO O3 I

FILTERED

WATER [l PPM 03 I

-----+---------0

CLARIFIED

c v-m -_--

20

40

60

60

COAGULANT DOSE - PPM WAC

Fig.
water

5. Effect
(Croissy,

of preozonation
France)

on

clarification

TOX
o---O CHCl3

and

filtration

of

Cormed

arter

chlortnntion

formed

arter

chlorination

aoo-

0z

a surface

-400

600-

t
\
z

-300

;4

-200

F
2
5w
?

E
2x

200-

-100

5
5

Oo

0.1t
03

Fig.6
rination

Effect
of

0.2I

0.3

0.4I

CONSUMED/INITIAL

of preozonation
black
lake
fulvic

on TOX and
acid
(from

0.5I
TOC-

0.6I
MOL/MOL

WC13
formations
Reckow,
Singer,

0.7I

0.8t

o.a"

RATIO

during
19841

subsequent

bhlo-

306
1000

I
TA 98 - S9

I
A

.
<
3
z>
:

///I
?,//

400

\I

\\\
\\\
\

d
200

Fig.
water

7.
at

Effect
three

lOOmI
H20

of ozonation
sample
volumes

conditions
(Le Pecq,

on mutagenic
France)

activity

of

a ground

30-

20-

lo-

0-

m
..:
A+..:.
.
/-=J/.-;
d,
MAY

Fig.
8. Effects
of a filtered

of
water

ozone
dose
(SFW)

JUL

(00)

and

SEPT

contact

OCl

time

(TC)

on

the

biodegradability

307

In
in

our

view

as

slow

mg/l

sand

advantage

an

of

effective

preoxidation

means

filtration.

slow

TOC versus

Post

full

with

preozonated

of

Walker

sand

filters

16 % in

the

can

removing

observed

a doubled
non-ozonated

only

be

obtained

biodegradable
in

comparative

removal

of

TOC,

control

filter.

when

used

subtances,

such

study

35 % of

(1984)

the

of

initial

3.7

Disinfection
The

to

the

combination

reason

kill

or

system

only

to

prevent

of

decreasing

is

the

barrier.

Fig.

chlorine
of

the

point
by

the

toxicity

Some
to

organic

improve

which

chlorine

be

UV

action

but

the

of

chlorine

of

UV).
and

to

verify

of
by

effect

- persistent

residual
of

of

have

toxic

four

like

to

a less

matter

on

in
the

be

basis
network

following

order

NH2Cl.
to

ozone

more

the

the

NHC12"

Ozone

maintain

may

Cl02

less

produce

some

is

chloramine

properties

minimum.

than

it

the

network.

At

formation

of

The

limited

in

has

such

the

that

the

+ hydrogen

peroxide

have

been

surface

water

for

treated

(Germonpre,
of

energetic

disinfectant

at

Besides

significant.

such

UV involves

remains.

extent.
throughout

is

insufficient

high

by-products

>

of

regrowth

efficencies

main

even

may

made

sufficient

a residual

of
be

bacterial

using

another

may

cost.

to

persistence

- germicidal

- no precursor

the

formation

problem

reduction

was

Disinfection

disinfectant

- low

of

exists

organic

oxidants

control

be

show

>OCl-

application

ensuring

matter

data

not

distribution
is

a residual

'HOC1

is

post-disinfection
must

is

the

necessity

case

disinfectant

life

treatment

regrowth.

problem

considered

disinfection

be done
03 t

half
the

life

this

water

protect
This

maintaining

03 'Cl02

treatment

combinations

shown

should

this

the

may

of

complete
to

Experimental

in

half

In

for

Moreover

long
of

choice

its

resulting

dioxide
its

present
quality.

efficiency

9).

matter

advantage

still

contamination.

but

the

hygienic

persistence

disinfectant

(see

after

abandoned.

The
and

further

biodegradable

chlorite

safeguard

germicidal

final

disinfectants

is

activity

best

For

of

prechlorination

any

residual

UV,

and

hygienic

germicidal

use

microorganisms

regrowth
if

of

acute

the

inactivate

from

pronounced
the

for

combinations

different
radicals

This
is

not
:

have

survey
quite

an

shows
easy

studies

03

(H20,

mechanisms
which

short

More

1985).

such
short
that
task.

+ H202
as

half

direct
lifes,

replacement
The

ideal

308

DECREASE

IN RESIDUAL

OZONE

o.51

WITH

TIME

- SEINE

WATER

0.4-

;;i
E
\

; 0.3z
::
0
<

02

2
z
: O.l-

0 0

10

15

T (mid

Fig.

9.

Decrease

in

residual

ozone

with

time

(Seine

water,

France)

TOC : 12mg/I
:2gmg/l
NH

l-!l

\
2

-1000
%
h
T

2
E

RATIO Cl/N
Fig.

10.

Chloroform

formation

during

conventinal

breakpoint

chlorination

curve

309

Chlorine
optimal

still

remains

conditions

for

minimizing

by-product

preferable

to

avoid

high

the

treatment

application
to

maximal

chlorinated

ammonia

to

and

must

be

of

by

disinfection.

determined

hygienic

content

However

with

respect

safeguard.

biological

It

treatment

to
is

in

still
order

to

can

of

compounds

: the

organics

The

may

halogenated

be followed

reduction

resins

USE OF CHLORINE

reduce

compounds.

alumina

means

ensure

FOR A BETTER

objective

strategies
a

its

available

demands.

STRATEGIES

With

best

formation
the

chlorine

ALTERNATIVE

after

reduce

the

and

of

improve

and

specifically

development

further

such

chloramination

the

as
the

mainly

new

the

adsorbents

removal

of

THM's,

use

of

two
chlorine

precursors

such

as

the

destruction

of

activated

precursors

Chloramination
As

illustrated

trihalomethanes
chloramines

of

Although

be

realized

line
to

to

the

measurement

of

are

objective

of

natural

disinfectants

reduce
In

is

this

ammonia,

or

easy

and

have

algal

compounds,

case,

with
not

to

they

halogenated

chloramine

chloramines

containing

corresponding

the
of

chlorine.

weak
to

water

dose

free

chloramines.

maximum
of

in

a chlorine

appearance

with
the

10

at

chloramines

With

adjusted

figure

formed

free

the

properties.
may

in
are

the

without
the

pretreatment

chlorine

dose

addition

process

inhibiting

the

of

control

must

be

ammonia.
is

On

difficult

realize.

The

main

effects.

(1984)

to

chloramines

monochloramine

traces

Krasner

Sensory

related

Although

correlated

TABLE

problems

of

di

(Table

an

is

the

are

tastes

and

predominant

trichloramines

have

form
offensive

odors
at

and
a

pH of

odors

as

2).

2
Threshold

Compounds

Values

Threshold
Aroma

Hypochlorous
Hypochlorite
Monochloramine
Dichloramine

acid
ion

0.28
0.36
0.65
0.15

(mg/l

as Cl21
Flavor

0.24
0.30
0.48
0.13

(from

: Krasner

some

1984)

health
8,

found

the
by

310
The

health

(organic

effects

chloramines

been

found

(Komorita,

cause

1985).

To
may

quality.
of

the

for

This
of

alternative

OPTIMIZATION
As illustrated

obtained

by
remove

to

removals

of

THMFP

in

TOC.

reduction
result

in

ddsorbant

like

clarified

water.

activated

water

which

chlorination.
of

oxidation

new
like

(see

less
adsorption

3 after
was

reduction

of

the

from

reduction

on

of

water

thus

chlorine

after

the

the

to

reduction

to

Figure

of

organics
toxic

In

action
removal

compounds

however,
of

03
which

during

and

final

by

(Ouguet

et

by

the

Duguet

et

al.

by

a factor
adsorption

This
to

chlorination.

are
in

increased

lead

al,

which

shifts

diminished

H202.
can

post-

optimized

products
by

an

organics

an

reported
was

water

feasible

with

illustrated

(TOC)

an

specific

during
be

polar

a study

alumina,

combined
of

is

isotherm

activated

by the

This

can

from

of

peroxide

produces

the

with

non

will

hydrogen

actual
that

drinking

compounds

cases

13.

in
rather

combined

and

organics

a fraction

adsorption

nature

all

Freundlich

optimization

the

with
in

leaves

in

ozone

of

routinely

be

A13+

coagulants
of

as

corresponding

metal

part

halogenated
of

the

water
may

) found

than

is

the

which,

(1983

of

used

of

such

combination

carbon

different

in

the
a large

carbon.

the

Singer
higher

already

yield

end

THM level

THM precursors

frequently

rise

the

Coagulants

utilization

retain

coupled

at
A low

be

but

is

the
of

With

formation

to

in

can

activated

enhanced

of

effects

development;

chlorine

70 %.

activated

of

shown

k-value

an

by

produce

only

TOC and

precursors

Ozonation

preozonation.

of

of

step.

tend

give

ozone

by

observed,

example

dialysis

health

water

changed

chlorine

% to

principle,

adsorbants

12).

of

40

operation

a good

isotherms
1 the

recently

kidney
and

a promising

THM formation.

of

However,

may

e.g.
Fig.

adsorbable

(1985b

unil

Improvements

research

use

treatment

about

carbon

This

while

1985b)

from

of

which

to

formed

have

CHLORINATION

use

each

improvements

adsorbant

the

of

Some

Europe.

the

11 the

reduction

in

in

by

concentrations

production

from

USA has

concentrations
range

a better

removal
monitored

in

BEFORE

of

significant
tends

odors

has

the

by-products

undergoing

taste,

chlorination

reduction

optimization

practice

patients
of

carefully

realized

figure

a great

the

chloramines

THM formation.

REMOVAL

by

permits

of

thus

extent.

OF ORGANICS

treatment

Fe3+

of

be also

a great

in

problems

be

knowledge

research,

utilities

control

the

by a chloramine

This

may

to

more

the

water

control

organics

solve

should

the

and

anemia

which

largest

chloramines

need

hemolytic

be followed

carbon

desired

chloramines

. ..)

to

chloramination
activated

one

of

more

case

is

effective

an

SAND FllTRATlON

SEOIMENTATIGN
/
\

12

CHLORINE
DISINFECTION

1
OZONATION
\\
-\o-GAC FILTRATION

oI

t II

312
100

n_.:_

I
I
I

ChP

1
o
I

75

5c

E
2

2:

(
Ce(mg/l)

Fig.
13.
(Chalet)

Effect
of
on alumina

An additional
is

the

lower
network
may

advantage

reduction
doses

ozonation
on
and activated

of

needed

multiple

of

chlorine
for

the

isotherms
carbon.

having

removed

consumption

maintaining

injections

for

organic

in

the

a desired

of

low

doses

adsorption

distribution

residual.
of

matter

chlorine

of

a lake

as

far

as

system
Depending
at

water

resulting
on the

several

possible
in

state

crucial

of

points

be necessary.

CONCLUSIONS

- There

is

no

satisfactory

. Prechlorination
. Algal

growth

may

. sedimentation
. Ammonia
. Chlorine
alternatives

alternative
should
be

be

for

chlorination:

abandoned

controlled

with

chloramines,

or

coverage

of

open

basins
can

be
dioxide

removed
and

biologically
chloramines

may

constitute

satisfactory

interim

313

. Ozone

should

- Combination

be

of

particular

for

- Chlorine

can

oxidants

might

oxidation

03

a complement

present

for

a replacement.

interesting

as a final
Process

should

be carefully

practices

not

synergistic

effects

in

+ UV.

removed.

biodegradation

Legionella,

as

be maintained

sufficiently

- Disinfection

used

should

disinfectant

sequences

if
of

organic

oxidation,

precursors

are

adsorption

and

designed.

be

revised

in

the

light

of

new

germs,

Giardia,

. ..

- Disinfection

mechanisms

should

be

further

investigated.

- Megatrends
. New disinfectants
Immunological
Immobilized
nascent

chlorine,

. Improved
micro
improved

applications
disinfectants,

removal
and

electrical

Ag

. . .
treatment

techniques

ultrafiltration
coagulants

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