Ascorbic acid reduction of residual active chlorine in potable water
 prior to  halocarboxylate determination!


 Edward T. Urbansky,* David M. Freeman} and F. Javier Rubio§

 United States Environmental Protection Agency, Office of Research and Development,
 National Risk Management Research Laboratory,  Water Supply and Water Resources
 Division, 26 West Martin Luther King Drive, Cincinnati,  OH 45268, USA.
 E-mail: Urbansky.Edward@EPA.gov; Fax:  +1 513 569 7658; Tel: +1 513 569 7655

 Received 7th February 2000, Accepted 23rd March 2000
 Published on the Web 9th May 2000
 In studies on the formation of disinfection byproducts (DBFs), it is necessary to scavenge residual active
 (oxidizing) chlorine in order to fix the chlorination byproducts (such as haloethanoates) at a point in time.
 Such research projects often have distinct needs from requirements for regulatory compliance monitoring. Thus,
 methods designed for compliance monitoring are not always directly applicable, but must be adapted. This
 research describes an  adaptation of EPA Method 552 in which ascorbic acid treatment is shown to be a
 satisfactory means for reducing residual oxidizing chlorine, Le., HOC1, CIO", and C12, prior to determining
 concentrations of halocarboxylates. Ascorbic acid rapidly reduces oxidizing chlorine compounds, and it has the
 advantage of producing inorganic halides and dehydroascorbic acid as opposed to halogenated organic
 molecules as byproducts. In deionized water and a sample of chlorinated tap water, systematic biases relative to
 strict adherence to Method 552 were precise and could be corrected for using similarly treated standards  and
 analyte-fortified (spiked) samples. This was demonstrated for the quantitation of chloroethanoate,
 bromoethanoate,  2,2-dichloropropanoate (dalapon), trichloroethanoate, bromochloroethanoate, and
 bromodichloroethanoate when extracted, as the acids, into tert-butyl methyl ether (MTBE) and esterified with
 diazomethane prior to gas chromatography with electron capture detection (GC-ECD). Recoveries for
 chloroethanoate,  bromoethanoate, dalapon, dichloroethanoate, trichloroethanoate, bromochloroethanoate,
 bromodichloroethanoate, dibromoethanoate, and 2-bromopropanoate at concentrations near the lower limit of
 detection were acceptable. Ascorbic acid reduction appears to be the best option presently available when there
 is a need to quench residual oxidants fast in a DBF formation study without generating other halospecies but
 must be implemented  cautiously to ensure no untoward interactions in the matrix.
Aim of investigation

Issues surrounding the decision to reduce residual oxidizing
disinfectants (Le., C12, HOC1, and NaOCl) have been discussed
previously as related to the analysis of halogenated disinfection
byproducts.1  The desirable characteristics of dechlorinating
agents and  the  relevant chemical  concerns  have  also been
covered,  including deficiencies of some reagents used in this
manner.1  In this  report, we evaluate  ascorbic  acid as  a
dechlorinating agent in the determination of haloacetic acids
containing bromine and chlorine. Previous work suggested that
ascorbic  acid (HAsc) might prove suitable for the  haloacetic
acids.1'2
  EPA's   Environmental Monitoring  Systems  Laboratory
(EMSL)  established Method  552 for the  quantitation  of
halocarboxylates (often referred to  as the haloacetic acids  or
HAAs) in 1990.3 This version used diazomethane (CH2N2) to
esterify the extracted carboxylic acids. In 1995, concerns over
diazomethane led EPA's National Exposure Research Labora-
tory (NERL, previously EMSL) to change the esterification
reagent to acidic methanol.4  However, many laboratories,
including our own, have continued to safely use diazomethane
tThis  paper is the  work product  of United States government
employees engaged in their official duties. As such, it is in the public
domain and exempt from copyright restrictions. © US government.
^Funding for  this position was  provided by  EPA's Research
Apprenticeship Program.
§On leave from Departamento de Ingenieria Quimica y  Energetica,
Universidad de Extremadura, Avda. de Elvas s/n, 06071, Badajoz,
Spain. E-mail: fjrubio@unex.es; Tel. 11 34 924 289385.
 for methylation.  In addition to changing the esterification,
 Revision  1.0 prescribes  ammonium  chloride  to convert
 chlorine-based oxidants to chloramine.4 EPA's NERL demon-
 strated that ammonium ion is satisfactory within a specified
 limit of error and under a variety of drinking water conditions,
 using multiple laboratory testing. Nonetheless, the search for
 chlorine-oxidant scavengers that are generally useful for a wide
 variety of analytes continues. Following from previous work,1
 ascorbic acid was evaluated as a dechlorinating reagent prior
 to the quantitation of certain  halocarboxylates  in  aqueous
 solution with particular interest in applying it to drinking water
 analysis.


 Experimental section^

 Part I. Effects at high analyte concentrations OSOngmL"1)

  Standards and test solutions. Halocarboxylic acid standards
 in  tert-butyl  methyl ether were  obtained   from  Supelco
 (Bellefonte, PA,  USA). Aliquots of the commercial solution
 were injected via gaslight syringes into 20.0 mL  portions  of
doubly deionized water  in  40 mL EPA vials  (polypropylene
screw caps and PTFE septa) to produce standard test solutions.
Twelve solutions at each  concentration  were prepared by
injecting 0,10,20, or 50 uL of the stock standard. This gave the
following concentrations: for chloroethanoic and dichloroetha-
noic acids, 0, 150, 300, TSOngmL"1; for bromoethanoic,

^Mention of  specific  brand names,  manufacturers, or models
throughout this paper should not be construed to reflect endorsement
of firms or products by the United States government.
DOI: 10.1039/b001046o
                                                                           7. Environ. MoniL, 2000, 2, 253-256
                                 This journal is © The Royal Society of Chemistry 2000
                                                    253

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2,2-dichloropropanoic, bromochloroethanoic, and bromodi-
chlorocthanoic  acids,  0,  100,  200, 500 ngmL"1;  and  for
trichloroethanoic, dibromoethanoic, and 2-bromopropanoic
acids, 0, 50, 100, 250 ngmL"1.
  These were acidified with 1.0 mL of 0.25 M sulfuric acid to
minimize hydrolysis. Analyte concentrations for Part I  are
about 100 times greater than what would be found in most
chlorinated potable water supplies. The concentrations were
intentionally elevated with the aim of magnifying any adverse
impacts as the concentrations of both the ascorbic acid and the
analytes are very large relative to the lower limits of detection.
A slow interaction, for example, might not be distinguishable
from the normal imprecision of the method at low concentra-
tions, but would be made more apparent if the concentrations
were increased.

  Ascorbic  add  addition. Six   of the standards  at each
concentration  were  reserved for  the  addition of ascorbic
acid. A 2.00 mL aliquot of I.I M L-ascorbic acid solution was
pipetted into each  test standard, producing a post-mixing
concentration of 0.10 M. This final concentration was chosen to
ensure excess  HAsc relative  to  typical residual chlorine
concentrations found in tap water and to make any interactions
more apparent.

  Sample  treatment. Half  of each set  (3  with  HAsc and 3
without) of standards was analyzed immediately. The other
half (3 with HAsc and 3 without) was retained for 16 d at
7±2"C. After addition of 2.0 mL of 98% w/w H2SO4, each
standard was  extracted with  4.0 mL  of pesticide residue
analysis grade rert-butyl methyl ether; dropwise addition of
0,25% w/w FD&C Blue No. 1  (Erioglaucine  [3844-45-9]
CI  42090)  aqueous  solution improved the  visibility  of  the
phase boundary.  Extracts were drawn  off from the aqueous
phase and dried with anhydrous environmental analysis grade
sodium sulfate. The carboxylic  acid moieties were esterified
with diazomethane using a method described elsewhere,5 then
transferred to autosampler vials and stored in a freezer at
-80 °C pending GC-ECD analysis.

  GC-ECD analysis. Extracts were  analyzed on a Hewlett-
Packard  (Palo  Alto,  CA, USA)  6890  GC-ECD  system
equipped  with  an  HP  7673  autoinjector.  Volumes   of
2.5-5.0 uL  (splitless)  were injected  onto  a J&W  Scientific
(Folsom,  CA,  USA)  DB-5MS  column   (30mx250um
id x 0.25 urn film) at constant  (high purity) helium flow of
1.0 mL rain"1;  inlet  and detector  temperatures:  270 °C.
Temperature  program:  hold   35 °C  for  10.0 min;  ramp
5.0°Cmin~' to 75"C, hold for 15.0min; ramp 5.0°Cmin"'
to 100 °C, hold for 5.0 min; ramp 5.0 "C min"1 to 135 °C; hold
for 2.0 min. Analytes, chemical formulae, and related informa-
tion are given in Table 1.
  Recovery from fortified  tap  water. Cincinnati tap water
(source: Ohio River) was collected from a laboratory faucet
and represents a typical chlorinated municipal water supply.
After 10 min of high flow to flush the pipes, water was collected
in glass vessels and used within 1 h of collection. Ten replicates
were fortified with 20.0 uL of the HAA standard and 1.00 mL
of 0.25 M sulfuric acid. Five of each were treated with 2.0 mL of
1.1 M ascorbic acid, the same as the standards. After capping
and mixing, samples were extracted and analyzed as described
above. Unspiked samples  were  used to determine the back-
ground levels of chlorination byproduct analytes.

  Determination of residual active chlorine in tap water.
Chlorine was determined titrimetrically with  ferrous ammo-
nium sulfate after reaction with 7V,A^-diethyl-/j-phenylenedia-
mine  (DPD).  Commercial DPD  #1 Powder  reagent  mix
(LaMotte Co.,  Chestertown,  MD,  USA) was  used.  The
method was essentially that in Standard Methods.6 Reduction
of residual oxidant was demonstrated by the absence of color
when DPD reagent was added  to  tap water pretreated  with
HAsc.

Part H. Effects at low analyte concentrations (2—10 ng mL"1)

  Standards and test solutions. Halocarboxylic acid standards
in /ert-butyl methyl  ether were obtained  from  Supelco.
Aliquots of the commercial solution were injected via gastight
syringes into 30.0 mL portions  of Cincinnati tap water in
40 mL EPA vials to produce standard test solutions. Three
vials with 0.10 M HAsc (made by direct addition of the solid
reagent) and three vials without were prepared at the analyte
concentrations shown in Table 2. These concentrations reflect
those likely to  be encountered  in  chlorinated potable water
supplies. The samples were analyzed immediately; therefore, no
additional acid  was added for preservation.

  Sample treatment and analysis. Other than the ascorbic acid
used to  reduce the  oxidizing  chlorine,  EPA  Method  552
(microextraction)4 was used for these samples. The methylated
extracts were analyzed on a Tremetrics 540 GC (Austin, TX,
USA)   with  a  J&W DB-1701   column   (30 mx 322 urn
id x 0.25 jim  film)  at constant  He  pressure  of 101 kPa
(ISpsi).  Injections  of 2.0 uL were  used. The  temperature
program was that of Method 552.


Results and discussion

Part I. Effects at high analyte concentrations (30-100 ng mL"1)

  Data treatment. Chromatographic peak areas were plotted
against volume of standard used (uL) in 20 mL of water; see
Table 1 for  further  explanation. Each  line  represents  3
replicates  at each  of 3  concentrations for  each analyte.
Table 1 Halocarboxylate analytes examined in this work
Analyte onion
                                 Formula of acid
                                                          CAS RN"
                    (,/min
Concentration/ug mL~l
Chlorocthanoate
Bromoethanoate
2,2-Dichloropropanoate''
Dichloroethanoate
Tricbloroethanoate
Bromochlorocthanoate
Bromodichloroethanoate
Dibromocthanoate
2-Bromopropanoate
ClCHoCOiH
BrCH,CO-,H
CH3CC12C02H
C12CHCO2H
C13CCO,H
BrClCHCOH
BrCl,CCO,H
Br,CHCO2H
CH3CBrHCO2H
[79-11-8]
179-08-3]
[75-99-0]
[79-43-6]
[76-03-9]
[55589-96-3]
[7113-314-7]
[631-64-1]
[598-72-1]
5.2
8.4
8.8
9.2
12.8
14.8
17.4
17.9
18.3
300'
200
200
300
100
200
200
100
100
"Registry numbers are for the acids, not the anions. 'Retention times are for the methyl esters and were established using a methyl ester blend
standard purchased from Supelco and refer to the DB-1701 column. 'Concentrations refer to the concentration of each acid in the standard
purchased from Supelco; thus, a lOuL aliquot of standard diluted into 20 mL of water gives a chloroethanoate concentration of 150 ngmL"1
(ppb), etc. ^Parent acid is also known as dalapon.
254     J. Environ. Monit., 2000, 2, 253-256

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 Table 2 Difference in analyte recovery near the detection limit for samples dechlorinated with ascorbic acid relative to untreated samples"

 Analyte                    Concentration/ng mL'1      Relative recovery (%)      Concentration/ngmL"1
                                                                         Relative recovery (%)
Chloroethanoate
Bromoethanoate
2,2-Dichloropropanoate
Dichloroethanoate
Trichloroethanoate
Bromochloroetlianoate
Bromodichloroethanoate
Dibromoethanoate
2-Bromopropanoate
5.0
3.3
3.3
5.0
1.7
3.3
3.3
1.7
1.7
-2±10
-17+4
+ 8±4
+ 1+3
-16±4
+ 19±5
-20+20
+ I4±6
+ 6±2
10
6.6
6.6
10
3.3
6.6
6.6
3.3
3.3 -
— 5+fi
JX o
— 11+4
1 1 3-*t
+ 3 + 2
+ 3±2
+ 10±5
+ 10+5
-S0±10
+5±5
-9±2
  Differences were calculated from the average of three fortified test solutions of Cincinnati tap water with HAsc and three without. Relative
 difference=(^w/HA5e-/4w/?)//4w;0, expressed as a percent. Uncertainty was propagated from the estimated standard deviations of the means  No
 data were rejected as outljers. Other than the use of ascorbic acid, Method 552 (microextraction) was strictly followed.
 Slopes and y-intercepts were determined by unweighted least
 squares linear regression; the ^-intercepts were either statisti-
 cally indistinct from zero based on the standard errors or less
 than 10% different from their standard errors.  Propagated
 error was computed in the standard way.7

   Initial effects.  The  effect  of ascorbic  acid  on  method
 performance is examined by computing the relative difference
 in the slopes of calibration curves made in deionized water with
 and  without  ascorbic  acid treatment: (fn^^^^-m^lm^i,,,
 where mv/0 is the slope without ascorbic acid and TOW/HA*; is the
 slope with  ascorbic acid. Relative differences  are  shown in
 Table 3. Comparison  of the slopes on  day zero shows that
 ascorbic acid has minimal, but quantitatable impact directly on
 the  analytical procedure in  deionized water. Although the
 difference for 2,2-dichloropropanoate is of debatable meaning,
 bromochloroethanoate   and   bromodichloroethanoate   are
 demonstrably  affected,  with signal reductions of  11% and
 17%, respectively. It is unclear whether this is due to a loss of
 sensitivity or a loss of the analytes themselves. Regardless, the
 standard errors  of the least  squares  parameters  and  the
 regression coefficients indicate that the effect is quantitatable
 and precise; therefore, it should represent a correctable bias in
 this  instance.   For   bromochloroethanoate  with  HAsc:
 m=383±16;  J?2=0.982; for  bromodichloroethanoate  with
 HAsc: m=258±13; .R2=0.976; ^-intercepts were statistically
 indistinguishable from zero based on their standard errors.

  Effects of extended exposure to HAsc. After 16 d of exposure
 to ascorbic acid, all analytes showed a signal reduction relative
 to samples stored without ascorbic acid except for  trichloro-
 ethanoate, which showed a gain of questionable significance,
 5 ±4% (see Table 3). The greatest loss that was distinguishable
 from the  propagated  error was 6% for  chloroethanoate.
 Consequently, we conclude that this reagent could be readily
 used for reducing residual chlorine,  provided that suitable

Table 3 Relative differences in slopes of  unweighted least squares
calibration lines showing the effect of ascorbic acid treatment"
                                DayO*
                                                   Day
Chloroethanoate
Bromoethanoate
2,2-Dichloropropanoate
Trichloroethanoate
Bromochloroethanoate
Bromodichloroethanoate
+ 0.2 ±2%
 +4±4
  -4±4
  -3±7
 -11±4
 -17 + 5
-6 ±2%
-3±2
-4±3
+ 5±4
-8±8
-6±9
"Calibration lines were plots of peak area vs. volume of standard;
each line was  determined from duplicate test solutions prepared at
five concentrations  by diluting specific volumes of standard into
20.0 mL of water: 0 (blank), 10, 20, 50, 100 uL. 'Relative differen-
ce=(mWrtiAsc—mw/0)/mw/0, expressed as a percent; uncertainty was
propagated from the  standard errors of the least squares  slopes.
"Sets with and without HAsc were stored for 16 d in a cold room at
7±2°C.
                                standards are prepared concurrently with sampling. It is not
                                possible to state whether the effects on bromochloroethanoate
                                and bromodichloroethanoate  that  are suggested  by the day
                                zero data are (1) mediated by other matrix elements over time,
                                (2) rapidly  brought about so that no additional effects are
                                observable over 16 d, or (3) masked by the uncertainties of the
                                experimental measurement. Any of these or some combination
                                thereof is possible.

                                  Recovery from  fortified  tap water.  The  concentration of
                                residual active chlorine, [Cl2]+[HOCl]+[CIO~], in the Cin-
                                cinnati  tap water samples found by DPD Fe" titrimetry was
                                13 UM=890 ug LT1 C12. Blank correction  was made by deter-
                                mining  background levels of chlorination byproduct analytes
                                in unspiked tap water samples  and these were subtracted prior
                                to comparison of HAsc-treated and untreated samples. Fig. 1
                                shows the results for the HAAs. Analyte  response in fortified
                                tap water is actually increased a few percent after ascorbic acid
                                treatment; however, this is certainly within  acceptable limits.
                                We note that EPA Method 552 allows for  up to 20% variation
                                in analyte  recoveries  for quality  control test samples in
                                deionized water, and up to 30% variation in analyte recoveries
                                for fortified (spiked) tap water samples.
bromodichloro
bromochloro
trichloro
2.2-dichloro-
prapanoate
chloro
C
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w
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5 10 15 20 25 3C
                               area/1000

Fig. 1 Relative recoveries (average chromatographic peak areas) for
several haloethanoates and 2,2-dichloropropanoate in deionized (DI)
water and Cincinnati tap water. Areas are based on a concentration of
300ngmL~' relative to chloroethanoate (see Table! to determine
other analytes) and are blank-corrected. Recovery  in tap water falls
within the permissible 30% window given in Method 552 relative to DI
water when not treated with ascorbic acid (black bars). Hatched bars
show effect of treatment with 0.10 M ascorbic acid. In general, ascorbic
acid  lowers the recovery in both DI water and tap water; however,
bromochloro- and bromodichloroethanoate showed increased recovery
in tap water. Although the allowable variation in recovery is 20% in DI
water for Method 552, we infer that this concentration of ascorbic acid
works well enough to allow quantitation, but probably influences
conditions enough to warrant careful consideration before it is used in
the matrix  under study.
                                                                                /. Environ. Monit., 2000, 2, 253-256    255

-------
  Based on the results  obtained under our  conditions, we
found  that ascorbic acid was  suitable for the reduction  of
residual oxidizing chlorine, even when used in very large excess.
We speculate that a more conservative addition of this reagent
might  result in even smaller effects. Because  the data show
precise biases, the effects we observed could be corrected for by
the appropriate treatment of standards and spiked samples.

Part n. Effects at low analyte concentrations (2-10 ng mL"1)

In order to determine the effect of ascorbic acid near the lower
limit of detection, relative differences were computed using the
average peak areas for the three treated and three untreated test
solutions made by spiking Cincinnati tap water. Table 2 shows
that there is a reproducible and quantitatable effect for all but
the most highly oxidized species, specifically, bromodichloro-
ethanoate and trichloroethanoate.  Bromodichloroethanoate
quantitation is intrisically imprecise and this effect is somewhat
magnified by the ascorbic acid, especially  near the detection
limit. At 6.6 ng mLT1, the mean peak area for three replicates
demonstrated a 16% RSD without HAsc, but  the imprecision
grew to 42% RSD for the HAsc-treated samples. Such effects
were previously observed1 for other analytes with  a highly
oxidized carbon atom (especially a trihalocarbon).
  Bromochloroethanoate experiences a rather curious gain in
response  upon  addition of  ascorbic  acid.  As  with the
trihalocarbon effect, this has also been observed1  for certain
analytes. The mechanisms through which these effects occur
remain unstudied. Based on these and previous results,1 it is
reasonable to  speculate that  ascorbic  acid  interacts  with
trihalogenated  carbon atoms.  The  magnitude of the  effect
appears to vary with analyte concentration. This variability is
especially noticeable for  bromodichloroethanoate. Caution is
therefore warranted when using ascorbic acid  to dechlorinate
water  samples prior to the  quantitative  determination  of
chlorination  byproducts containing   trihalo  (haloformyl)
carbon atoms. In  a  DBF formation study, it would  be
necessary to carefully assess the side effects of ascorbic acid
(used as a chlorine reductant) within a particular matrix.  In
routine monitoring of drinking water, ascorbic acid may  be
suboptimal for bromodichloroethanoate, but it has minimal or
no effects on the monohalogenated species. It is worth pointing
out, however,  that Method  552  was never validated for
bromodichloroethanoate, which we included in  this study.
Furthermore, we have found that methylation of brominated
trihaloethanoates with diazomethane suffers from complicat-
ing side reactions;8 this  implies that ascorbic acid treatment
should be verified separately using acidic methanol  (Method
552.2)  for the brominated  trihaloethanoates. The reaction
chemistry  of the  dihalo-  and  trihalocarboxylates   under
drinking water conditions is not well-developed. Consequently,
it  is   difficult  to  predict  what conditions  will  promote
dccarboxylation,  hydrolysis,  reduction,  or substitution and
thereby complicate the analytical chemistry.  Under the best
conditions, the quantitation of these  species is  challenging;
thus,  careful attention must  be paid to  avoid introducing
additional sources of error.

Concluding remarks

Our results suggest that,  under some conditions, ascorbic acid
can be used to reduce oxidizing chlorine compounds in order to
fix the concentration of chlorination byproducts in tune. Such
quenching is particularly useful in studies on the formation of
chlorination byproducts where very substantial concentrations
of oxidizing disinfectants are likely to be present. In these cases,
the ammonium ion used in Method 552.2 would be inadequate
as it reacts stoichiometrically with  hypochlorite to  give
chloramine (except under breakpoint conditions). If samples
are to be drawn as a function of time, it is clearly necessary to
prevent subsequent chlorination of carbonaceous material.
Obviously, any reductant chosen must not adversely interfere
in the analysis. These preliminary experiments showed  that
ascorbic acid met  the  criteria1 for the following analytes:
chloroethanoatej bromoethanoate,|| 2,2-dichloropropanoate,||
dichloroethanoate,|| trichloroethanoate,|| bromochloroethano-
ate,|| dibromoethanoate,|| and 2-bromopropanoate in deionized
water and a local  chlorinated potable  water supply.  None-
theless,  care must be taken to evaluate any method modifica-
tion  in a particular matrix, as we pointed out previously when
we used ascorbic acid in the Ames assay.9 In light of the other
reductants that we have considered, ascorbic acid has been the
most successful  in meeting  both  the  bioanalytical  and
chemoanalytical needs of disinfection  byproduct formation
studies. As always, there is a balance to be struck between the
objectives of a particular study  and the requisite levels of
accuracy and precision in analytical measurements. We believe
that judicious use of ascorbic  acid can serve an important role
in drinking water analytical  chemistry  and warrants further
consideration in this capacity.
Acknowledgements

We thank Warner-Jenkinson Co., Inc.  (St. Louis, MO), for
providing a complimentary sample of FD&C Blue No. 1. We
mention key staff, without whom, the Research Apprenticeship
Program would not  be  possible:  Andy Avel, Steve James,
Milton Wiggins, Randy Parker, Tiffaney Livingston (EPA) and
Jim Wade (University of Cincinnati).  FJR  acknowledges a
grant from the Junta de Extremadura.
References

1  E. T. Urbansky, /. Environ. Monti., 1999, 1, 471, and references
   therein.
2  Y. Takahashi and  M. Morita, Kankyo Kagaku, 1997, 7, 495.
3  E. T. Urbansky and W. J. Bashe, J. Chromatogr. A, 2000, 867, 143.
4  J.  W. Hodgeson,  J. Collins and R.  E.  Barth,  Method 552.
   Determination of Haloacetic Acids and Dalapon in Drinking Water
   by Liquid-Liquid Extraction, Derivatization, and Gas Chromato-
   graphy  with  Electron  Capture Detection,  US  Environmental
   Protection Agency, Cincinnati, OH, July 1990.
5  J. W. Hodgeson, D. J. Munch, J. W. Munch and A. M. Pawlecki,
   Method 552.2. Determination of Haloacetic  Acids and Dalapon in
   Drinking Water by Liquid-Liquid Extraction, Derivatization, and
   Gas Chromatography with Electron Capture Detection, Rev. 1.0, in
   Methods for the Determination of Organic Compounds in Drinking
   Water,  Supplement III, US Environmental Protection  Agency,
   Cincinnati, OH, August 1995, EPA/600/R-95/131.
6  Standard Methods for the Examination of Water and Wastewater,
   American  Public  Health  Association/American  Water  Works
   Association/Water  Environment Federation,   Baltimore, MD,
   20th edn., 1998, Method 4500-C1:G, pp. 4.63^.64.
7  P. R. Bevington and D. K. Robinson, Data Reduction and Error
   Analysis for the Physical Sciences, WCB/McGraw-Hill, Boston, 2nd
   edn., 1992, p. 43.
8  F. J. Rubio, E. T. Urbansky and M.  L. Magnuson, J.  Environ.
   Monit., 2000, 2 (DOI: 10.1039/b000674m).
9  E. T. Urbansky and K. M. Schenck, /. Environ. Monit., 2000, 2,
   161.
UThesc analytes are  often collectively  referred to as HAA6 (six
haloacetic acids included in EPA's Information Collection Rule).
256     J. Environ. Monit., 2000, 2, 253-256

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