United States
                  Environmental Protection
                  Agency	
Environmental Monitoring
Systems Laboratory
Las Vegas, NV 89193-3478
                  Research and Development
EPA/600/S4-88/011 August 1988
v>EPA         Project Summary
                  Interlaboratory Evaluation of
                  SW-846 Methods  7470 and
                  7471   for the  Determination  of
                  Mercury in  Environmental
                  Samples

                  Werner F. Beckert, J.E. Gebhart, J. D. Messman, and G. F. Wallace
                    The EPA protocols for SW-846
                 Methods 7470  and  7471 are cold-
                 vapor atomic absorption spectro-
                 metric (CV-AAS) methods for the
                 determination of mercury In aqueous
                 and solid environmental  samples,
                 respectively. In continuation of a
                 previous single-laboratory study in
                 which a more sensitive mercury CV-
                 AAS method for environmental anal-
                 yses  was evaluated, the revised CV-
                 AAS method has been subjected to
                 an interlaboratory study. The revised
                 CV-AAS  system, operated  in  an
                 open configuration,  incorporates a
                 dedicated gas  sparging bottle  for
                 reduction-aeration  and an on-line
                 amalgamation/thermal  desorptlon
                 step.  With these modifications, the
                 CV-AAS method provides increased
                 sensitivity and  also alleviates non-
                 specific background absorption  in-
                 terferences so that instrumental
                 background correction is not  re-
                 quired.
                    Silver-wool  amalgamation  cells,
                 mercury stock standard and spiking
                 solutions, a deionized water sample
                 with spiking instructions, a coal fly
                 ash reference material, and instruc-
                 tions for analysis  by the amal-
                 gamation CV-AAS  method  were
                 sent to 18 participating laboratories
                 having prior experience  with the
                 current EPA protocols for Methods
                 7470  and 7471. Ten of  the 18 lab-
                 oratories were  then invited to par-
ticipate  In a  more rigorous col-
laborative study. To  evaluate  the
revised Method 7470, three aqueous
sample types were analyzed: ground
water, waste water,  and dilute nitric
acid. To evaluate the revised Method
7471, three solid sample types were
analyzed: marine sediment,  incin-
erator fly ash, and municipal sewage
sludge. Some  of the samples were
designated for  spiking with inorganic
or organic mercury and also with
copper, a potential interferent
   The analytical results reported by
the collaborating  laboratories were
statistically examined in an attempt
to characterize the overall accuracy,
precision, and ruggedness of  the
amalgamation  CV-AAS method. In
general, the interlaboratory results
indicated that the amalgamation  CV-
AAS  method currently  is  not
sufficiently rugged  for routine  use
but, when properly  implemented by
proficient  laboratory personnel, may
serve  as an alternative approach to
the recirculating CV-AAS method
described in the current  EPA
protocols. To  fully realize the ana-
lytical benefits of the  amalgamation
CV-AAS method  and to  obtain
accurate and precise  data, a
complete appreciation of the integral
factors for successful trace analyses
is essential, and a high  level of
sophisticated operation and operator
skill is required.

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    This  Project  Summary  was
developed by  EPA's  Environmental
Monitoring Systems Laboratory,  Las
Vegas, NV, to announce key findings
of the research  project that is fully
documented in  a separate report of
the same  title  (see Project Report
ordering information at back).

Introduction
    Included  in  publication  SW-846,
entitled  "Test Methods  for Evaluating
Solid  Waste,"  by  the  Office of Solid
Waste and  Emergency Response of the
U.S. Environmental  Protection  Agency
are two analytical protocols,  Methods
7470 and 7471,  for the  determination of
mercury in aqueous and solid  waste
samples by cold-vapor atomic absorp-
tion spectrometry  (CV-AAS).  In  a
previous single-laboratory study, these
EPA  protocols  were  evaluated  and
revised  to  improve  analytical  perfor-
mance.  The protocols  were evaluated
using  aqueous and solid  environmental
samples of homogeneous  and known
compositions in  order to  assess  ac-
curacies and precisions of the methods
without introducing uncertainties due to
sample heterogeneities.
                         The results of  the single-laboratory
                     study indicated, in general,  that  the
                     digestion procedures were satisfactory
                     for  the  samples analyzed; only  minor
                     revisions that would improve, clarify, or
                     increase the flexibility of the  digestion
                     procedures  were recommended. The
                     recirculating  CV-AAS method described
                     in the current EPA protocols was found
                     to   be  adequate  only   for  mercury
                     determinations in samples of  relatively
                     high mercury concentrations.  Significant
                     modifications of the cold-vapor  appa-
                     ratus were recommended and  evaluated
                     to overcome its inadequacy for mercury
                     determinations in samples of  low
                     mercury levels  and to  minimize inter-
                     ferences  caused  by  non-specific
                     absorption  of  the primary  mercury
                     radiation by  organic vapors.  Instrument
                     detectability  was improved  10-fold  by
                     the  use of a gas sparging bottle as a
                     dedicated  reduction-aeration vessel  and
                     silver-wool amalgamation in  the CV-
                     AAS system  operated in  an  open
                     configuration.  The on-line  amal-
                     gamation/thermal desorption process of
                     the  modified CV-AAS   system also
                     effectively  eliminated interferences from
                     water and  organic matrix vapors so that
                            an instrument without dynamic bacl
                            ground correction  capabilities  could b
                            used. Good accuracy and precision wer
                            obtained  with  the amalgamation  CV
                            AAS  system for the analyses  of  foi
                            reference sediment materials.
                               The objective  of this project was  t
                            conduct an interlaboratory  evaluation  c
                            the  revised  EPA protocols  for  th
                            determination  of  mercury in  environ
                            mental samples.  The interlaborator
                            study  was conducted  in three phase;
                            Phase 1 - fabrication and testing of th
                            silver-wool  amalgamation cells  an
                            characterization  of  selected  inter
                            laboratory  study  samples  by the  lea
                            laboratory; Phase  II - preliminary eva
                            uation of the technical  capabilities of th
                            participating  laboratories; and Phase III
                            evaluation  by the  qualifying  lab
                            oratories  of  the amalgamation  CV-AA!
                            method for the determination of mercur
                            in a marine sediment reference materie
                            and in representative aqueous and  solii
                            waste samples. The test  samples  con
                            tained  concentrations  of  endogenou
                            mercury  or  were  spiked with  con
                            centrations  of inorganic or  organ!
                            mercury that were  in the optimal range c
                            the  amalgamation  CV-AAS method  /
 Needle Valve
Charcoal
  Trap
                                   Glass Stopcock
          \
                                                                                                     Absorption
                                                                                                        Cell
                                                           Tygon-to-Glass
                                                            Connections
                                                                                         Chrom-Alumel
                                                                                        Resistance Heating
                                                                                            Winding
  Nitrogen
  Cylinder
            Flow Meter
  Purging Cylinder
(Reduction-Aeration
   Sample Cell)
  Figure 1.    Schematic diagram of the amalgamation CV-AAS system.

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statistical analysis  of  the  mercury
concentration data submitted to Battelle
was  conducted  in an  attempt to char-
acterize  the interlaboratory accuracy,
precision and ruggedness of the amal-
gamation CV-AAS methods.

Experimental

Instrumentation
    The  schematic  diagram of  the
amalgamation  CV-AAS  system  is
presented in Figure 1. Mercury  vapor
evolved from the reduction-aeration  cell
is  trapped and  concentrated by  amal-
gamation on   the  silver-wool plug
positioned  in  the  center  of  the
amalgamation cell.  After the reduction-
aeration and the on-line amalgamation
steps are completed, mercury  is  de-
sorbed from the  silver wool by resistance
heating  to approximately 500°C. The
mercury  vapor is transported  via  a
nitrogen-gas  purge into the absorption
cell,  and the maximum peak  absorbance
is recorded. The appearance time of the
mercury  peak on  the  strip-chart
recorder  with a  1-second  time constant
is  approximately 17 seconds;  the max-
imum peak absorbance occurs between
25 and 30 seconds after heating  of the
silver-wool plug is  initiated.  The  amal-
gamation/thermal  desorption process
eliminates interfering water and organic
vapors prior  to  the mercury absorption
measurement without compromising the
instrument detection limit. Although
continuum-source background correc-
tion  should also compensate  for such
vapor interferences, the increased noise
level in  most  of the  older atomic
absorption systems when operated in the
background-correction  mode degrades
the detection limit. An  additional benefit
of  amalgamation  CV-AAS  is that  the
method can be  successfully  implement-
ed even  by using an atomic absorption
instrument that  is not  equipped with  a
dynamic background-corrector  acces-
sory.

Amalgamation Cells
    To minimize experimental variability,
all mercury amalgamation cells used in
this  study were manufactured, assem-
bled, and tested by Battelle staff. The
amalgamation cell, with an overall  length
of 105 mm, consists of ST 12/5 male and
female ball joints  annealed  to opposite
ends of Pyrex glass tubing (5 mm i.d.). A
silver-wool  plug  (Fisher  Scientific
Company, Fair Lawn, NJ) of 0.7 g, with  a
mass uncertainty of 0.05 g, is inserted
into the Pyrex tube and then compacted
into  a cylinder having  approximate
dimensions of  5 mm diameter and  20
mm length.
    A  92-cm   length   of  22-gauge
Chromel A wire (Fisher Scientific Com-
pany, Fair Lawn, NJ) is wrapped around
the Pyrex  tubing, providing 30 windings
and a resistance of 22 ohms/ft. The 0.7-
g  plug  of silver  wool  quantitatively
amalgamates mercury vapor at a nitro-
gen  carrier-gas flow rate of 0.55 L/min
with no  apparent  buildup of  leak-
inducing backpressure.

Reagents and Standards
    All reagents and standards specified
were reagent  grade or  better; the
deionized water was specified as ASTM
Type II  water (ASTM  D1193).  All
glassware  for sample digestions, sample
dilutions, and standard preparations must
be  prewashed sequentially  with  an
aqueous  detergent solution,  mineral
acids, and Type II water.
    The following samples were used in
this study:
 •  Coal fly ash (NBS-SRM  1633a) with
    a certified  mercury concentration of
    0.16  ± 0.01 jig/g for a sample size
    of at least 250 mg.
 •  Marine   sediment  (MESS-1  ,
    National   Research Council  of
    Canada) with  a reference mercury
    concentration of 0.171 ± 0.014 jig/g
    for a sample size of at least 500 mg.
 •  Incinerator  fly  ash (crushed, sieved
    and   homogenized)  with  no
    detectable  mercury.
 •  Municipal  sewage  sludge (dried,
    sieved and homogenized) with  a
    determined mercury concentration of
    approximately I.4 \iglg.
 •  Ground water  (filtered and acidified
    with nitric  acid) with no detectable
    mercury.
 •  Waste water  with  no  detectable
    mercury.
 •  Deionized water (acidified with nitric
    acid) with no detectable mercury.

Sample Preparation
    The samples  were  prepared  for
analysis  by  using  the  digestion
procedures specified in the  revised
SW-846  Methods  7470  and  7471.
Liquid samples were  digested  with
sulfuric acid, nitric  acid, permanganate
and  persulfate  at 95°C;  solid  samples
were digested  either  on a steam  bath
with aqua regia and permanganate, or in
an autoclave with sulfuric acid, nitric acid
and  permanganate. All sample  digests
were  diluted  to calibrated  volume  in
100-mL volumetric flasks with deionized
water following the addition  of the
sodium chloride-hydroxylamine  hydro-
chloride  reagent  solution to  reduce
manganese  dioxide  and  excess
permanganate to the soluble divalent
manganese  form.  This  procedure
permitted  sampling  of multiple  aliquots
and  further  dilutions  as needed.  The
sample aliquot added to the  reduction-
aeration vessel was diluted to 100  mL
with Type II water.


Results and Discussion

Phase / - Amalgamation Cell
Testing and Sample
Characterization
    To  minimize variability  in  the
instrumental  responses,  the silver-wool
amalgamation cells were fabricated and
individually  tested  at  Battelle.  The
parameter used to assess uniformity  of
performance  among the amalgamation
cells was  the  slope of  their calibration
curves.  The  slopes  of  four-point
calibration curves for  the first  8 cells
ranged  from  0.0048  to  0.0065
absorbance units/ng of mercury, with an
average  value of  0.0058  ±  0.0006
abs/ng. The  average recovery of a 50-
ng mercury standard, using a calibration
curve with a slope of 0.0052 abs/ng, for
15 additional cells was 98  ± 6 percent,
with  a recovery  range  of 89  to  108
percent.  The  overall  testing  results
indicate uniformity in performance among
the 23 amalgamation cells with respect to
amalgamation  efficiency and  thermal-
desorption   characteristics.  The
differences in  instrument responses for
the different amalgamation cells are
expected  to  be small  compared to the
overall measurement variabilities
between the participating  laboratories.
    Battelle  staff analyzed  NBS-SRM
1633a, with a certified mercury value  of
0.16  ± 0.01 yg/g; the results of duplicate
0.2-g portions  were  0.145 ng/g  and
0.160 ng/g. The recoveries of inorganic
mercury predigestion spikes added to the
fly ash samples were 130  percent  for
duplicate  10-ng mercury spikes,  and
112  percent  and 104 percent  for
duplicate  50-ng  mercury spikes.  In
triplicate  0.2-g  samples of  incinerator
ash analyzed according  to  the  revised
Method 7471, no mercury was detected.
   The average mercury concentration
determined in 8 replicate 0.2-g portions
of the  sewage sludge sample was  1.4
ug/g; the  compiled results ranged from
approximately  1.2 ug/g  to 1.4 ^g/g  of
mercury. These results indicate that the
mercury content of the municipal sewage
sludge is homogeneous to approximately
± 0.1 mg/kg.

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    The average recoveries of duplicate
90-ng  and  180-ng Hg  predigestion
spikes (as methyl mercuric  chloride)
were 75  percent and  90  percent,
respectively, and the average recoveries
of duplicate  100-ng  and 200-ng Hg
predigestion  spikes  (as  inorganic
mercuric chloride) were 108 percent and
106  percent,  respectively. The  overall
recoveries of organic  and  inorganic
mercury added as predigestion  spikes
are within  ± 25 percent of full recovery.
    No  mercury  was  found in  four
replicate  50-mL  test  aliquots  of the
ground-water sample.  The  average
inorganic spike recoveries of four  sample
replicates  were 106 percent for 50-ng
mercury  spikes  and 105 percent for
100-ng mercury  spikes.
Phase II - Preliminary
Laboratory Evaluation
    Method  evaluation  materials  were
sent to 19 laboratories participating in the
preliminary laboratory evaluation phase.
Each package contained: (1)  a tested
silver-wool amalgamation  cell,  (2)  in-
structions  for the  installation and use  of
the amalgamation  cell, (3) two samples
and  appropriate evaluation standard so-
lutions,  (4)  instructions for  the prep-
aration and analysis of the samples, and
(5) instructions for reporting  the ana-
lytical  results  to  Battelle.  One  lab-
oratory  withdrew  at  the  beginning  of
Phase  II  after receiving  the  package,
leaving a total  of  18  participating
laboratories. The two samples shipped to
the participating laboratories consisted of
deionized water  for the  evaluation  of
revised  Method   7470,  and  NBS-SRM
1633a (Coal Fly Ash) for the evaluation of
revised Method 7471.  A spiking solution,
containing mercury at a concentration  of
1.5 mg/L, was included  for spiking the
deionized  water sample. The participants
were instructed to add 50 nL of the 1.5-
mg/L spiking solution (equivalent to 75
ng Hg) to a 20-mL aliquot of  the  water
sample  as a  predigestion  spike.  The
laboratories were also provided a stock
solution  containing  mercury  at  a
concentration of 1000 mg/L to be  used
for  preparing intermediate and  final
calibration standards.
    For sample  analyses,  the  partic-
ipants were instructed to: (1) construct a
4-point  calibration curve comprised of
the  absorbances for  a  reagent blank,
10-ng,  50-ng,  and  100-ng Hg  stan-
dards,  (2) analyze  the spiked  water
sample  according to the revised Method
7470, (3) analyze the coal fly ash sample
according  to  the revised Method 7471,
and (4) prepare and analyze one reagent
blank each for the revised Methods 7470
and 7471.
    The slopes of the calibration curves
generated by  the  18 participating
laboratories for the two revised methods
ranged  from 0.0001   to  0.0056  ab-
sorbance  units/nanogram.  Ten labora-
tories reported slopes between 0.003 and
0.006 absorbance  units/nanogram for at
least one of the revised methods. Battelle
researchers  have  found that this is  a
typical  range for the  slope of  the
calibration curve obtained by using the
amalgamation  CV-AAS  system  ac-
cording to  the  specific  instructions
described  in  revised Methods 7470 and
7471. Ten laboratories reported reagent
blank values  less than 0.03 absorbance
unit. Battelle researchers  have consis-
tently  measured absorbance  values
between 0.02 and 0.03 absorbance units
for reagent blanks analyzed according to
the revised  Methods 7470  and  7471.
Based on  a typical instrument calibration
slope  of 0.005  absorbance units/
nanogram, reagent blank absorbances in
this range correspond to approximately 5
ng  Hg. Reagent  blanks  for aqueous
mercury calibration standards, consisting
only of  the  stannous chloride reductant
and  deionized water,  generally produce
0.001 absorbance  unit; this  is negligible
relative  to the absorbance values for the
reagent  blanks  carried  through th<
digestions.  Some  of  the  apparent lov
reagent blank values  reported  by th<
laboratories may be suppressed in (host
cases  in which  the reported calibratioi
slopes were lower than the typical range
of values.
    Two laboratories  did not  submi
results for  the spiked deionized  wate
sample, and five laboratories did no
report results for the coal fly ash sample
The  results  reported  by one  laboratory
were excluded as obvious outliers. Tht
other  laboratories reported  mercury
concentrations  for the  spiked   wate
sample ranging  from  0.00076 to  0.007^
mg/L,  and  for the coal fly ash sample
from  0.04  to  1.1 mg/kg.  Thus, the
calculated mercury recoveries  for the
water samples ranged  from 20 percent (<
5-fold  negative bias)  to 200  percent  (e
2-fold  positive bias),  and  those for the
coal  fly ash samples  ranged  from  2E
percent (a  4-fold negative bias)  to 69C
percent (a 7-fold positive  bias).
    A summary of the statistics across al!
laboratories  (except the obvious  outlier]
for the mercury  measurements on the
spiked deionized water and coal  fly ash
samples is  presented  in  Table  1. The
means and standard deviations, reporteC
as percent recoveries,  were calculated for
all laboratories and also for  only those
eventually selected for Phase III. After the
outlier  results had been  removed, the
remaining data were smoothly dispersed,
and no additional outliers were obvious.
    The data reported by some of the
participating laboratories  for  these
preliminary  sample  analyses  are  in
appreciable  error. Possible contributing
factors to  the  wide  range  of results,
especially for the coal fly ash  sample,
include high absorbance  values  for  the
reagent blanks  resulting  from sample
digestions, a propagation of errors in the
calculated data submitted to Battelle, and
the general  lack of operator  experience
with  the technique of silver-wool amal-
            Table 1.     Statistical Summary of Mercury Measurements on Spiked Deionized Water and Coal Fly Ash

                                                                     Percent Recoveries
                   Number of Laboratories
           Spiked Deionized Water
     Coal Fly Ash
            All Labs3
                Mean
                Standard Deviation
            Phase III Labs
                Mean
                Standard Deviation
              99
              53


             110
              57
         230

         200


         230

         210
            a Recoveries for the obvious outlier laboratory were not used in the calculations of the means and the standard
             deviations.

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gamation.  Some laboratories  measured
reagent blank values  as high as  0.6
absorbance unit, which is equivalent to
approximately 120 ng of mercury based
on  a  calibration  slope  of  0.005
absorbance  units/ng; such  a reagent
blank value exceeds the linear range of
the  amalgamation CV-AA8  method.
Battelle staff discussed the results with
many of the laboratories; recommen-
dations  for improvements in  controlling
mercury contamination of the reagent
blank  and test sample, as well  as
suggestions  for implementation  of  the
amalgamation CV-AAS system,  were
provided. In general, the high  dispersion
of data between laboratories for  both
samples indicates a lack  of ruggedness
for  the  amalgamation CV-AAS method
in this testing phase of the study.
Phase ///- Interlaboratory
Evaluation
    The  results  of  the preliminary
sample analyses in Phase II were used
as  a qualitative guideline but not  as
absolute criteria for the selection  of  10
laboratories for participation in  Phase III.
    Five laboratories obtained results
which were in close agreement with the
target mercury values for both samples.
Five other laboratories  obtained  less
satisfactory results  but  exhibited suf-
ficient  interest and enthusiasm  in  the
silver-wool amalgamation technique;
these 5 laboratories were judged  to  be
capable participants in Phase III.
    Two different sample  sets, denoted
as Option A and B and  which  comprised
three solid and  three aqueous samples,
were shipped to the participants in Phase
III,  together  with detailed instructions.
Some of the samples required addition of
a predigestion spike.  Option A samples
were supplied in duplicate and Option B
samples in triplicate.  The samples were
shipped  unspiked to  avoid  potential
losses of trace mercury spikes added to
samples with a reducing matrix.  Pre-
digestion  spiking solutions  containing
organic and inorganic mercury were sent
to the  participants  with  spiking  in-
structions. One solid sample in Option B
was also to be spiked  with  copper, a
potential interferent in CV-AAS analyses
for mercury.
    The slopes  of the calibration  curves
reported by the  10  participating lab-
oratories ranged from 0.0010  to  0.0065
absorbance units/nanogram of mercury.
Six of the 10 laboratories reported slopes
within the range experienced by Battelle
staff (0.003 and 0.006 absorbance units/
nanogram). The absorbance values for
the reagent  blanks ranged from  -0.004
to 0.075  absorbance units. Eight of the
10 laboratories reported  reagent  blank
values less  than 0.03  absorbance unit.
Based on a typical calibration slope of
0.005 absorbance  unit/nanogram,  a re-
agent blank value  of 0.03 absorbance
unit  corresponds  to a maximum  con-
centration of 6 ng  Hg  in  the  reagent
blank. In  general, the 10 laboratories in
Phase III  reported a  lower dispersion and
a narrower range of results for calibration
and  reagent blank  data  than  the  18
laboratories  in Phase II. The  10  Phase-
Ill laboratories represent  a more  con-
sistent range  of  personnel  skills  and
demonstrated competence in  trace ana-
lysis. The lower dispersion in the data
may  also  be a direct  result of  the
acquired  experience and  familiarity  with
the silver-wool amalgamation technique
by  the  10 laboratories from  their
participation in the Phase II study.
    The  statistical  summaries of  the
interlaboratory  study  results  are
presented in Tables 2 and  3. The means
and  standard deviations are reported in
concentration  units for those environ-
mental  samples   originally  having
nondetectable endogenous  mercury
concentrations, and in percent recoveries
for  those samples  having detectable
target mercury concentrations. The  per-
cent recoveries are  calculated  as  100
times  the   measured  concentration
divided by the target concentration.
    Outlier  tests  were performed on the
laboratory means for each  option  within
each  sample type.  One laboratory  was
identified as an outlier for most samples,
and  its  results  were  excluded from
statistical treatment for all sample types.
    The  average mercury concentration
or percent recovery over  all laboratories
in a given option is  reported in the third
column of  Tables  2 and  3.  The  fourth
column  contains  the  pooled within-
laboratory  standard deviations  of  the
mercury concentrations  or percent
recoveries.  The within-laboratory  var-
iances are  simply  calculated  as  the
averages of  the   variances for  the
individual laboratories. The  between-
laboratory  standard deviations  of  the
mercury concentrations  or percent
recoveries   are  reported  in the fifth
column.  This statistic characterizes the
variabilities  in  the true  average mercury
concentration or percent recovery values
across the   laboratories. The between-
laboratory   variances  are  calculated
according to the following formula:

            212     2
         S   =-(S_-S  )
            B   n   x    w
where
is  the  variance of the average percent
recoveries for an  individual laboratory, n
is the number of  sample  results used  to
calculate the average percent recovery
for each laboratory, and
                   w
is the within-laboratory variance. If

                    2
                  S_
                    x
is less than
 then
                   w
                    B
is  set  to  zero. The total standard
deviations are  reported  in  the  last
column. The total variance is simply the
sum  of the  within-laboratory and
between-laboratory variances.
    The  high  dispersion  of  the
interlaboratory  data  precludes  any
statistical treatment of the results for the
revised  Methods 7470 and 7471  that  is
more  rigorous  than  the  analyses
conducted and summarized  in Tables 2
and 3, respectively. As shown in Table 2
for  the  revised  Method 7470, the total
standard deviations for Options A  and  B
are similar for each of the 3 test samples.
However, as  shown  in Table 3  for the
revised  Method 7471, neither  option
demonstrates a  consistently lower total
standard deviation for all  samples. For
example, the total standard  deviations of
the results  in Option A are  4-fold  lower
than those in Option  B for the incinerator
fly  ash  and  the  marine  reference
sediment samples.  However,  the total
standard  deviation  in  Option   B is
approximately  2-fold  lower than  that in
Option A for the spiked incinerator fly ash
sample. The total standard  deviations of
the results in  both options are similar for
the unspiked  and  the spiked  municipal
sewage sludge  sample.  The  relative
differences between  the  total standard
deviations in  Options  A and B  by the
revised  Method 7471  for the 5  samples
appear to be random.
    With the  exception of  the  spiked
waste-water sample  in Table 2  and of
the spiked  incinerator  fly-ash sample in
Table 3, the  grand  means using the

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          Table 2.
            Statistical Summary of Mercury Measurements Using Revised Method 7470s
Sample
Samples Having Nondetectable Target Concentrations &
Ground Water
Ground Water
Samples Having Detectable Target Concentrations c
Waste Water, Spiked
Waste Water, Spiked
Dilute Nitric Acid, Spiked
Dilute Nitric Acid, Spiked
Option

A
B

A
B
A
B
Mean

4
6

140
150
82
82
Pooled
Standard
Deviation

1.8
1.5

17
15
27
31
Between
Standard
Deviation

1.4
2.1

45
39
27
17
Total
Standard
Deviation

2.3
2.6

48
42
38
36
         a Results for an outlier laboratory in Option A were not used in the statistical analyses for any sample.
         b Results are in absolute concentration units (ng).
         c Results are in percent recovery.
Table 3.
                     Statistical Summary of Mercury Measurements Using Revised Method
Sample
Samples Having Nondetectable Target Concentrations &
Incinerator Fly Ash
Incinerator Fly Ash
Samples Having Detectable Target Concentrations c
Marine Sediment MESS- 7
Marine Sediment MESS- 7
Incinerator Fly Ash, Spiked
Incinerator Fly Ash, Spiked
Municipal Sewage Sludge
Municipal Sewage Sludge
Municipal Sewage Sludge, Spiked
Municipal Sewage Sludge, Spiked
Option

A
B

A
B
A
B
A
B
A
B
Mean

0.021
0.074

110
110
74
39
90
88
97
90
Pooled
Standard
Deviation

0.0090
0.021

6.5
48
8.6
15
14
20
26
12
Between
Standard
Deviation

0.0076
0.041

10
0
32
11
18
21
25
26
Total
Standard
Deviation

0.012
0.046

12
48
34
19
22
30
36
28
         a Results for an outlier laboratory in Option A were not used in the statistical analyses for any sample.
         b Results are in absolute concentration units (mg/kg).
         c Results are in percent recovery.
revised  Methods  7470  and  7471,
respectively, are  generally  within  25
percent of  the  target values.  However,
the total standard  deviations  for  all
sample types represent relative standard
deviations   as  high  as  50  percent.
Because  of such  highly  dispersed
results, in  addition to the contradictory
results of the copper interference test,
the revised  Methods  7470  and  7471
presently lack the necessary ruggedness
to be successfully used for  routine
testing by analytical laboratories without
additional analyst  training and demon-
stration of proficiency.

Conclusions
    The  results  of this  interlaboratory
study  indicate that only a  few of the
collaborating laboratories  demonstrated
proficiency   in incorporating the silver-
wool  amalgamation apparatus into their
                                CV-AAS  systems within a  relatively
                                short learning period. These laboratories
                                reported  calibration slopes  in  an
                                acceptable  range based on  Battelle's
                                experience  with  the  amalgamation CV-
                                AAS  method.  Only  a few  of the
                                laboratories  were   able to  perform
                                accurate and  precise  measurements on
                                both aqueous  and solid  environmental
                                samples.
                                    A  statistical treatment  of the
                                interlaboratory  results indicates  that the
                                amalgamation  CV-AAS  method  cur-
                                rently lacks sufficient  ruggedness to be
                                successfully  used  by analytical lab-
                                oratories  for routine  testing  but, when
                                properly implemented by proficient lab-
                                oratory personnel, it may serve as an
                                alternative to the recirculating  CV-AAS
                                method described in  the current  EPA
                                protocols of Methods 7470  and 7471.
                                However, to fully realize the analytical
benefits of the  amalgamation CV-A/
method and to  obtain accurate ai
precise data, a complete appreciate
and  awareness of the  critical facto
affecting successful  trace  analyses  a
essential,  and  a  high   level
sophisticated operation and operator si
is  required. Moreover,  because  of  tl
increased  sensitivity of the amalgamate
CV-AAS method, improved  analytic
techniques and  the  use  of  high-puri
reagents are required  to minimize m<
cury contamination that would not be
problem when   using  the recirculati
CV-AAS method with samples of  high
mercury concentrations.
    To achieve  better results, many
the laboratories reported that  they  had
modify the operating parameters  of  t
silver-wool amalgamation  apparat
from those specifically  described  in  t
revised protocols. This may  have be

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necessary  when  the  silver-wool
amalgamation  apparatus was  not as-
sembled  and configured properly ac-
cording to the directions in the protocols,
or when the amalgamation apparatus had
to be  reconfigured to  fit  a specific
commercial or  customized CV-AAS
system.  The different operating  con-
ditions used by some  laboratories may
have contributed to the  high dispersion in
the  amalgamation  CV-AAS   data
submitted to Battelle.
    Most of the comments from the
collaborating laboratories addressed the
increased sensitivity  and  the  longer
analysis time of  the amalgamation CV-
AAS  method.  Many  laboratories
recognized the need for  higher operator
skill and the importance of the need for
high-purity reagents to minimize  mer-
cury contamination.  The benefit  of an
amalgamation CV-AAS method  with
increased sensitivity but  at the expense
of longer analysis time was  challenged
by some laboratories  from  a business
economics viewpoint; the longer analysis
time would  increase  sample analysis
costs to the laboratory that would have to
incur  the additional costs  or charge
higher  analysis  fees to  the customer.
Although the faster recirculating  CV-
AAS method was considered adequate
for the majority of  their  samples,  other
laboratories expressed  special needs for
the increased sensitivity of  the  amal-
gamation   CV-AAS   method  and
indicated  that it  would be  valuable in
research and for  difficult  analysis
problems. Some  laboratories expressed
enthusiasm  about  the  amalgamation
CV-AAS method and indicated that they
plan to incorporate this  method into their
laboratory  operations for   additional
flexibility. The extent of  time and cost
constraints  for  adapting  the  amal-
gamation CV-AAS method to a specific
sample workload  may  be influenced by
whether the  emphasis  of the analytical
laboratory is  on commercial testing or on
research, development  and specialty
problems in a support function of a larger
organization.
    In  conclusion,  it is  recommended
that the CV-AAS methods be used to
characterize  waste samples for mercury
as described below:
(1)  The current  EPA  protocols for the
    recirculating  CV-AAS method
    should be  used for  analyses when
    the threshold concentration value for
    mercury is relatively  high and when
    the samples  do not  contain  volatile
    organic compounds that could cause
    nonspecific absorption interferences.
(2)  The amalgamation CV-AAS method
    should be used for the analyses of
    samples  containing  low mercury
    concentrations which  can not  be
    easily  determined  by the  re-
    circulating CV-AAS method.
(3)  The amalgamation CV-AAS method
    should also be used for the analyses
    of samples  containing  volatile
    organic compounds which will cause
    nonspecific absorption interferences
    and  inaccurate  results  with  the
    recirculating CV-AAS  method.
    Because  of the greater sensitivity
and the more sophisticated apparatus of
the amalgamation  CV-AAS system, it is
emphasized that the laboratory analysts
be  properly   trained  and  that they
demonstrate  proficiency  with  the
amalgamation  method  before initiating
regulatory analyses for mercury.

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  The EPA author, Werner F. Beckert, (also the EPA Project Officer, see below)
       is with the Environmental Monitoring Systems Laboratory, Las Vegas, NV.
       Judy E. Gebhart, Jerry D. Messman, and Gordon F. Wallace are with the
       Battelle Columbus Division, Columbus, OH 43201-2693.
  The complete report, entitled  "Interlaboratory Evaluation of SW-846 Methods
       7470  and 7471 for  the  Determination  of Mercury in  Environmental
       Samples," (Order No.  PB 88-196 001/AS; Cost: $14.95,  subject to
       change) will be available only from:
           National Technical Information Service
           5285 Port Royal Road
           Springfield, VA 22161
           Telephone: 703-487-4650
  The EPA Project Officer can be contacted at:
           Environmental Monitoring Systems Laboratory
           U.S. Environmental Protection Agency
           Las Vegas, NV 89193-3478
United States
Environmental Protection
Agency
Center for Environmental Research
Information
Cincinnati OH 45268
Official Business
Penalty for Private Use $300

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