Final Report: Analysis of Tank 41 H Saltcake Sample 2 and .../67531/metadc...In March 1993, a single 1.5 inch depth saltcake sample was caken from the €3-3 riscr and analyzed[l]

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WS R C-TR-94-0 057

Final Report: Analysis of Tank 41 H Saltcake Sample # 2 and Comparison to Sample #I

by D. T. Hobbs Westinghouse Savannah River Company Savannah River Site Aiken, South Carolina 29808 C. J. Coleman

DOE Contract No. DE-AC09-89SR18035

This paper was prepared in connection with work done under the above contract number with the U. S. Department of Energy. By acceptance of this paper, the publisher and/or recipient acknowledges the U. S. Government's right to retain a nonexclusive, royalty-free license in and to any copyright covering this paper, along with the right to reproduce and to authorize others to reproduce all or part of the copyrighted paper.

DISCLAIMER

This report was prepared as an account of work sponsored by an agency of the United States Government. Neither the United States Government nor any agency thereof, nor any of their employees, makes any warranty, express or implied, or assumes any legal liability or responsibility for the accuracy, completeness, or usefulness of any information, apparatus, product, or process disclosed, or represents that its use would not infringe privately owned rights. Reference herein to any specific commercial product, process, or service by trade name, trademark, manufacturer, or otherwise does not necessarily constitute or imply its endorsement, recommendation, or favoring by the United States Government or any agency thereof. The views and opinions of authors expressed herein do not necessarily state or reflect those of the United States Government or any agency thereof.

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Available to the public from the National Technical Information Service, U. S. Department of Commerce, 5285 Port Royal Road, Springfield, VA 22161.

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DISCLAIMER

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WESTINGHOUSE SAVANNAH RIVER ~ M P A W WSRC-TR-94-MT SAVANNAHRIVERTECHNOUXY CENTER

&yWmds: ffigh-level wade, Criticality, FTP, salt, Plutonium, Uranium, Isotopics, Chemical, Elemental, Radiochemical

January 26,1994 TO: S. D. Fink, 773-A mid+ ea j From: D. T. Hobbs, 773-A and C. J. Coleman. 773-A

Technical Reviewer:

Final Report: Analyds of Tank 41H Saltcake Sample lf2 and Comparison to Sample#10 a

SUMMAlRY

, Three saltcake samples taken from Tank 41H on July 12-13,1993 have been analyzed for chemical and radiochemical content, identification of crystalline phases, and solubility in inhibited water and compared to the results for the d e r sample taken in March 1993. The maximum total h u m content of the as-xtmived samples was determintd to range fmm 3.0 to 7.3 pg/g with 8 maximum uranium-235 enrichment of between 15 and 16% at the 95.2% (20) confidence level, The maximum total plutonium content was determined to range from 0.034 to 0.061 pg/g with a maximum Pu-239 enrichment of between 26 and 32% at the 95.2% (20j confidence levcl.

Based on the ICP/MS data, uranium appears to be distributed unifarmilyradially, but not vertically in the top l2-inch layer of the saltcake. There was approximately a factor of two Werence in the uranium content between the top sample (6.0 crg/g) and the bottom sample (2.7 pg/g). All of the sampks wcne comprised of a xnixtm of light and dark solids. The light- colored solids readily dissolved in inhibited water. Uranium and plutonium were not nnifomrly distributed among the white and dark solids. Less than 5% of the total plutonium, but 6342% of the total &um was determined to be asstx5ate.d with the water-soluble solids fraction of the

Based on the chemical and radiochemical analytical results, the salt solution that will be produced upon dissolution of the saltcake would have the following impacts on ITP messing: (1) the salt solution in Tank 48H will exceed the current process requirement fix insoluble solids content of 400 m&, (2) the removal of Sr-90 wouId not be necessary to meet the xecommendtd Saltstone feed requirements, and (3) the amount of potassium tetraphenylborate precipitate that will be produced in the ITP process will be 10-258 of that based on @e average flowsheet.

samples. L

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WSRC-TR-94-057 -page2 -

January 26.1994

INTRODUCTION

p

Several nuclear safety issues have arisen associated with the dissoIution of sal t presently stored in Tank 41H. Based on estimates of the inventory of plutonium and uranium in the tank, the accumulation of a critical mass of uranium and, to a lesser extent, of plutonium is postulated if the fiiile materials do not completely dissolve. To detedne the total plutonium and uranium content and the isotopics for tach, saltcake samples are being taken from thc tank and analyzed. Other chemical and radiochtmicd analyses are ais0 being carried out to provide data for planning ITP operations with salt solution prepared from tbis saltcake.

In March 1993, a single 1.5 inch depth saltcake sample was caken from the €3-3 riscr and analyzed[l]. In July 1993 three additional saltcake samlplcs were t b ~ t . These samples were taken from the El riser, which is Iocatcd on the oger =de of the center s q q o r t column of the tank from the B-3 riser. Two samples were taken on July 12 and one samplc on July 13. It was estimated that the total depth of saltcake sampled was 12 inches.

EXPERIMENTAL

The handling and analysis of the samples were performed in accordance with the requirements specilicd in the Task and Quality A s m c e Plan[2]. During sampling, the saltcake samples taken from the &I riser were reported to bc much mon fluid than the March sample. me samplc cups had been placed inside plastic sleeves. Sample cap WL had an additional layer of containment as it had been p k c d wirhin a htex glove within the plastic sleeve. The plastic sleeve was opened and thc contents of tach placed onto a stainless steel my. Liquid was ' observed to have Leaked through the plastic slceves into the doorstop for samples #2 and #3.

The total chemical and radiochemical content for each sample was determined by completely dissolving two 2.5 gram sub-samples in 2M nitric acid Approximately 22.5 grams of 2M nitric acid w t n used for cach dissoIution. AU solids wen obsMvcd to dissolve with the evolutiop of gas bubbles. 'Ihe acid solutions were divided into two portions; one portion WBS sent to the Analytical Services Group of SRTC and the other portion sent to the Analytical Laboratories (AL) in 772-F for determination of plutonium and uranium content and isotopics. At SRTC, the plutonium and uranium content and isotopics were determined by inductivcly-coupled plasma mass spectrometry (ICP/MS) and by alpha spcctrorneay (a-PHA). At AL, the uranium and plutonium were chemically separated by iontxchangc chromatography. The plutonium content and isotopics were determined by alpha spectrometry and the uranium content and isotopics determined by themud ionization mass spectrometry mS). After completion of the uranim and plutonium analyses, ?he remaining chemical and radiochemical analyses were performed.

Water solubility tests were c o n d u d in the SRTC shielded cells. Inhibited Ater was pxeparcd by dissolving reagent grade sodium hydroxide in deionized, distilled warn to provide a sodium hydroxide concentration of0.015 molar. The water solubility tests consisted of weighing a , known quantity of the saltcakc sample into a graduated centrifuge tube, adding increasing amounts of inhibited water, and measuring the volume of undissolved solids. After the final inhibited water addition, the sample was centrifuged, and the clear solution femoved from the undissolved solids. The undissolved solids wexe rinsed with two small portions of inhibited water and dried at 100OC. The dried solids were either submitted for x-ray diffraction analysis to identify crystalline phases present or dissolved in 2M nitric acid and analyzed for radiochemical and chemical composition.

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WSRC-"R-94-057 -pagt 3 -

January 26,1994

During the second series of inhibited warn dissolutions, it was determined that not all of the water insoluble solids dissolved in 2M nitric acid. A second dissolution of the remaining solids was d e d out by the addition of 4 mL of aqua regia. Approximately 20% ofthe remaining solids did not dissolve in the aqua regia. The solids nmaining sfter the aqua regia dissolution were dried at 100°C and stored for possible future analysis.

Blanks and standards wcrc also analyzed along with the saltcake samples. Two blank salt solutions were used; one consisted of a simulated salt dissolved in 2M nitric acid, and the second consisted of a simulated salt dissolved in inhibited water. A uranium standard solution was prepand by dissolving asimulated salt containing a hown amount of uranium in 2M nitric acid. The blanks and uranium standard were handled in the shielded cells Using the same procednns as the saltcake sample. This provided a check to dctemine the amount of cross contamination of the samples as a nsult of handling in the shidded cells. The three solutions used in the dissolutions (it., inhibited water, 2M nitric acid solution, and aqua regia solution) wen also analyzed to establish a baseline for the ICP-ES results.

RESULTS AND DISCUSSION . . %of light-colored, crystalIinemlids and dark-colored solids. The appearance and weight of the isolated as-received smplts from each cup arc given in Table I. Included io Table I the data for the March 1993 sample, which is Eferred to as Sample #I-1. Sample #2-1 n f d to the first (top) sample taken in July, #2-2 to the sccond (middle) sample, and #2-3 to the third (bottom) sample.

Based on the weight of sample isolated and the volume of the sample cup, the packed densities of samples #2-1 and #2-3 were determined to be 0.75 and 0.66 g/cd, zespectively. This is considerably lower than that determined for the March 1993 sample (1.9 g/cm3). It was reported that the saltcake taken from the E-1 riser was "slushy", whereas, that from the B-3 riser wqs "hard like concrete"f3J. The ~ Q W packed densities of the July samples m the result of liquid and/or air trapped in the sample cup. The nportad weight p a n t solids for sample -3 is higher than the actual material, because a portion of the liquid was Iost during transport to the shielded c c k No attempt was made to . mover the liquid contents in the sample because of the possible mss-contamimtion of the samples. Apparently, the salt in the vicinity of the E-1 riser has a much higher liquid content than that at the B-3 riser.

Sub-samples of the damp saltcakes were dried to constant weight at 100°C to determine weight percent solids. The dried solids were then analyzed by x-ray diffraction to idintify crystalline phases present. The d t s axe presented in Table TI. Sodium nitrate and sodium carbonate wen the only crystalline phases identified in the as-received samples. These findings were consistent with the results of ion chromatography and IB/ES analyses, which indicated that sodiutn, ' nitrate, and carbonate arc the predominant components of the saltcake (see sections "Elemental and X-Ray Diffraction Analyses of Solids" and "Anion Analyses of Water-Soluble Solids").

The interstitial supematant liquid content of the as-received samples was estimated fipm the weight percent solids analysis. .Assuming the weight loss upon drying to be solely due to water present in the interstitial liquid and that the interstitial liquid has a composition of that

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January 26,1994

determined for a Tank 41H supemate sample taken in October 1992 141, the iuterstitial liquid in the samples was dctMmintd to range from 12 to 24 percent by weight or 17 to 35 percent by volume. The assumption that a l l oftht weight loss is due to interstitial liquid ovenstimam that quantity, since some amount ofwater is associated with the solids as waters ofhydration in the crystalline lattice. For samples #/2-2 and#2-3, the actual liquid content of ?he sample was higher than that npmttd above since some liquid had penetrated the plastic bags smrounding the sampling cups and was present in &e doorstops.

sb Table L Quantity and Appearance of Saltcake SampIes

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e S a m f d AD- #1-1 77270 thin layer of dark colored solids at bottom of

remainderof samplecup sample CUP, light c o l d solids tightly packed in . 3/29/93

7/12/93

7/12/93

7/13/93

#2-1

#2-2

' #2-3

85.169

9.308"

55.835'

mimm of light and dark'colored damp solids packed in sample cup

wet, slushy light and dark solids most of which had leaked fhm sample cup

damp light and dark solids Ioosdy packed in sample cup

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The densities of the as-received saltcake solids were estimated from &e inhibited water dissolution tests. The volumes of the solids and total mixtun were measured immediately after the addition of an aliquot of inhibited water, and before significant dissolution of the saltcake solids. Based on these measurements, the densities of the solids were determined to be 1.4 & 0.1 g/cm3 for sample #2-1 and 1.3 & 0.1 g/m3 for sample #2-3. These densities 81t considerably lower than that determined for the March 1993 sample (1.9 g/cm3). Since, the XRD and chemical analyses of a l l the samples are very similar, the densities of. the samples should be the m e .

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Table IL Weight Percent Solids and X-Ray Diffraction Results Pate S-ID wt % S&!jsl 3/93 #1-1 86.3 f 1.3 NaN03, Na2C03, Na2c03*H20 7/93 #2-1 89.0 f 3.6 'NaNo,, N%C%, N a ~ ~ ~ ~ H ~ O 7/93 #2-2 * nd nd * 7/93 #23 89.2 5 24 NaNo3 ,

uranium and P I u t a Co ntent and htm 'c AbundanR Two sub-samples from each of the three askceived saftcake samples were dissolved in 2M nitric acid and analyzed in duplicate far d u m and plutonium content and isotopics by IB/M!3, TIMS, and a-PHA. The avmgc concentrations determined by ICPM and a-PHA for each mass and the total uranium and plutonium content an pnsentedh Table IlL The isotopic abundances for uranium and plutonium are presented in Table IV. The average total uranium content of the three July samples was determined to be 4.5 f 1.7 pglg, which is very similar to that found fm the March sample (5.7 f 0.44 g/@. The uranium isotopic

samples w m taken from two dif5exent riser on opposite sides of the tank, it appears that the uranium is dis~buttd rmifomniy radially in the top 12 inch layer of the tank. Tht similarity of *the isotopic distribution in all of the samples indicates that the uranium is from the same sottrce.

The relative standard deviation (RSD) ofthe total uranium content f a the individual saltcke samples ranged from about 5% to 10% whereas the RSD for the average of the thee July samples was 37%. At the 952% (2a) confidence level, the total uranium content for samples #2- 1 and #2-2 are not statistically differtnt, but m statistically different from sample #2-3. These results suggest that them is some inhomogeneity in the distribution of the uranium in the 12 inch vertical sampling profile, Based on the July samples, the total uranium content varied by a factor of about two over the 12 inch vertical segment. The average total plutonium content oftbe July samples was determined to be 0.033 0.0081 pg/g, which is about half of that found in the March sample (0.06!5 &0.0098 pglg). The average Pu-238 and Pu-239 abundames WCR determined to be comiderab1y'Mmnt for the March and July samples. However, at the 952% (20) confidence level, thcn was no sta&ticdy significant differences between the March and July samples because of the greater uncertainty in the March

The RSDs of the total plutonium content ranged from about 3% to 23% for the individual samples compared to that of 25% for the average of the three July samples. The high& RSDs for plutonium, compared to the uranium values, were attributed to the lower plutonium concentration and the higher analytical uncertainty for the a-PHA measurement. Because of the

abun.dances for the March and July samples were also very M a r . B incc the March and July

sample ~ S u l t s .

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WSRC-TR-9M57 -page6 -

January 26,1994

similarity in the RSDs for the individual and average samples, it cannot be determined if the was any difftrence in vertical distributionof plutonium. The factor of two difference in the plutonium content between the March and July samples is attributed to the difference in the amount of water-insoluble solids. For both the March and July samples, 95% or more of the total plutonium in the saltcake samples is associated with the insoluble solids Wtion (see section '1Detemhation of Water Soluble and Insoluble Uranium and Plutonium Content"). 'Rtc quantity of insoluble solids in the July samples was about one- half of that found in the March sample. Thus, it follows that the lower plutonium content is due to the lower insoluble solids content in the July samples.

From the ICP/MS data, the average weight ratio of h-239/240 was 4.9 for the thrtc July samples. This is lower than the ratio of 6.9 found for the Match sample. The weight ratio of Pu- 239/240 for heat-source plntoniUm is 7.0 and for wtapons-grade plutonium is 16. The measured weight ratios for the March and July samples were closer to that for heat-source plutonium, which is consistent with H-canyon processing. H-canyon wtt would be the principal contributor to the waste stored in this tank.

Table ITI. Uranium and Plutonium Content I Average Concentration (&g) 1 '

#1-1. #2-1 2 3 Ave.#t2 %= U-233 2.7 f 0.14 E42 2.3 f 0.73 13-02 1.7 i0.79 E42 9.6 f42E-03 1.79.69 EQ2 41 U-234 2.5f0.18E-01 25f038E-01 2.0~0.22E-01 l.lfO.11 E-01 lJf0.69E-01 36 U-235 7.5 f 0.52 Ea1 6.8 1.4 E-01 5 5 f 0.84 E41 3.1 f 0.48 E41 S.lfl.9 E41 37 U-236 ' 28 f 02OE-01 26k 051 E41 21 0.32E-01 1.1 f 0.17 E41 19fo.72E-01 38 U.238 4.4 f 035 Ei-0 4.8 j9.39 E+oo 39k 0.11 E+OO 21 f 0.070 E+oo 3.6i1.3 E M ' 36 Total U 5.7 f 0.44 E40 6.0 & 6 3 M ,4.8 +. 0.25 E+OO 27 f 0.15 &OO 45k1.7 E+OO 38

PU-238 3.8 0.45 E02 2.OkO.13 Eo2 3.3 f 0.69 E42 23 * 0.15 Eo2 Mfi.67 E-02 27 pu-239 23~0.15E-02 5.3 f1.6E-03 7.6.f1.6E-U3 5.1~1.5E-03 6.Ck1.4E-03 23 PU-240 3.3 f 0.45 E-03 1.1 ~ 0 3 0 E-03 1.5 f 0.95 E43 1.0f 0.25 E-03 12f 026 E43 22 h - 2 4 I 6.7 f 1.1 E-04 2.3 f3.3 Eo4 33 24E-04 3.4 f O . 6 0 E44 3.0& 0.61 E44 20 Pu-242 3.7f'l.lE-04 ~ 9 f O A l E 0 4 l.Of0.67E.05 20&1.7E-04 I.lfl.95E-04 87 Total Pu 6.5 f 25 E-02 27 f 0.085E-02 4.2 f 0.97 Eo2 2.9 f 0.27 E42 3.3ko.81 E-02. 25

~ ~ ~ ~ ~ g e c o n c e n t r r t i o n s f a r t h e ~ ~ v ~ ~ r m p l ~ 6 m m ~ ~ ~ o f ~ l o d i ~ ~ a m t d i u o l u t i ~ i n n i e i c . c i d -apt for ttmple Y1-1 for which drrplicrss m e a ~ ~ n a r r s of fwe diffaau diisratutiono w a o performed. h-238 dctcrmind by dphaPHA,dI o~imtoperdetemrincdbyIcpIMs. U-23BalsoincludtpPn-238. Fiomthstlphatpecarrmeayrtrulu,Ls &untof Pu-238isbctwceaOA1A%~woreightof~taealm~rtmaso238. ~ c v ~ r a e l t s s ~ t I l c v r r i a r r e e obsavcdforthedupltcate~ysuofitplicuenrb-umpk+Imd~~thecosrypolldingU-~vllutsh.vemtbecn cone#ed Average #2 quais the average of rrtmples #2-1. #2-2, d a - 3 . %I RSD equaLs the smdard deviation diviabd by the

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WSRC-TR-94-057 -page 7 -

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Table IV, Uranium and Plutonium Isotopic Abundances

AilmmWal #GI 1 m-2 #a-3 Ave.#2 %=

u-233 0.48f0.17 037f0.08 035k0.15 036&0J4 , 0.37~0.020 55

U-235 13 f 1.8 11 f1.1 11 fl2 11 f12 11 *O.O 0 U-236 5.0 )rO.O71 43 f0.41 43 f0.43 43 f0.40 43 A0.0 0 U-238 77 k032 80 k1.8 80 f20 80 f19 80 fO.0 0

U-234 4 3 f0.064 4.1 f031 4.1 i0.25 4 2 k0.18 4.1 ~ 0 . 0 5 8 ' 1 A 5)

pu-238 58 f23 75 *5b 78 f24 nka.7 : nf1.s 2.0 Pu-239 35 f14 20 f6.1 18 f5.7 17 f4.4 18 f 15 83 Pu-240 5.1 i2.1 4.1 k1.1 3.6 f2.4 3.5 f0.89 3.7 f 0.32 8.6 pu-m 1 1.0 f 0.43 0.87 f 1.2 0.78 &OS9 13 & O B 095&0.!22 . 23 Pu-242 057 f 039 0.45 f 0.16 0.025 f 0.017 0.69 f 058 0.39f: 0.34 87

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The TIMS method analytical results for the uranium content and isotopics are presented in Table V. The average total uranium content as determined by the TIMS method for the tlkee samples taken in July 1993 (1.3 p&) is approximately a factor of three lower than that deterrpined by ICP/MS (4.5 pdg). This is in contrast to thc March 1993 sample, where the Tuls nsult was slightly higher than the ICP/MS result. The variance in the TIMS results suggests that the d u m may not be distributed uniformily radially, which is in contrast to the conclusion suggested by the ICP/MS &ts.

At the 95.2% (2a) confidence level, the total minium contents for &e three July samples as dctennined by TIMS were not statistically different. The RSDs for the individual total uraniufn contents of the four samples w m equal to or greater than the RSD detcrmincti for the average of the three 3uly samples. Fmm the TIMS results, there was no evidence for a non-uniform distribution of uranium in the vertical sampling pf i le . The greater variation in the TIMS method results compared to the ICP/MS method is attributed to the additional sample preparation

, steps required for the separation of uranium prior to the TIMS &tamination.

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January 26,1994

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A synthetic saltcake material containing d u m of known content (2.46 pg/g) was analyzed at the same tirne as the other samples as a uality assurance check. The total uranium

TIMS method. The slightly higherresult by the IB/MS methodmay be indicative of a small bias of between 4 and 8 percent for this method. For the TIMS method, the bias was 13% which is higher than that for the ICP/W method. Based on the results of the d m standard * material, it is concluded that the uranium results for the Tank 41H saltcake arc valid for both methods. For nuclear safety assessments, i t is nxommwrdcd that the higher ICPNS result be used since this would conservatively ovtrtStimatt the total amount of fissile d u r n in the saltcake.

concentration determined by the ICF'/M 3 method was 2.62 f 0.0497 Wg and 2.78 p/g by the

TabIe V. Thermal Ionization Mass Specbr.ometrk Results for Uranium Content and Isotopic Abundances

Concentration @g/g) , #1-1 .m-1 AveM %68sp

Total U (TIMS) 7.8f 1.8 15 f 0.74 1.4 f 0.42 l.O* 024 1.3k0.25 19 Total U (ICP/MS) 5.7 f 0.44 6.0 f 0.63 4.8*025 2.7 f 0.25 45f1.7 38

*

Abundance (%) #1-1 82-1 ##2-2 3

U-234 3~ koa7 z.7i 0.18 2.2+0.@ 23i1.5 2 4 ~ 0 % 11 u-235 7.9 flfi 7.6 f 27 63f 1.8 6.4 f 3.9 6.8f0.72 11 U-236 3.4 kO.60 3.0k0.086 23f0.70 2.4 f 1.6 2.a0.38 15 u-238 85 f2.8 87 k3.6 . 89 f3.1 89 f7.0 88k12 9.4

,

Other Actinidm The ICP/MS data included masses 237,243 and 244. Tbtsc masses should be primarily due to neptunium-237, americium-243 and curium-244. The analytical results for these actinides are presented in Table VI. After comcting for the salt blank, the amounts of mqricium-243 and curium-244 were very low. The low americium and curium content was also confirmed by yPHA and a-P€iA analyses.

The americium-241 content of the watm-soluble solids fraction of sample #2-lwas g.0 E-04 ' pg/g and ~4.8E-02 for sample #2-3. The dum-244 content of the water-soluble fraction of sample #2-1 was 3.2 f 2.8 E-05 p@g and c6.2E-06 pg/g for sample #23. The= was no detectable americium-243 or curium-244 in the ICPW analyses of the #2-1 or #2-3 insoluble solids fractions. Based on the analysis of the water soluble and insoluble fractions, all of the dum-244 appears to be water solubIe. In contrast, most or al l of the neptunium-237 appeared to be associated with the insoluble solids fraction. This was unexpected since nepainium is

WSRC-TR-94457 -page 9 -

Janumy26,1994

reported to have an equal or greater solubility than Uranium in alkaline salt salutions[5J. A possible explanation of the low solution concentration is that the nqttlnium is adsorbed by the insoluble solids.

TabIe VI. I C P M Results for Other Actinides Concentration Wg)1

#Ill #&I m-2 WL-3 Neptunium-237 0.163 f O.OOp3 0.058 2 0.013 0.14 f 0.023 0.065 0.010

AmenCi~m-243 5& 13 E-OS 3-32 3.1 E-05 1.9 f 2.6 E44 12k 1.OE-o.4

Curium-244 3.2~ 3.2 E-05 9.7 f 9.1 E* 32& 3.4 E-05 2.4 f 0.32 E-04

l Average amcentrrtions for the as-received Ssmple from dupliwts ICPMS ntwmements of two different dissolutions m N d c acidexapt f o l r a m p l a # l - l f o r w h i c h ~ ~ m ~ o f f i v a d i f f e r r a r d i s s o h r t i D n s waepafamcd. . Dark solids were observed in all thnt of the July samples as well as the earlier March sample. As found in the March sample, these solids do not dissolve in inhibited water. The quantity of insoluble SOW was determined for cach sample and is presented in Table VII, The amount of dark solids in the July samples was about half of that found in the March sample. Two separate inhibited water dissolutions weie carried out for sampIes a-1 and #2-3. Because of the limited quantity of the #2-2 sample, no inhibited water dissolutions wen conducted with this sample.

The darlcalored, water-insoluble soIids settled rapidly from the salt solutions produced ly+ dissolving the saltcake samples in inhibited water. Within 60 minutes, the majority of the solids had scttlcd to the bottom of the container. After standing overnight, alI of the solids had settled to the bottom of the container producing a clear solution with no suspended solids. One of the two dried samples for each of the first set of dissolutions was submitted for XRD analysis. The crystalline phases identified in these two sampIes are reported in Table VII. Sodium nitrate was found in all the samplcs andyzd by XRD. The other crystalline phases found included sodium aluminum silicate, zinc sodium phosphate, sodium fiuomphospbate, and zinc sodium silicate. Thc composition of the dark solids is not identical for a l l samplcs indicating some degree of heterogeneity for the insolnble solids among the pial and 12inch vcrticalpmfiles.

The sccond sample from the first dissolution set and both samples from the second dissolution set wcm dissolved in 2M nitric acid fm chemical and racIiochcmical analysis. The nitric acid' dissolution of the first set was canid out in the Shielded Cells and the second set in l a b o m module B-126/130 of 773-A. All of the dark solids appeared to dissolve for the first set in the Shielded Cells. In the dissolutions canid out in €3-1242130, not all of the soIids dissolved., After contacting with nitric acid, the nmaining undissolved sorids were light tan in color. Because of the small quantity of matend and the poorer visibility in the Shielded Cells the light colored solids may also have been p e n t , but not identified in the fmt dissolution tests.

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January 26,1994

After contacting with nitric acid, the undissolved solids were trtaEed with aqua regin (3HCvHNo3). Some but not all of the remaining solids dissolved in the aqua regia. It is estimated that about 515% of the water insoIuble solids did not dissolve in the nitric acid or the aqua regia. Based on the low solubility in nitric acid and aqua regia, these solids may be silica and/or aluminosilicates. These dais areknown to have low solubility in these acids.

The distribution of the watcr-insoluble solids in saxnple #2-1 docs not appear to bc uniform based on the large difference in the quantity of insoluble solids between the two separate dissolution sets. From the first dissolution set, the quantity of insoluble solids was determined to be 0.89 2 0.11 wt %, and from the second dissolution set, the quantity was 0.13 f 0.0064 wt 45. For sample #2-3, the variation between dissolution sets was much smaller, perhaps indicating a more a uniform distribution. I Upon dissolution of the Tank 41H saltcake for processing in Tank 48H, there will be insoluble solids. Based on the soluble sodium concentration and tht insoluble solids content dettrmined for the Match and July samples, the concentration of insoluble solids in'the redissolved salt solution is calculated to range from 580 to 7900 mg/L at a sodium ion concentration of 5.2M Process requirements for ITP cuncnffy Iimit the insoluble solids content to 400 mg./L[q. Thus, the insoluble solids content in the redissolved salt solution may exceed the current limit. D e insoluble solids limit is provided to minimbe possible impacts on filter performance by insoluble solids other than monosodium titanate and tettaphenylborate salts. Removal of the insoluble solids from the redissolved salt solution may be nqnircd to prevent any impact on the perfonnance of the ITP filters.

,

Table ML Solids Content and Crystalline Phases of the Dark Solids

l imrMR Wt % Solids

I

W e t 1 PrvB-2 - D Resultq 1.7 f 0.026 2.0 3- 0.026 Na&&%6O&(N03)2.4H20 #I-1

NflOs, ZU2NaP,O16*9HzO

#2-1 Diss. #1 0.90fO.11 1.0 f 0.12 NaNo3

Nag (A16Si6024) (S,O3)=SH,O Diss. #Q . 0.13 fr 0.0064 0.15 f 0.0096 Average 0.52 f 0.54 0.58 & 0.60

a - 3 Diss. #I ' 0.68 2 033 0.76 f 0.26 NaNO3 I

N ~ F ( P ~ ~ ~ - I ~ H ~ o , ~ a z z n ~ i 0 4 Diss. #2 0.84 & 0.054 0.94 & 0.065 Average 0.76 f 0.1 1 0.85 4 0.13

..

WSRC-TR-94-OS7 -page11 -

Januq 26,1994

e

of W-ble U- The uranium and plutonium content of the M e r soluble and insoluble solids is given in Table Vm. Fhm the ICP/MS data, there was no detectable plutunium in the soluble .fraction of the July samples, indicating all of the plutonium was associaad with the insoluble solids. Alpha- PHA spectrometry indicated that the soluble solids did have a smalI amount of plutonium activity. It is ts~matcd that no more than 5% ofthe total plutonium present samples was associated with or rcmaincd in the dissolved salt solution. The percent of the total uranium and plutonium in the water-soluble and water-insoluble fhctions as well as mass ba?ances for plutonium and d u m an provided in Table E. %st results were consistent with March sample which found that 4.7% of the plutonium and 89% of the uranium are pnsent in the water soluble crystalline solids. Although the percent soluble uranium for sample #2-3 (64%) was lower than that for samples #1-1 and #2-1, it was not statistidy different because of the higher analytical uncertainty.

Comparing the measured total d u m and plutoniumcontent for the sa i tcak t sample to that based on the analysis of the two fractions indicattd a fairly goodmass balance for plutonium and uranium. The calculated range of total &wn and plutonium conccntmtions for samples #2-1 and #2-3, calculated as the sum of the soluble and insoluble solids concentrations, wcm all within the 95.2% Qa) confidence interval determined fiom the total sample dissolutions in nitric acid. There was no detectable uranium and plutonium in any of the aqua regia dissolutions. This confiied that the alI of the uranium andplutonium in saltcake samples was measured upon dissolution of the samples in 2M nitric acid.

the July saltcake

I

,

. -. a: . * - . . :. .. . . . . , . . ~ . . . .:. ..: L . . .... . . - . .

WSRC-TR-94057 -page 12 -

January 26,1994

I

Table Vm, Uranium and Plutonium Content and Isotopic Abundances of Soluble and Insoluble SoEds1

SampIe #2-l Soluble Solids2 Insoluble Solids? -

0 234 0 235 0.36 10.013 236 0.063 2 0.0017 238 3.3 f: 0.048 TotaI U 3.7 f 0.060

% d l s4hundanr;e 0 2.3 f 0.89 0.36 & 0.18 0 4.1 4 1.8

9.7 * 0.20 11 k.5.2 1.7 k 0.074 4.2 f 1.9 89 + 0.13 81 +37 100- 100-

238 239 240 241

' 242 Total Pu

Sample #2-3 Soluble Solids2

8.8 f 0.82 2.6 i- 0.12 0.31 i: 0.097 0.057 f 0.654 0.46f0.44

0 0 11.8 f 1.1 100

75 fr 9.9 22 f 2.3 2.6 2 0.85

Insoluble Solids3 c PI 96-

233 0 0 . o w 2 1 0.36 & 0.022 ---- - 234 0 0 3.9 k 0.033 235 0.10 fi 0,019 7 2 2 0.32 11 f: 0.(196

Total U 1.4 f 0.32 98 f: 1.4.-

236 0 0 3.9 f 0.046 238 1.3 f 0.31 7 9 k 1 2

238 239 240 241 0 242 0 TotalPu 0

0 0 0

2.7 k 0.42 0 . 6 6 ~ 0.038 0.080 f 0.046 0.018 0 3.46 f: 0.50

4.0 ~3.066 11 f 0.18 4 n + n n 7 ~

,78217 . 19 ~3.0 2.3 + 0.59 0.5F 0 loo .

. ...


January 26,1994

Table M.

Soluble U Insoluble U Soluble Pu Insoluble Pu

Uranium and Plutonium Concentration in SoIuble and Insoluble SoIids, Mass Balance and Percent oFTotal Content

Concentration and % of Totai #2-1

3.7k0.060 82k2 620it200 18k0.43 0 0 11.8f 1.1 loo

#Id

4.6& 0.05 89 32.8 f 0.9 11 1.24 tf: 024E-3 4.7 1.45 f 0.04 , 95

w 5zf.ma w23

1Ak032 63k20 98f1.4 37&12 0 0 3.46k0.50 100

#l-1 w'

Calc. Avc. U 5.164 0.4 Meas. Ave. U Calc. 2 c m g e - 5.1-5.2

5.66 4 0.28

Meas. 20 Range Calc. Ave.Pu &feas. AVG. Pu Calc. 2c Range Meas. 20 Range

5.1-6.2 0.026 f 0.0026 0.027 f 0.0016 0.021-0.031 0.024-0.03 1

Mass Balance #2-1 JSk

4.5 & 0.090 6.0 f 0.63 4.3-4.7 4.7-7.3 0.016 f 0.0014 0.027 2 0.0085 0.013-0.019 0.010-0.044

#2-3 Udg

2.2 f 0.50 . 2.7 & 0.15 1.2-32 2.4-3.0 0.029 & 0.0042 0.029 5 0.0027 0.02 1-0.037 0.024-0.034

m n t a l and X-rav Diffraction An*ses of Soli& The elemental compositions of &e as-received samples, the water-soluble fractions, and the water-insoluble fractions were determined by ICP-ES and atomic absorption spectroscopic (Ah) analytical methods. The xedts for the March sample and the three July samples are presented in Appendices 1-4.

The predominant elements found in the as-received samples included Na, P and Al, with smaller amounts of 251, Cr, and IC The results for each of these elements fur the March and Yuly samples am presented in Table X Far the as-received samples, three solid phases wcrc identified from

. . . .-* . .

... - . .

d

WSRGTR-94-057. -page 14 -

January 26,1994

the XRD patterns: sodium nitrate WaN031, sodium c h n a t e [Na2CQ] and hydrated sodium carbonate [NazC03~x€€~O]. The identification of these salts was consistent with the chemical analysis that found sodium, nitrate and cadxmate comprised h o s t 80 wt % of the as-received samples. . The potassiurn:sodium (ENa) weight ratio in the soluble fraction of the saltcake sample was determined to be 0.0013 for sample #1-l,O.O0052 for sample #2-1, and 0.00074 for sample #2-3. Thus, concentrated salt solutions prepared having these KNa ratios would have a potassium concentrations of 0.0048M(#1-1), 0.0019M(#2-1), and 0.0023M(##2-3) at a Na+ concentration of 6.3M. These potassium concentrations range h a factor of 3.8 to 9.5 lower than that reported for average concentrated salt solution[7J. Consequently, much less pomssium tctraphenylbmte precipitate (-lO-ZS%) would be produced from salt solution resulting from the dissolution of Tank 41H saltcake having the RNa ratios measured m these samples.

The wam-insoluble solids wcrt found to contain Na, Zn, Cr, P, Al, Fe, Ca, and Si The concentration of the predominant elements an presented in Table XI. These mlts were consistent with x-ray diffraction results that indicated the presence of a number of crystalline phases including sodium aluminum silicate, sodium zinc phosphate, sodium flumphosphate, and sodium zinc siIicate. chromium, iron, and calcium apparently w m present as amorphous solids.

Table X Major Elemental Concentrations Found in Total Sample . Weight %a

Na 28.0f0.57 27.9f 1.6 26.6 f 0.80 273 f 038 273 f 0.S 2A 02ifo.ai6 0.1ifo.m o ~ s ~ 0 . 0 ~ 8 o . i o ~ 0 . 0 ~ 8 o.15~0.084 56 -- AI

P 0.41 f 0.040 037 f 0.090 0.43 f 0.16 033 f 0.060 038 f 0.050 13 zn 0.059 f 0.015 Oil14 f 0.0023 021 f 0.064 0.069 & 0.031 0.098 f 0.10 . 100 cr 0.058 f 0.0036 0.092 & 0.021 0.079i 0.022 0.058 f 0.014 0.076 & 0.017 22 K 0.032~0.0001 0.019~0.oM4 O.Mlf0.0074 0.024~0.0028 0.025&0.006 24

/

. . . -....>..*., .?.".. . .. 1 . . . ..: .... : .. .

. . :. .

-page 15 - January 26,1994

Table XI. Major Elemental Concentrations Found in Water-Solubb Solids

Weight %a t #I-1 1 #2-2 m-3 Ave.#2

Na 258 27.0~ 12 nd 27.1 f 1.2 27.1 f 0.071 0.26 Al 0.21 0.093~0.W50 nd 0.095 2 0.057 0.094 f 0.0014 15 P 037. 034 f 0.0024 nd 025 & 0.073 030 & 0.064 22 zn 0.040 0.ocn1*0.0011 nd 0.026k 0.030 0.014 f. 0.017 120

0.0088 0.021 f 0.0032 nd 0.0068 &O.aOlO 0.014;tOBlO 72

25 cr K 0.034 0.014 f 0.0043 nd 0.020 f 0.00I 1 0.017 f O M 2

Table XIL Hemental Composition of Insoluble Sofids Fraction

Weight %a #bl 1 la-2 Ave.#Z a m

Na 85 232f 0.12 nd 239&025 236i 0.49 21

P 0.90 0.92 f 0.028 mi 7.0 f 0.12 4.0 f 43 110 zn 2.a 12f 0.011 nd . 33k0.054 2.2~ 1.4 '64 cr 2.4 5.7 f 0.051 nd 3.9 f 0.081 48* 1.3 . 2 7 ca 0.40 28-* 0.050 ad 23f Oa36 25 f 0.42 17

0.011 0.039&0.00046 nd 0,033 f 0.ooMCs 0.036 f 0.0042 I2 MI3 Fc 055 23 f 0.020 nd 7a 0.12 4.7 f 33 70 Si 024 026io.060 nd 020 f 0.055 - 0.23 f 0.042 18

AI 0.62 0.66 f 0.015 nd 0.48 f: 0.016 _. 0.57 f 0.13 i3

I

I

. . . .. . . .., . .. . . . '.. .'I . . .

. .. . .

WSRC-TR-94-os7 -page 16 -

January 26,1994

of Wa- The solutions obtained from the inhibited water dissolution of the saltcake sample were analyzed by ion chromatography and gravimetric metfiods to determine anion content. The d t s are shown in Table XIII . Niaate and carbonate were the major anions in the saltcake sample. These results were consistent with the XRD analysis that identified sodium nitrate and sodium carbonate crystalline phases in the dried saltcake sampk. The concentrations of the other anions were consistent with previous reports which have estimated the composition of high-level waste [8,9]. The higher mhna te concentration reflects the absorption of atmosphcric carbon dioxide and reaction with hydroxide to form carbonate in the aged waste.

Table XIIL

Anion #Ll #2-1 wt-3 Ave.#t a= Fret OH- 2.0 f 0.16 1.0 f O.Oo90 15 * 0.0061 33 f 0.35 27

Anion Analytical Results for Water-Soluble S,oIids Concentration (wt %)a

AKom4- 1.0 f 0.15 0.22 f 0.012 0.70~ 0.17 0.46 f 034 74 cop 113fO.60 6.5 f 0.79 4.7 f os2 5.6 f 13 23 N03- 40.6 f 1.6 44.1 f 15 463 f O.OOO34 453- 1.6 3.4 NOz- 0.98 f 6.048 O S 0 f 0.0089 0.80 f: 0.026 0.65 f 021 32 Pod3- 0.71 f 0.20 0.98( k0.11 054 f 0.043 0.76 f 0.3 1 41

czo42- 0.17f 0.016 c0.07q f 0.0040 4.077 f 0.0010

3


January 26,1994

Table XIV. Comparison of Analytical Results for Aluminum and Phosphokus

Conoentmion (wt 56). d #lo1 1 #2-Q

Al(OH)4- Oravimtnic 1.0 f 0.15 0.22 f 0.01 0.70 5 0.17 Al ICP-Es 0.21b 0.093 f0.005 0.095 f 0.06 Po43' IC 0.72 f 0.20 0.98 f 0.11 054 0.043 P 0.37b

The total cation, total anion, and insoluble solids cantents for each sample were summtd to determine a total solids content for the as-received samples (see Table nt). The CaICulatEd total solids content was then compared to that deermined by dqying the as-received sample at iOO°C. Fairly good agreement between the two totals was obtained for each of the samples. This indicated that the overall elemental and chemical analysts of the samples were consistent and that no major component(s) had not been identified

The total equivalents far cations and anions were calculated for each sample. Both should be the same to maintain an overall neutral charge. For sample #1-1, excellent agreement in the cation and anion equivalents was observtd. For samples #2-1 and ##2-3, the agreement was not as good, and suggested that not all of the anionic species had been accounted for in the chemical analyses. The unaccounted anionic species may be carbonate. For samples #2-E andrn-3, the C&OM~C content was about half of that found in sample #1-1. All other anionic species were similar for each of the samplcs.

I

. . . . .. ~

. * '. 1

..

-page 18 - January 26,1994

I

Tqble XV. Saltcake Solids Mass and Charge Balance

Concentration (wt %)a #Ll 1

Total Cation 28.0 & 0.6 27.9 & 1.6 27.3 f 0.4 Total Anion 58.0 f 3.0 53.3 f 2.4 55.2 f 1.3

, Insoluble Solids 1.7 f 0.03 0.89f: 0.11 o.n rt 0.15 CalcuIatedTotal Solids Contcntb 87.7 32 82.1 f 4.1 83.3 f 1.9 Measured Total Solids Content 86.3 4 1.3 89.0 3s 3.6 89.2 f 2.4

Total Cation EquivalentsC Total Anion Equivalentsd

Concenfration (molellW g saltcake) 1.22 1.21 1119 1.23 1.03 * 1.05

-*

-and the wattr soluble solids w m analyzed far radiochemical content. The results are given in Table XVI. Radionuclides detected included Cs-137, Q-134, Sr-90, Tc-99, and Sn-126. Cesium-137 was the predominant radioactive matuial found in all of the samples.

The concentration of Sr-90 was fairly low, most of which was not soluble in inhibited water. Because of the low concentration, removal of Sr-90 would not be necessary to meet the recormntndcd saltstone feed requirements[lO]. The Tc-99 rcs:sults for the total sample and soluble solids w m not consistent for the March sample (#l-1). Mare Tc-99 was found in the water-soluble solids than would be predicted based on that mtasuIcd for the total sample. The Tc-99 content was not dctcrminedfor the as-received saltcake for the July samples. However, based on the results for both the March and July samples, salt solutions prepared from the dissolution of the water-soluble solids would meet the Tc-99 limit for %Area salt solution feeb specifications.

I

- . . . . . . . ' 8 -

J


January 26,1994

Table XVI. Radiochemical Analytical Results

Concentration of As-Received Saltcake Sample(pCi/gp e #I-1 M.1 m 2 3

CS- 137 108 f 4 65 & 14 175 f: I1 40&2 CS-134 0.1 1 f 0.01 0.047b 0.16 0.02 0.042 & 0.015 Sr-90 ' 0.012f0.001 nd nd 'nd TC-99 0.013 -i- 0.001 nd nd nd Ru-106 4.057 nd nd nd Eu- 154 4.22 nd nd nd Eu-155 4.22 ' nd nd nd Sn-126 4.18 nd hd nd

Concentration of Water-SdubIe Solids (pCi/g)* de #lo1 I 2

CS-137 1062 3 634. 0.3 nd X15&27 cs-134 0.1 1 f 0.01 osob nd -0.16b Sr-90 0.0034 f 0.0002 ,

WSRC-TR-94-057 - page 20 - January26,1994

I

QUALWY ASSURANCE

The handling and analysis ofthe samples wmptrfbrmcdin accordance with the requirements specified in the Task and Quality Assurance Pfan[2]. Based on the results obtained from the earlier March sample, the number of replicate dissoIutions was decrcasbd from five to two. Two synthetic saltcake materials containing no added uranium and a known quantity.of uranium were rncasurcd along with the unknown saltcake samples. Based on the mults of the uranium saltcake standard material, it is concluded that the uraniumresults for the Tank 41H saltcake ate valid by both the IB/MS and TlMs methods. The thnx solutions used in the dissolutions were also analyzed to establish a baseline for the ICP-ES results. AU laboratory data are recorded in laboratory notebooks, WSRC-Ni3-93-175 and WSRC-NB-93-339 maintained by D. T. Hobbs.

REFERENCES

1. D. T. Hobbs, C J. Coleman, and R N. Mahannah, 'Final Report: Analysis of the Tank 41H

2. D. T. Hobbs, "Task and Quality Assurance Plan for the kalysis of Tank 4lH Saltcake Samples 0," WSRC-RP-93-495, EV. 0, March 28,1993.

3. P. L. Gray, presentation at the POW Meeting, July 16,1993.

4. Memorandum from J. A. Pike to B. L. Lewis, ctal, "Tank Chemistry Report, November 1992 o", WER-HLE-921380, December 17,1992.

Saltcake Sample #1," WSRC-TR-93-377, August 20,1993.

s

5. G. A. Bumey andR M. Harbour, "Radiochemistry of Neptunium," National Academy of Sciences Report, NAS-NS-3060, Published by the Technical Inf'on Center, Office of Infomation S d c e s , United States Ammic Energy Commission, IssuedDecember; 1974.

6. "Process Requirements for the In-Tank Precipitation Process," WSRC-IM-91-63, Rev. b, September 21,1992.

7. D. D. Walker and B. A. Hamm, "Matexial Balance and Planned Operating Schedule for the In-Tank PmcessO," WSRC-RP-89-1303, December 27,1989.

8. J. R Fowler, "Composition of F Ana Soluble High-Level Waste," DPST-8WL-390, March IO, 1982.

9. J. R Fowler, "Cobposition of H Area F d SRP Soluble High-Level Waste," DPST-82-502, April 28,1982. ,

10. C. A. Langton and E. L. Willritc, "Recommended Saltstone Feed Specifications for ZArea,"

.

DPST-88372, March 15,1988. I

.. . i

. . . . . .. ;.: . . . - . :;. . . .. ' :. *. .

WSRC-TR-94-O57 -page 21 -

Janua1y26,1994

Appendix 1 Elerriental Composition of Sample #l-1

TotalGb Total insoluble^ Solublehc iwt %I iwt %I (wt %I

1.9 E-04 85 4.6E-03 e65 E-05

' 1.19E-03 53.8 3.18E-03 l.24E-03 tA As 3.67E-04 12.7 4.91E-03 856E-04 Ag

Se ca ai co cu Mg Mn Pb zn 23. Al Ba Fe La Li Mo Na Ni

. Sn Sr Ti V B cr P Si K HJ3 U Pu

23.E43 4.9 E45 1.65E-04 3.22E-04 2 3 E-04 6.28- 205E-03 5.94E-02 4.2 E-04 2.12E-01 3.01E-04 9.34503 2.8 E-04 UE-04 9.76Ei-04 28OE+O1 4.ooE-04 8.63E-04 5.15E-05 1.61E-04 4.86E-04 1.27E-03 5.84E-02 4.13E-01 4.52E-03 3.20E-02 1.04E-04 5.66E-04 z73E-06

I

69 75 120. 55.3 52 10.3 . 48.8 24.8 76

41.0 25.0 , . 77 79

7.44 ,

5.82 2.04 67.6 25.9 67.5 90.1 28.1 39.4

4.0 E41 5.0 E43 1.4 E63 1.63502 1.1 E-02 3,503-02- -. 6.28E-02 . 2.83EtOO 3.1 E43

7-163.03 5.52E.01 9.7 E04 1.02E-03 1.04~3 8.5OE+OO 1.67E-02 2.343-03 6.72E-04

621E-01

1.34E-03 .. 2.13E-03 4.7 E-03

6.21 2.43E.too 9.61 8.99EO1

23.7 2.36E-01 3.03 1.50E-02 27.2 4.87W 7.71 3.21E03 6.73 1.45E-04

a Wt % of r ~ k . Avaage of five dissolotbnr. Average of two sepxlte diswhtions.

12 E-04 ~4.1 E65 4.7 E-04


January 26, 1993

Appendix 2 Elementat Composition of Sample #2-1

Total SampleEl] Water Soluble Fractionlll Water Insoluble Fractioa[2]

Average Std. Ifev.[3] Average Ski. DevJ31 Average Std. Dev.[33 W L % Element Wt.96 Wt% Wt.% Wt.% . WL%

Ag As SC ca Cd co cu

Mn Pb zn zr Al Ba

. Fe La LI Mo

. Na Ni Sn Sr Ti V B a

- P Si K Hg U Pu

Ml?

r

c 1.75E-04 c 1.7SEo3

3 . m 3 2.65E-05 855E-05 1.28E-04 1.74E-M 2A3E-04 639304 1.42E-M 8.92w)5 l.ME-01 1 .ooW 3.12E-M

. 2.62E-w 3.93E-05 539E.04

‘ 279E+O1 1.95E-04 1.30E-03 1.62E-M

4.22E-W 4j7E-w 9.19E-02 3.74E.41 12fE.03 191M2 2.91W 6.0E-04

- 2 . m

m

453E-M

< 635307 e 635306

121Ml3 8.54E.W 3.89E-05 4.09E-05 1.15E-04 1ZE-04 1.01E-06 232E-03 196E-05 2.02E-02 2.27E-05 2.59E-02 6.1ZE-05 15E-05 1.14E-04 156E+OO 5.19505 6.64E-04 6.09E-06 1.83wH 1.75304 1 .oOw 2.13E-02 8.97E-02 4.81E-04 2.41E-03 3.7lE-06 6.3E-05 8.5E-08

1.68E-04 < 1.68E-03

2 . m 8.49E-04

c 8.4oE-05 < 3 x 4 4 < 8AOEM

22.3E-05 e 252E-05 c 1.6XE-03

2.08E-03 c 1.68E-04

9.27E-02 < 3.36E-05

4.48E-04 < 252E-04 c 6.72EM c 336E-04

270EM1 c 4 2 0 W

1.22E43 c 1.68E-05 C 8AOE-05 e 8.40E.05 567E-04 2.13E-02 3398-01

c 5.65E-04 1.37E-02

< 7.60E-06 3.7E-w nr

e 1.93E-M < 1.93E-04 554E-W 525E-04

< 9.66Eo6 3.86E-05

< 9.66E.06 138E.05

< 2.90E.06 < 1.93E-04

l.lzE-03 e 1.93E-05

5.02E-03 c 3.86E-M

c 2.90E-05 c 7.73E.06 < 3.86E-M

123E+OO c 4.83305

3.62Ei-04 e 193E-06 < 9.66E-06 < 956E-06

3aEm 237502 -

4.2!)E-o3 < 3.9x-07 6.0E-06

. . . . . . 4 r .. .. ._ . . . . ,. . - .

c 7.23E-04 .8.49E-03 1.L5E-02 2%1E+OO

< 3.61E-04 < :lA5EX3 354E-03 3.86E-02

’ 3.35E-02 93.9E-03 l.l6E+OO 6.63E-03 6.55E-01 4.12E-03 2.33Etoo 835E-03

..c 2.89E-W 1.99303 232EtOl 7.95303 1.01E-02 159E-03 1.19E-03 1.45E.03 357E-02 5.72Ea-l 924E-01 259E-01 n d . mi

I 622-02 15E-03

I

...- .. ..

. -

4 9 W 2 -

5.11Ei-04 4.60E-04 332E-04

1.07E-02 9.45E-w 1.4SE-02 358E-04 2.OIE-02

I

12OE-01 1.94E-03 13oE.03 153W

7.66E-M 6AbE-03 5.13E-02 279E-02 5.9fiE-02

2.oOE-02 1.4OE-M

. .

b


January26,1994

!

I

Appendix 3 Elemental Composition of Sample #2-2

Total !jampleTl]

Average std. DeP421 Element WL% WL%

Ag As Se ca Cd co cu Mi3 Mn Pb zn zr A i - Ba F42

La Li Mo N8 Ni Sn Sr Ti V B 8 P Si K

U pu

Hg

c 4.01E-04 < 4.01Wn

8.23E-03 4.47I3-05 6AOW I .70Eo4 I.Im-03 2.07E-04 1.29EX3 214E91 rsE-04 2.47E-01 139E-w 2.40E-02 2.22E-M 2.50E45 1 . W 3 2.6m-01 1.03E-04 1.26E-03 1.4OE-M 355E-05 33!x& 7.62E-W 7.88- 4.32E-01 215E-02 3.07E-02 5.41E-05 4.8304 4.2E-M

m 6.93E-03

. 9.66E-06 157E-M 257E-05 1.16E-03 8.92EM 1 9 m 639E-02 1 . 7 M 5.78E-m 9 2 M 1.6oE-02 7.96E-M 1.WE-05 5.08E-05 7.98E-01 1.12E-05 8.77E-05 1.16E-06 1.ME-05 4 . M W 3.94E-05 219E-02 1.62E-01 2.34E-02 7.44E-04 1.22E-05 2.5505 9.7E-07 ,

I

f

t

. ... . . __. ... . . . : r _ . a,. - . . . . . . . -.

..


January 26, 1994

Appendix 4 Elemental Composition of Sample #2-3

Total SampIe[l] Water Soiuble Fraction[l] Water lasoluble FradIon[2]

Average Std. Lh?v.[31 Average Std. Dev43 J Average Std. Dev.[31 Element Wt% . Wtsb WL% ' Wt% wt. Qk Wt. z

Ag As Se Ca cd co cu Mg Mn Pb a zr Al Ba

. Fe La Li MO

Na Ni Sn St Ti V B cr P Si K Hg U Pu

< 1.71E-04 < 1.71E-03

3.29E-03 5.12E-05 6.80uM 1.68Eo4 2.64504 2.07E-w 1.03E-03

1 . 1 m 1.01E-01 9.05E-05 3.58E02 257E-04 3.17E-05 75E-w 2.73EtOl 1.18E-w 1.06E-03 1.75E-05 438wH 5.04E-04

5.78E-02 3.26E-01 238E-03 237E-02 5.93E-05 2.7E.a 2 9 W

nr

6.87~~02

5JjEo4

c 5.07E-07 1.69E-M < 5.07E-06 1.69E-03

3.29E-M. 1.62EZ-03 8.65E-04 1.22E-05 8.43-

597305 8.43E.05 1.66E-04 2.10E-05 138E-04 2.53- 2.07E-04 1.69F.43 3.12E-02 264E-02 6.68E-05 1.69E-04 4.79E-02 9 . 4 0 2 4.3E-05 337E-05 2.17E-m 1.69E-04 5.61E-05 ' ' 253- 1.82E-05 6.74E.05 139E-M 5.48E-04 3.78E-01 2.7lEMl 3.64E.05 4.2IEo4 4.08E-04 6.78504 7.39E-06 1 -69E-05 1.79E-05 8.43E-05 1 JOE44 8A3E-05 9.26E-05 337Eo4 136E-02 6.79EM 5.95E-02 251E41 8.44E-04 5.06E09 2.7- 1.98E-02 1.17E-M C 7 . 6 8 E a I S M 1.4- 27E-07 m

336Jxn 337i-04

1

1.76EM 1.76E-04 6.04E-05 7.11E-04 8.81E-06 3.53E-05 8.81E-06 7.26E-M 2.m46 1.76Eo4 3.01E-02

. 1.7- 5.68E-02 3 5 3 w 1.76E# 2.64E-05 7.05E-06 2 . 0 M 12om 4.4lE-05

1.76E-06 8.81E-06 8.81E-06 353E-M 1.OOE-03 728E.02 5.29E-05 1.13E-03

< I.OIE07 3 2 4 %

c 6.04- 8.24E-03 8.00E-03 2.17Eia.l 3.3z-03

cI.21E-03 ' 1.24E42 33lE-02

* 3.82E-02 24232-02 3.17E+00 3.76E-03 4.84E-01 1.02E-02 697EW 7.12E-03

.< 241K-W 2.54E-03 239E#1 5.m-M 156E-02 t5sFi-03 1.07E-03 8.72E-03

e 8.72E-03 393EM 7.05EW 2.01E-01 nd nd 9.m-03 3.8E-04

3.63E-02 . 5.76E-04

1.02E-03 23- 726E-M 5.76E-03 5.42302 1.13E-03 1.63E-02 6.40E-04 121Eo1

I '

. 253E-3-01 1.17Eo3 1.28E-03 .. 1 A9E-04 7 . m 12OE-03

8.11E-02 1.24E01 551602

1.4E-04 42-05

I

L. ...

WSRC-TR-94-057 L .

-page25 - January 26,1994

.. .

CC: G. T. W@ht, 773-A T. M. Monahon, 703-H €2 A. Scaggs, 703-H J.Morin, 719-4A R 0. Croley, 241-12OH J. N. Brook, 241-12OH

D. C. Wood, 7W21C W. E. VanPtlt, 241-15W

P. Rutland, 241-1523 J. E. Maria, 703-H PI L. m y , 703-H \ M. C. Chandl~r, 70343 3. S. Clemmons, 703-H P. D. d'Entremont, 703-H W. R. Jambsen, 703-1OC P. C. Padczanin, 772-3F J. E. SEW- 772-3F C M. Grtgory, 772-3F S. L. Maxwell, 772-F C. Y. Boler-Melton, 7724

L. M Papouchado, 773-A C. R. WoEe, 773-A

M. K. Holland, 772-3F 3. Satkowski, 772-3F

W. L. Tamosaitis, 773-A A. L. B l i ~ ~ ~ e t t , 773-A W. S. Cavin, 773-A P. F. Clocssner, 773-A D. D:Walker, 773-A M. J. Barnes, 773-A N. E. Bibler, 773-A M. C. Thompson, 773-A D. G. Karraker, 773-A TIM, 703-43A IWT-LWP File, 773-A

A. Q- GOSICII, 773-22A

4

1

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