ML20206H733

Thermal Effects on Precoat Matl for Spent Fuel Pool Filter/ Demineralizers,Vermont Yankee Nuclear Power Station

ML20206H733
Person / Time
Site:	Vermont Yankee File:NorthStar Vermont Yankee icon.png
Issue date:	03/31/1987
From:	Mackoul L STONE & WEBSTER ENGINEERING CORP.
To:
Shared Package
ML20206H290	List: ML20206H288 ML20206H733
References
NUDOCS 8704150428
Download: ML20206H733 (26)

Text

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• ENCLOSURE 2'

.g. b THERMAL EFFECTS ON PREC0AT. MATERIAL FOR SPENT FUEL POOL FILTER /DEMINERALIZERS VERMONT YANKEE NUCLEAR POWER STATION 1

Prepared for Yankee Atomic Electric Company.

Framingham, MA By L. J. MacKoul March 1987 1

\

Stone & Webster Engineering Corporation Boston, Massachusetts P l l

l 7955-17055-B1 u.

. g. .s TABLE OF CONTENTS

!! Section Title Pate j- I. BACKGROUND 1 II. CONCLUSIONS AND

SUMMARY

1 III. SPENT FUEL POOL FILTER /DEMINERALIZER SYSTEM 3

.IV. ION EXCHANGE RESINS 4 V. TEMPERATURE EFFECTS 5 VI. ALTERNATE PREC0AT MATERIAL 12 TABLES FIGURES REFERENCES I

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i3 I. BACKGROUND Yankee Atomic Electric Company retained i Stone & Webster. Engineering Corporation to demonstrate'the acceptability of the precoat material used in.

the Vermont Yankee spent fuel pool filter /demineralizer under the present technical specification fuel pool . temperature limit of 150*F. during all Nuclear Regulatory Commission postulated conditions. Nuclear Regulatory Commission Standard Review Plan 9.1.3.', " Spent Fuel Pool Cooling and Cleanup System," stipulates a maximum fuel pool temperature of 140*F.

The report herein has evaluated the thermal effects on precoat s.aterial over a temperature range of 120 F - 200*F (50*C - 90*C).

Recommendations on a maximum operable temperature for the presently used.

precoat material and alternate precoat material have also been evaluated as part of this report.

II. CONCLUSIONS AND

SUMMARY

The evaluation of thermal effects on precoat material for the - spent fuel pool filter /demineralizer system has. established the following:

• Cation exchange resin leakage and ionic capacity are not affected in the evaluated temperature range of 120*F-200*F.

7955-17055-B1 1

• .The crud holding- capacity of- the various precoat material formulations used in 'the filter /demineralizer system are not affected in the evaluated temperature range.-

• Increased silica leakage and a reduction in' strong base anion capacity are experienced in the evaluated temperature range.

• An increase in silica l'eakage -of less than 10 percent and a reduction in strong base anion capacity of less than 2 percent would be experienced at 150*F as compared to at 140*F for 7-day, 14-day, and 30-day time periods.

Based on these findings, the present technical specification fuel pool temperature limit of 150*F has minimal impact on the performance of precoat material experienced at 140*F. The impacts on filter /demineralizer run length associated with reduced strong base anion capacity and on the effluent quality associated with increased silica _ leakage at ' the 150*F temperature are barely measurable and would not be expected to affect the spent fuel pool water chemistry.

The impacts on run length and effluent quality become more pronounced at-temperatures above 150*F. At 180*F, approximately 80 percent of the-initial strong base capacity remains while silica leakage' increases . by about-60 percent of its value-at 140*F over a 30-day time period. At-200*F, less.

than 50. percent of the initial strong base capacity remains .while silica leakage increases by almost 90 percent of its value at ' 140*F. over a 30-day time period. The acceptability of this performance depends on the station's -

7955-17055-B1 2

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. capability of dealing with. the potential of shorter run lengths :(half the run lengths to anionic exhaustion at 200*F for a 30-day time period) and (the permissiveness of experiencing -longer times to reduce spent fuel' pool silica concentrations.

i a-There are no other precoat materials having ion exchange : and filtering

! capabilities that would not experience the same thermal effects 'within th'e 4 120*-200*F temperature range.

III. SPENT FUEL POOL FILTER /DEMINERALIZER SYSTEM f

4 The ~ spent fuel pool filter /demineralizer system. includes two filter / >

i deminerlizer units each rated at 450 gpm and having approximately 267 square feet of filter element surface area. Normally the filter elements are

, precoated . with Ecodex P-205H. consisting of 1 part fibrous material and 9 parts powdered resin in a ratio of 5 parts strong' base anion resin in the i hydroxide form and 4 parts strong acid cation resin in the hydrogen, form.-

i; This material is applied at a dosage of .0.2 lbs of precoat per square foot l of filter element area. The precoat material and the cation to anion resin

! ratio can change depending on chemistry conditions within the spent fuel i pool. Table 'l presents guidelines for precoat material used under various chemistry conditions taken from R. P. 4628, " Sampling and Treatment of the-Fuel Pool System."

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$ A filter /demineralizer unit remains in service until:

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• The differential pressure across-the unit reaches 15 psid j i  !

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• The unit is operating . at a: flow rate . less than rated, but an-increase in flow would' result in a 15' psid ' differential pressure

• Samples indicate the demineralizer resin is near exhaustion:or the effluent conductivity is high To ensure continuous optimum results, precoat service life is limited to 4 weeks during normal chemistry conditions.

The system is designed to operate to the spent fuel pool chemistry condi-tions listed in Table 2.

IV. ION EXCHANGE RESINS The basic physical structure of whole bead and powdered cation and anion

exchange resins contains long chain polymers (polystyrene) which are-cross-linked together with divinylbenzene to provide strength, insolubility, and resistance to melting and distorting over a range of temperatures (Reference 1). Ion exchange sites (functional groups) are added to the structure to provide ion exchange capability. In the case of strong acid cation resin, a sulfonic group is fused into the. polymers. In the case of type I strong base anion resin, a quaternary ammonium group is fused into the polymers (Reference 2).

The stability of ion exchange resins depends on the physical and chemical environment to which the resins are exposed. Factors which affect resin stability and degradation include:

7955-17055-B1 4

• Temperature

• 0xidation

• Fouling

• Osmotic shock

• Radiation

• Mechanical attrition Degradation. can lead to the decross-linking of polymers and the loss of ion exchange sites causing losses in capacity, physical integrity, density, and ion exchange reaction kinetics (Reference 3).

Cation exchange resins are generally more stable than anion exchans,e resins.

Losses in cation exchange resin typically range between 2-5 percent per year.

while losses in anion exchange resin usually range between 5-25 percent per year (Reference 3).

/

For purposes of this report, only the temperature effect on ion exchange and

fibrous precoat material are addressed. Other influencial factors are not I considered.

V. TEMPERATURE EFFECTS Ion Exchange Resins Cation exchange resins are more resistant to thermal degradation than anion exchange resins. A typical maximum temperature recommended for hydrogen

. form operation of cation resins is 250*F (120*C) while the maximum i

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temperature . recommended . for anion resins - in the hydroxide ' form is 140*F (60*C)' -(Reference 3) . ~(The hydrogen and hydroxide . forms lare used '. in : the precoat material for the spent : fuel pool filter /demineralizer system.)

.Although the thermal stability of ' strong -base anion exchange resin iis

greater in the chloride form .(Reference 4), this form-cannot be used'in the filter /demineralizer system sine'e . it would'. result in- high chloride-concentrations in the

pool.

It is important to understand that the maximum recommende'd temperatures cited above are intended to be reference points. There is no fixed.

temperature below which resins are considered stable and above'which they are considered unstable- . Thermal degradation of ion exchange resins occurs at all temperatures with the rate increasing with temperature. At approximately 750*F, resins - are reduced to an a'sh and rendered completely useless (Reference 9).

The thermal degradation of cation exchange resin will not be further i-discussed in this report, since the temperature range of concern 1

(120 F-200 F) is well below temperatures at which degradation effects are -

measurable.

1 Increasing temperatures increase the silica leakage and decrease the ion l 1

I exchange capacity of anion exhange resins. Silica leakage is important since the concentration of silica in the spent fuel pool is limited.' Anion exchange capacity is important since it establishes the service run length of a filter /demineralizer unit to anionic exhaustion.

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Silica Ldakage.

. Silica, leakage from strong base anion exchange resin is a function of water temperature as shown in Figure 1 (Reference 5). This phenomenon is .-

' attributable to the hydrolysis of silica from the anion resin - at higher temperatures. Silica leakage from strong base anion exchange ~ resins. doubles as the temperature increases from 60*F to 90*F and quadruples : as the temperature is# increased to 140*F.

,p Using 140 F as the base temperature and . extrapolating . data 'from the literature .to $00*.", the pezcentage changes in silica - leakage ' from anion

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resin has been calculated and presented in Table 3.

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The percentage.Ehange in silica leakage at 150*F is only 9.8 percent.

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4 Operating at demperatures up to 170*F produce changes in silica leakage of

't less than 50 percent. I 1 \ ..

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Anion Capacity '

The thermal degradation of strong base anion resin is accompanied by losses of total anion capacity and strong base capacity (Reference 6). Degradation

,y curvesj for strong base capacity and total. anion capacity as a function of

<L time- and temperature are shown in Figures 2 and 3, respectively (Reference 4). 'I-3 j

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. ..t LDuringLthermal' degradation . of strong - base.' anion exchange 2 resin, lthere ~is

. both . a - loss . of. exchange sites and 'a partial conversion 1 of the strong base

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, Jexchange sites to weak base : exchange : sit'es. The: strong base sites are icapable of L removing both the highly ' dissociated istrong acids (sulfuriciand:

hydrochloric) ' and ' the.. weakly dissociated weak acids ~ (carbonic and silicic).

$ The weak base sites, on the . other hand, f are .' only' capable of removing - the highly dissociated strong ' acids (Reference 2).

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This Laccounts . for the

. slightly higher -capacities 'in Figure ~ 2 : than in Figure 3. - Table 4 is ~ a

-tabulation of _ thermal degradation half-lives of strong . base -capacity as' a-f' -

function of. temperature (Reference 4).

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l. This' data'~is based on a first order reaction ' to describe the loss -of anion

. strong base capacity.

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l Using the half-lives in Table 4 and considering 7-day, 14-day, 30-day,.and i 100-day time periods, Table 5 shows the ' ratio of the anion ' strong . base.

capacity at the end of the time period to the initial strong base capacity resulting from thermal degradation. Half-14ves were used to make these 4

determinations rather than Figure 3 due to the difficulty interpreting the.

t graphical data at these short exposure periods.

The data in Table 5 shows - that over 90 percent of the. initial. strong base t i

capacity of the anion resin remains up to temperatures of 176'F for 7-day and 14-day time periods and 167*F for a 30-day time period.

4 The percent losses in capacity'at 150'F as compared to 140'F are 0.25, 0.50, f:

> and 1.30 for 7-day, 14-day, and 30-day time periods, respectively.

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Using 140*F as the base temperature, Table 6 shows the changes in strong base anion capacity which would result-from operating at temperatues between 120 F and 212 F~for 7-day, 14-day, 30-day, and 100-day time periods.

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The loss of anion capacity causes a proportional decrease in filter /

demineralizer' run length to an anionic endpoint or . complete anionic exhaustion. Thus, if run lengths were terminated on either of these bases, they would decrease by - less than 2 percent for 7-day, 14-day,land 30-day.

time periods, respectively, at a temperature of 150*F _ as compared to run -

lengths at 140*F.

Crud Holding Capacity Testing by Graver Water Conditioning Company indicates that temperatures in-the range of 200-285 F do not significantly affect insoluble removal or the crud holding capacity of precoat material (Reference 7).

4 Testing was performed at temperatures of 286*F, 248*F,194*F, and 148 F for three days at each temperature. The pilot unit was operated at a service

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flowrate of 4 gpm per square foot and with a precoat having 'a cation to anion ratio of 2:1 for each run. Results of the testing indicated:

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• High temperatures do not_ adversely affect the pressure drop-of the  !

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• High temperatures do not significantly affect insoluble removal-7955-17055-B1 9

.a Pressure drops across the_ pilot unit were unchanged over each of the'threel day T runs and average percent insoluble ' removals were . 87, 89, '92, and 93 at temperatures of 286*F, 248 F, 194 F, and 148*F,_.respectively.

Additional-testing was performed at 245*F to determine operating run~ length.

and _ capacity . of precoat for . suspended solids. After twenty-one days',1the pressure drop was less than 8 psid and ' the- precoat capacity for susp' ended metals was estimated to be 0.12 pounds per dry pound of precoat.

-Extrapolated to a pressure drop endpoint of 25 psid, the precoat capacity for suspended- metals was estimated to . be 0.20 pounds per dry pound of precoat.

, Figure 4 shows pressure drop as a function of pounds of suspended solids removal per dry pound of precoat material for a 245*F and an 80*F run. In this figure, the weight of crud is based on converting metals to their respective oxides. The figure shows that crud- ho'1 ding capacities are comparable at_the two temperatures.

Operating Data Spent fuel pool ~ filter /demineralizer influent- and effluent chemistry data froa February 22 to March 17, 1987, is presented in Table 7. During this period pool temperatures ranged approximately between 100*F and . 110 *F .

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- 1 1 The Ecodex -P-205H precoat material formulation 'used during .the .above time

' period, contains _- fou'r parts strong Jacid cation . resini and 'five' parts: strong

- base ' anion ' resin. This ratio provides equalcionicicapacities for eachitype4 resin since cation resin has a. capacity of 5. meq/gm and anion ' resin has a 1

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. capacity of 14 meq/gm. Reductions in anion resin.Leapac'ity due- to - thermal degradation thus cause an imbalance in the two ~ capacities ' which leads '.to -

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-faster -anion breakthrough, increased effluent conductivity and shorter ,

service runlengths. Service runlengths expected at higher temperatures for the chemistry conditions shown in Table 7 'can be approximate'd by multiplying i

the 24-day' runlength experienced . above by the ratio ' of the residual" anion.

capacity at thirty. days"(Cao) to the initial anion capacity (Co) presented in Table 5 for a ; articular temperature. -

Typical silica leakage from a mixed resin bed filter /demineralizer is about .

10-20 ppb at 70'F for the influent chemistry conditions shown iti Table 7. '

Applying silica -leakage correction factors . from Figure. I to this leakage, the effluent silica leakage would be expected to be about 15 ppb ~ to 40 ppb at temperatures of 100'F to 110*F. (Actual effluent silica -values taken during the service run averaged 38.5 ppb.) Based .on. the chemistry conditions of Table 7, silica leakages would approach' influent silica values throughout the service run !at operating temperatures not much .above 110'F, resulting in limited silica removal. Silica removal expected under other chemistry conditions would depend on the influent sil'ica concentration and the effluent silica leakage at a particular temperature.

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'7955-17055-B1 11

-VI. ALTERNATE'PREC0AT MEDIA 4

There are no other precoat materials available . which possess- ion exchange and filtering capabilities that would not experience the same i thermal effects within the 120*F-200 F temperature range evaluated

.(Reference 8). If the loss of anion strong' base capacity with

, temperature becomes a limiting factor, it may be possible to provide i additional capacity by increasing the anion to cation resin ratio or by 4

adding more anion resin to the precoat formulations shown'in' Table ~1.

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TABLE l' PREC0AT DATA FOR FUEL POOL'DEMINERALIZERS ,

f Resin Ratio Dosage (lb/ft 2 Approximate (Cation: Anion) Mixed Resin) Dry Operation ' Dry Basis Dry Basis Weight' High Metal 3:1 0.2 38 lb Cation Content 13.6 lb Anion High Anion ~ 1:2 0.2 19 lb Cation Content (e.g. 37.5 lb Anion I, SO4 , etc.)

High Metal and 1.52:1 0.2- 38 lb Cation Anion Content 25 lb Anion Normal 4:5 0.2 21.3 lb Cation 26.6 lb Anion 5.4 lb Fiber n

1 7955A-17055-B1 1 of 1

A TABLE 2-FILTER /DEMINERALIZERS DESIGN PERFORMANCE' 4

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Constituent Influent Effluent-Conductivity, Micromhos/cm <1.0 - 0.1 at 25'C ,

pH 6-7.5 neutral 4

Heavy Metals, ppm <0.1 __<0.05

. Silica, ppm <1 <0.05 i

Chloride, ppm '<0.5 <0.02 Total Solids, ppm <1 --

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, SILICA ~ LEAKAGES 2

i ~ Temperature Correction Percent Change in I ('F) Factor Silica Leakage-

! 120 3.1 -24.4 1 130 3.6 -12.2 140 4.1 base

, 150 4.5 +9.8 i 160 4.9 +19.5 ,

170 5.6 +36.6

, 180 6.5 +58.5 i 190 7.0 +70.7 200 7.7 +87.8 l-4 1

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~ THERMAL DECOMPOSITION HALF-LIVES' TYPE I. STRONG BASE RESIN Temperature Temperature Half Live- Half Live

(*F) (*C) (Days) (Years) 122- 50 2,750 .7.5 140 60 1,870- 5.1.

'149 65 930 2.6 158 70 480 1.3

=167 75 258 : 0.71

-176 80 .139 0.38 194 90 43 0.12 212 100 14.2- 0.04' i

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TABLE 5 RESIDUAL STRONG BASE CAPACITIES Tempera- Tempera- Half ture ture- Live C7 C7 /Co C 24 C14/Co Cao C3o/Co Cgoo C3 oo/Co

(*C) (*F) (Days) (meq/gn) at 7 days (meq/gn) at 14 days '(meq/gn) at 30 days (meq/gn) at' 100 days -

50 122 2,750 3.99 0.998 3.99 0.996 3 97- 0.992 3.90 0.975 60 140 1,870 _3.99 0.997 3.98 0.995 3.96 0.989 3.86 0.964 65 149 930 3.98 0.995 3.96 0.990 3.91 0.978 3.71 0.928 70 158 480 3.96 0.990 3.92 0.980 3.83 0.958 3.46 0.866 75 167 258 3.93 0.981 3.85 0.963 3.69 0.922 3.06 0.764

<80 176 139 3.86 0.966 3.73 0.932 3.44 0.861' 2.43 0.607-90 194 43 3.57 0.893 3.19 0.798 2.46 0.616 0.48. 0.120' 100 212 14.2 2.84 0.711 2.02 0.505 0.92 0.231 0.03 0.008-Nstes: H

1. Initial anion strong ba'e scapacity (Co) is 4.0 milliequivalents per gram (meq/gn).

2. First order chemical kinetic reaction of the -form:

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TABLE'6 CHANGE-IN STRONG BASE ANION CAPACITIES Temperature . Temperature Percent Change in-Capacity-

-(*C) (*F) 7 Day 14 Day- 30 Day. -100 Day 50 122 0.0 +0.25 +0.25 - +1.04 60 140 base base base base 65 -149 -0.25 -0.50 -1.26' -3.89

'70 158 -0.75 -1.51 -3.28 -10.36 75' 167 -1.50 -3.27 -6.82 -20.73 80 176 -3.26 -6.28 -13.13 -37.05 90 194 -10.53 -19.85 -37.88 -87.56 100 212 -28.82 -49.25 ' -76.77 -99.22 7955E-17055-B1 1 of 1

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OPERATING CHEMISTRY DATA >

SPENT FUEL' POOL FILTER /DEMINERALIZERS- _ .

FEBRUARY'22 - MARCH 17, 1987' Conductivity . . Filterable pH (micromhos/cm) ' Cl (ppb) . 'SiO2 (ppb) Solids (ppb);

Dste' In- -Out In~ Out In- .Out. -p1 . Out- In. Out-

2-22-87/ - -

0.19 0.07 - - -- -- --  :

2-23 - 1- 0.21 0.10 -- -

'15 < 10 =: -

2-24-87 -~ -

0.23 0.15 - -

33 28  :- -

2-25-87 .0.22 O.26 - -

50 -40 - -

2-26-87 6.42 6.13- 0.32 0.30- < 10 < 10 58- 37. <.10 -< 10-2-27-87. - -

0.40 0.39 -- -

'55 55 - -

2-28-87 - -

.0.45 '0.44 -

55 55 - --

3-1-87 - -

0.49- 0.49 -- -

,. '45 45 -- -

~3-2-87. - -

0.53 0.52~ - -

55 50 - -

3-3-87 - -

0.55 0.55 - -

35 .

40 - -

3-4-87 - -

0.58 0.58 - --

35 35 - -

3-5-87 7.27 6.71 0.61 0.61 20 < 10 35 25 < 10 < 10 3-6-87 - -

0.64 0.64 - -

40 30 - -

3-7-87 - -

0.68 0.68 - -

40 35 - -

3-8-87 - -

0.71 0.71 - -

40' 35 -- -

3-9-87 - -

.0.72 0.72 - -

48 39 - -

3-10-87 - - - - - - - - - -

3-11-87 - - - - - - - - - -

3-12-87 5.82 5.96 0.72 0.72 < 10- < 10 59 57 < 10 -< 10-3-13-87 - - - -

3-14-87 - - - -- - - - - - -

3-15-87 - - - - - - - - - -

3-16-87 - - - - - - - - - -

3-17-87 Fuel Pool F/D Precoat Changed Average - -

0.49 0.46 13.3 10 43.6 38.5 . < 10- l< 10 1

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4

. e REFERENCES

, i

1. . Owens ,- Dean L., Practical Principles of Ion Exchange Water Treatment.

Voorhees, New Jersey, Tall Oaks Publishing, Inc., 1985.

2. Applebaum, Samuel ~'B., Demineralization by Ion Exchange. New York,

. Academic Press, 1968.

3. Dow Chemical Company, " Water Conditioning Manual", 1981.

4. McGarvey, F.X., " Efficient Operation _of Strongly Basic Anion Exchangers Part 1- High Temperature Effects", . presented - at ' the 16th Annual Liberty ~ Bell Corrosion Course, Philadelphia, PA, September 11 - 13 ,

-1978.

5. ..Rohm and Haas Company, "Amberhilites", Nos.'137 and 139,.1973.

6. Wirth, Louis, "The Expected Life of Anion . Exchangers", Combustion Magazine, May 1954.

7. Graver Water Conditioning Company, " Powdered Ion Exchange in Nuclear Cycles", presented at the 30th ! Annual American .~ Power Conference, Chicago, Illinois, April 23 - 25, 1968.

8 -Conversation with Al Taveras of Graver Water Conditioning Company.

9. Conversation with Dwight Tamaki of Ionac.

1 i-

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