ML19317H508

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Discusses Cryogenic Separation Process Developed for Removal of Kr-85 from Reactor Containment Bldg.Basic Process Scheme Is to Link Cryogenic Air Separation Plant to Bldg Atmosphere in Closed Recycle
ML19317H508
Person / Time
Site: Crane 
Issue date: 04/09/1980
From: Lytton M
MITRE CORP.
To: Vollmer R
Office of Nuclear Reactor Regulation
Shared Package
ML19317H507 List:
References
RTR-NUREG-0662, RTR-NUREG-662 W85-049, W85-49, NUDOCS 8006120075
Download: ML19317H508 (8)
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Text

,p

& fS'l The MITRE Corporation Metrek Division i

April 9, 1980 W85-049 Richard H. Vollmer, Director Division of Engineering Nuclear Reactor Regulation Nuclear Regulatory Commission Bethesda Office, Room 542 Washington, D.C.

20555

Dear Mr. Vollmer:

Confirming my process disclosure to you in our meeting of March 21st and my prior meeting on March 10th with Messrs. Sydney Miner, Mark Greenberg and Jerrold Carter of your staff, I have developed a cryogenic separation process for the removal of radioactive Krypton 85 from the Three Mile Island nuclear reactor containment building. The process will reduce the estimated 57,000 curies radiation content to a total of 5 curies or 2.5 microcuries per SCF vent air.

The engineering and design details of my process disclosure are shown in:

e Figure 1: " Proposed Process Schematic Diagram for Krypton 85 Removal..."

00 e Table I:

" Basic Process Scheme, Derivation of Kr Reduction Equation and Calculation of TMI Containment Building Reduction" e Figure 2: " Reduction of Krypton 85 Curies Radiation..."

The basic process scheme is to link a cryogenic air separation plant to the containment building radioactive atmosphere in a closed recycle. Thecryogenicplantwillseparatetheatmosphereigoits constituents: oxygen, nitrogen, argon, and enriched Kr + Kr fraction.

All the constituents, except for this enrichen fraction, will be re-cycled to the containment building. The Kr + Kr85 fraction will be filled into shielded metal gas cylinders, and the '57,000 curies re--

moved for burial in a remote location. Depending on removal efficiency, the clean-up will require 3.6 to 16.2 days of continuous operation.

The cryogenic separation technology has been known for more than 40 years (see M. Ruheman, "The Separation of Gases," 2nd Ed., Oxford Univ. Press, 1949, p. 228-236). The proprietary patentable features of my process are (1) use of a normal krypton fresh make-up feed to enable the delicate, complex vapor-liquid equilibria to function at 1420 Dodey Madison Bouisvarc. McLean, Virguus 22102 Teiephone W3152* 4000

  • Telex 39-9118

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Richard H. Vollmer April 9, 1980 Page Two low krypton solute concentrations in the distillation columns and 85 and (2) a process combination of air separation to sweep out the Kr plant, krypton distillation column, and molecular sieve filter bed to remove the radioactive Krypton 85.

A 50 Tons / Day oxygen air separation plant will be required.

The entire installation, including modifications to add a krypton dis-tillation column, molecular sieve filter bed, supplementary cryogenic refrigeration, and a centrifugal compressor, will cost between $10 to

$20 Million. A used air separation plant can be obtained on short notice from Union Carbide (Linde Div.) or Air Products. The fresh make-up gas feed (about 900 liters) can be readily obtained for about

$0.70 per liter from three U.S. suppliers: Union Carbide (Linde Div.),

Air Products, and AIRCO. Other equipment and installation materials can be purchased new or used from a variety of suppliers. The project schedule would require 11 months: procurement, fabrication modifications and installation - 9 months; start-up, debugging and optimization -

1 month; and removal of the Kr85 from the building - 1 month.

My credentials for the validity of the proposed process and project engineering details are as follows:

e Employed 1955-1969 with AIRCO, Inc., second largest cryogenic air separation plant gases manufacturer in U.S.

Engaged in process engineering, design, project engineering, construction and capital investment planning for sixteen plants.

Developed AIRCO engineering and design for proposed e

Kryptc 2 85 removal from U.S.S. Savannah nuclear reactor, and installation of krypton recovery units in air separation plants.

The MITRE Corporation would be pleased to offer a proposal to NRC for consulting services to carry out the proposed process and project engineering / management details. We look forward to the opportunity to meet with Mr. Harold R. Denton, Director of NRC Nuclear Reactor Regulation, te discuss our proposal which you indicated that you will try to arrange.

Should you want additional information or clarification, please telephone me at (703) 827-7198.

Sincerely, Milton Lytton Enclosures i

ML:njo l

l no _ -

o we e ~

~=w

18aff5:

l. Tyytcc! Cayogente air Separetton Flaat CRYtX;FNIC SEFADATION FIJulT C(AD Bot wist. Egyptua Eevistement biatillstlun l

Columns to dieduce by Continuuea Recycle el.e Cuutalement Sulldlag Atmusp*. ore Air NECYCl1 DESukB NITROCEN WlY10 01YCEN & ABCtJII CASES 0I g

SF,uust cus tas Es to S Cartes ur 4

6 4

2.S Macau-Cuttem/SCF Vent Air.

  • O U
8. Separattues Plant Erypton Beneval Cycle l

,IM

2. oposat ten testalle Casa Se Readily i

NJIf l.J 6us opa l,et antion.

g kECTCIE OKYGEN & ARCON CASES l0 Et t 8c tes ty Variatela Fr. s 20 % to 901 AuusJtug Tu Destges. Require 16.2 to RECYCLE 3

,j 1.6 Days ActerJiantly For at=Juctices.

JITRUCEN CAS

4. Supplementary Cycle Nitrogen Refrig.

g m

Speten May Be Required To Balance loads.B

,p 1.1 4000 BCFtt RECYs1E SEFAkATEI) CASES DEFtETED IN Es0I

  • g lg AND EkTFTON L

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10.000 SCFH RECYCLE AftR)S. AIR 0

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,61 4000 SCtti ATHOS. AIR I3 70 CRYOGENIC SEPARATI ist g

mm g

Int a I

PURCHASED CYLINDERS e

I ERYFTON & Kr85 e gmYpitet gg NokMAL Al?tOS. ERYFTON FRACTION TO REMUTE CAS FEED HAKE-UF BURIAL.

l. TNI Nuclear Reactor Containment But! Jing; 2,000,000 Cu.Ft.;

57,000 Curtes Kryptosi 85.

FicuRE I

2. Eatsting Ventilating Air Blowers (2). Eacts 24,000 SCHI Air Flow.
3. Furtlineed Normal Atmusplaeric Esyptoen Feed Hake-Up Frue Cas CylinJer. Total Required: 887 Litare.

Fmorosit!

4. Cent rif ugal Ces Compreemor 4000 SCFM at 8$ FSI A Delivery.

PaoCESS SCHrMATic DIACRAM S. Als teolatuse Dryer, S!!!ca or Alumina Bed 40 0F, Dual Swing Vessela - AJeoul>/Deaurb.

2 mend 51 0 by Cool-Down Attout -250 "F.

Folt

6. Cayugenic Multi-Fammage Reverstag Eaolemagers; Remuve CO 2
7. Juulu-11eumeues Espanaton Valve to Coul-Duwrn Air to about -280 "F to Fusa LiqutJ/ Vapor Him.

gg g,~

j 8.9. Duutele Distillation Culumns

8. Nitrogen Section,
9. Oxygen Sectiost to. Hul cular Slave Flitar for Nydsucasbust Impurittaa.

Futet letN:tKAR Rt AC10R

85) Dieg)!!atlast Coluant -

Bottomas Er0I, Er, Re, Ar, 0

  • I E

son I

(Including Kr 2

88. Enssched Egyptoen Fraction (Isicluding Kr Waportter to Castfy.

T11R1E HilE ISIANta, FFNNA.

44 t.in,le Hulecular Steve F8 tter, Dual Swing Vessela. Operate stauut -295 0F.

Adaurb og and Ar.

ii. Nit sugen Wase Cae Desusta Ituater for Holecular Steve Bed Demosptioen of 02 and Ar.

16. bemoeb Cam 8 tower.

C000FIDENTIAL HILTON LY1TOII

87. kusiched Krypton Nanture (1:arluding Kr85. Kr. Xe) Compreemur For Filling Cam Cylisidera.

FROFRIETARY M11RE CORF.

18. SteinlJed Metal Kayptun Hlature Cam Cylinder Filling Bank.

Falled CylinJers Reunved To Disposal.

DISCLOSUgg HARCH 24, 1980

M. Lytt:n Tha MITRE CIrporatica March 24, 1980 TABLE I BASIC PROCESS SCHEME DERIVATION OF Kr85 REDUCTION EQUATION, AND CALCULATION OF TMI CONTAINMENT BUILDING REDUCTION GIVEN: Kr

= 57,000 curies Volume of TMI nuclear reactor containment building = 2,000,000 C.F.

Normal Kr in atmos. air = 1.0 ppm = 1.0SCF/1,000,000 SCF air TMI containment bldg. air blowers = 24,000 SCFM (two each)

OBJECTIVE: Reduce total Kr ' within building to 5 curies, or 2.5 microcuries/SCF vent air 1.

BASIC PROCESS SCHENE The cryogenic plant and the containment building are in a closed recycle with only one stream being discharged, namely, an enriched concentrated krypton 85.

It is necessary to maintain an inventory of normal krypton in the system of containment building atmosphere volume and the cryogenic plant in order to maintain a proper vapor-liquid equilibria in the cryogenic fractionation columns. Therefore, as normal krypton and krypton 85 are depleted in closed system re-cycle, purchased fresh normal krypton is fed into the recycle system to maintain the overall krypton inventory at 1.0 ppm or higher. The Kr85 is depleted continuously during the recycle and is replaced by krypton. This is the unique patent-sought feature of the process design. The closed recycle system returns the separated oxygen-nitrogen-argon streams from the cryogenic fractionation plant to the containment building atmosphere. The only change in the overall total system is the continuous depletion of krypton 85.

Therefore, the derived equation below represents this significant change in the total system.

The enriched krypton 85 stream is further concentrated by gas passage through molecular sieve filter beds at cryogenic low tempera-ture which effectively separate the krypton 85 from the oxygen and argon (which are in very much larger amounts). The separation is based on the sieve physical adsorption of the smaller molecules:

oxygen - 3.46 Angstroms and argon - 3.40 Angstroms. The concentrated stream consists of about 93 percent Kr and Kr 85 and the remainder is xenon; nitrogen is extremely low. The Kr85 rich gas is filled into radiation shielded metal gas cylinders and removed for disposal.

See Process Diagram, Figure 1, for illustration.

L J

P 2.

REDUCTION EQUATION DERIVATION 85 A.

~ Conversion of Curies Kr to Grams, Liters and SCF 5

85 3.578 x 10 Kr Half Life = 10.72 yr.

10.72 x 85 Kr85 Atomic Mass = 85

    • E##*

= 392.7 curies /g g

SS 85 Kr

= 22.414 liters /g-mol g-mol Kr85 = 0.2637 liters /g

= 1489 curies / liter 85 Bldg. Content = 5

= 145.15 g Kr 39 7 c rie g 57,000 curies

= 38.28 liters

= 1489 curies /1 38.28 liters

" 23.316 liters /CF = 1.352 SCF B.

Equation for Reduction of Kr 85 Let:

k = Kr b1dg. content at time t = 0, = 1.352 SCF 8

k = Kr 5 bidg. content at any time e t = Tin :, minutes R = Cryogenic Plant Kr85 recovery efficiency A = Bldg. sweep air flow, SCFM to Cryogenic Plant V = Air volume of Containment Building 8

= Kr 5 removal coefficient Y

Assume: R = 0.9, 0.7, 0.6, 0.5, 0.4, 0.3, 0.2 A = 4000 SCFM (1/6 of 24,000 SCFM Air Blower)

V = 2,000,000 C.F. = 2,000,000 SCF At time t = o, k = k, 1

Kr Bldg. content at time t = k,y = k - Yk.t g

9 g

where:

85 A

Kr Removal Coefficient, Y=Rxy Differentiate:

h = - Yk

= - Ydt Integrate:

t+C in k

=-

t=0 C = in k, at t = 0 2

in k - in k,= - Yt g

t in p = - Yt u

o I

-YU

=e o

k = k,e' g

Now, given objective is residual Kr85 = 5 curies in Containment Building, or 5 microcuries/SCF 85 5

= 1.186 x 10 ' SCF

~

Residual Kr

=k

= g 28.316 l

Assume: One 24,000 SCFM building blower in recycle operation.

4,000 SCFM side-stream is taken as feed to Cryogenic Plant.

2,0b 000

.0 x 10 R

Y=Rx

=

k = 1.352 e (2.0 x 10 Rt) t But 85

~

Residual Kr

=k

= 1.186 x 10 '

g e (2.0 x 10 Rt), 1.186 x 10"

-4

= 0.8772 x 10

~3

-4

- 2.0 x 10 Rt = In 0.8772 x 10 1

in 0.8772 x 10 '

~

t=7x

_3

- 2.0 x 10

,1

- 9.3416 R

~3

- 2.0 x 10 Time to Complete Reduction 8

of Kr 5 to 5 Curies

t

3 l

l l

^

3.

CALCU1ATION OF Kr REDUCTION Assume: Recovery Efficiencies:

0.9 down to 0.2 R

MIN.

DAYS 0.9 5190

'3.60 0.8 5839 4.05 0.7 6673 4.63 0.6 7785 5.41 0.5 9342 6.49 0.4 11677 8.11 0.3 15570 10.81 0.2 23355 16.22 4.

CALCULATION OF PURCHASED NORMAL KRYPTON FEED MAKE-UP Note: It is necessary to maintain an inventory of normal krypton in the system of containment building atmosphere volume and the cryogenic plant in order to maintain proper vapor-liquid equilibria in the cryogenic distillation columns. Therefore, as normal krypton and Krypton 85 are depleted in closed system recycle, purchased fresh normal krypton is fed into the re-cycle system to maintain the overall krypton inventory at 1.0 ppm or higher.

Norr l Krypton in Atmosphere

= 1.0 ppm = 1.0 SOF/1,000,000 SCF Air in Containment Bldg.: Nopn11 Kr = 2.000 SCF Kr 5

= 1.352 o

Total

= 3.352 In one - 4000 SCIH sweep cycle:

8 Removal of Kr + Kr 5 = R x 3.352 SCF x h

2 00 at R = 0.9:

Krypton Make-Up = 0.9 x J.352 x x 5190 Min.

2,000 00

- 31.314 SCF = 887 Liters at R = 0.2 Krypton Make-Up = 0.2 x 3.352 x x 23,355 Min.

2, 0 00

= 31.314 SCF = 887 Liters Therefore, Total Fresh Normal Krypton Make-Up is a Constant.

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