RETS – REMP Workshop NRC Activities June 25, 2007 Presented by Steve Garry
1 Serving the Power Industry problem solvedhps.ne.uiuc.edu/rets-remp/PastWorkshops/2010/4 GEL... ·...
Transcript of 1 Serving the Power Industry problem solvedhps.ne.uiuc.edu/rets-remp/PastWorkshops/2010/4 GEL... ·...
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14C COMPOUNDS OF INTEREST
Organic Carbon Gases – primary form for PWRs14CH4 and other hydrocarbons
Inorganic Carbon Gases – primary form for BWRs14CO2, 14CO not formed in appreciable quantities
Particulate CarbonCarbonate, bicarbonate, incorporated in debris
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SAMPLE MATRICES
AirPotentially high moistureLimited oxygen at some locations% levels of hydrogen at some locations14C activities can vary by factor of 106 between locationsWide range of gas flow rates and pressure at sample locations
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ANALYTICAL PROTOCOL REQUIREMENTS
Differentiate between organic, inorganic, and particulate 14CAccommodate wide range of sample activitiesSeparate 14C from other interferencesHandle flammable, low oxygen atmospheresEmploy practical sample times and gas volumes
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ANALYTICAL PROTOCOL REQUIREMENTS
Accommodate differences in sample flow, sample pressureAdaptable to differences in process interface hardwareEmploy hardware that can be reliably and conveniently transported to and returned from facilities
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PRIOR STUDIES
Thompson – 1978Combustion/mol sieve/cryo-trap/LSC
Kunz – 1985Combustion/Ascarite/cryo-trap/gas proportional counter
IAEA – 2004Review including combustion/NaOH soln/LSC
Magnusson – 2008Combustion/NaOH soln/LSC
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SAMPLE COLLECTION SYSTEM
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CHEMICAL REACTIONS
CO2 AdsorptionCO2 + 2NaOH Na2CO3 + H2ONa2CO3 + CO2 + H2O 2NaHCO3
CO2 DesorptionNaHCO3 + HNO3 NaNO3 + H2CO3
H2CO3 H2O + CO2
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CHEMICAL REACTIONS
CombustionCH4 + 2O2 CO2 + 2H2O
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METHANE COMBUSTION EFFICIENCY 2 LPM
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Temperature F
Met
hane
Con
cent
ratio
n pp
mv
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CO2 ADSORPTION EFFICIENCY 1LPM
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Minutes
CO
2 C
once
ntra
tion
ppm
v
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14C LABORATORY DISTILLATION APPARATUS
Air Flow Inlet
To Vacuum
Condenser
Digestion Flask: Solid Sorbent
Tritium Trap (HCl)
CO2 trap
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VALIDATION OF SAMPLE ANALYSIS PROTOCOL
Method Blank0.042 pCi/L (4.2 x10-11 uCi/ml)Based on a 2 hour sample at 300 ml/min gas sample flow rate
LCS95.1 +/- 3% for spike equivalent to 2.0 pCi/L (2x10-9 uCi/ml) (total volume sampled=3.6 x104ml)
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VALIDATION OF SAMPLE COLLECTION AND ANALYSIS PROTOCOL
14C
14C
14C
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VALIDATION OF SAMPLE COLLECTION AND ANALYSIS PROTOCOL
71.71 99%71.71 97%71.71 92%71.71 94%71.71 95%71.71 91%71.71 96%71.71 96%71.71 98%71.71 91%
Average 95%
Nominal(pCi/sample)
LCS Recovery%
LCS(spiked into flask w/ascarite)
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VALIDATION OF SAMPLE COLLECTION AND ANALYSIS PROTOCOL
10486.49 83%10486.49 85%10486.49 82%
71.71 85%71.71 85%71.71 85%717.08 90%
Average 86%
Nominal(pCi/sample)
LCS Recovery%
Wet DigestionWet Digestion of standard to produce 14CO2
in sample gas stream
71.71 99%71.71 91%71.71 94%717.08 92%717.08 91%
Average 93%
Wet Digestion of standard followed by combustion to produce 14CO2 in sample gas
stream
Wet Digestion/Combustion
Nominal(pCi/sample)
LCS Recovery%
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SAMPLE COLLECTION HARDWARE
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SAMPLE COLLECTION HARDWARE
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EQUIPMENT AND SAMPLE SHIPPING
Sample box – limited quantity radioactive materialSample tubes – contain sodium hydroxide (a hazardous material), excepted quantity
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EQUIPMENT PERFORMANCE PARAMETERS
Carbon to CO2 Conversion Efficiency>95%CO2 Capture Efficiency>95%14C Measurement Range (to Date) <7x10-11 to 5x10-3 uCi/mlSample Rate (typical, other sample rates can be used) 0.1 - 3 liters per minutePower Requirements120V 20 ampSample Collection Interface uses an interface adaptor that can appropriately extract sample gas from plant systems under a wide range of plant gas flow and pressure conditions