Development and Testing of a Prototype Modular Tritium and Carbon-14 Gas Environmental Monitoring System

Hilary Phillips, Marc Parisot2, Julian Dean1, Lauren Perrie1 and John Sephton1
1

National Physical Laboratory, Teddington, United Kingdom 2 Grenoble INP-Phelma email: hilary.phillips@npl.co.uk

Abstract:
Increasing quantities of radioactive waste are being placed into storage facilities. Many of the waste products contain organic materials which may undergo degradation leading to the release of tritium and carbon-14 species into waste containers and potentially into the environment. Monitoring for radioactive gas release is required for environmental regulatory compliance and for radiation protection of facility workers. Research is currently being undertaken at NPL as part of the EMRP MetroRWM project to improve and automate environmental sampling equipment for tritium and carbon-14 species. An innovative modular system is being developed which will lead to the introduction of an on-site small scale system capable of gas collection, liquid scintillation sample preparation and measurement. This paper outlines the evaluation of the liquid scintillation system that has been performed to date using radioactive spiked samples of trapping medium of activity concentration similar to that envisaged in service. An initial prototype of the AERGMS was constructed and the feasibility of the design demonstrated. A revised modular prototype is under construction for field trial evaluation. The Automated Environmental Radioactive Gas Measurement System (AERGMS) will consist of:  A time-integrating gas-in-air sampling module based on gas bubbler technology  Automated modules for fluid handling and sample preparation  A Liquid scintillation counting module (NE LSC2 based)  Automatic data transferal to a remote control centre The NE LSC2 counter is a dual photomultiplier tube (PMT), dual measurement channel liquid scintillation counter. The NE LSC2 counter is operated using dead time units and scalars for each of the PMTs and a PC for data acquisition. The operating voltage (900V) is supplied by a dedicated power supply.

Evaluation of scintillant performed and Optiphase HiSafe 3 identified as suitable. (High flash point. Compatible with alkaline samples necessary for 14CO2 stability)

Initially single trapping medium for CO2 and HTO envisaged but preliminary tests have indicated that separate media will be required. Testing is on-going.

Evaluation trials of NE LC2 performance have indicated that chemiluminescence (a phenomenon that occurs when a chemical reaction occurs between the sample and the fluor molecules in the scintillation cocktail) and quench will effected the measurements performed using the AERGMS. Three methods of minimizing chemiluminescence have been considered; increasing the lower measurement channel threshold to prevent luminescence count detection; addition of a delayed coincidence counting circuit to enable removal of the chemiluminescence count rate or the Quench has caused the 14C response in the NE LSC2 counter to occur in the tritium channel (A). 14C activity will be determined in channel B, and the count rate from 14C in channel A estimated based on trials using standard AERGMS operating conditions. Correction of the total counts in channel A will enable determination of the 3H count rate present. The activity concentration of 3H and 14C species in the sampled air stream will be derived from these count rates using the volume of air sampled during gas trapping.
Nuclide NE LSC2 Efficiency Unquenched
3

introduction of a measurement delay time. A delay will be introduced between sample preparation and mixing in the AERGMS to enable the decay of spurious luminescence pulses. Tritium and carbon-14 liquid scinitillation vials containing sodium hydroxide exhibited a significant reduction in detected count rate when measured on both the NE LSC2 and commercial counters due to quench. Whilst the level of quench in a scintillation sample is evaluated using the tSIE index in commercial liquid scintillation counters, no method is available for the NE LSC2 counter.

Quenched 30% 87%

Queens Printer and Controller of HMSO, 2013. 10673/1013

H C

50% 70%

14

Future work will include generation of low level standards of 14C and 3H at NPL, which will be used for controlled active testing of the system. This will be performed using the NPL HTO conversion rig to generate HT gas from tritiated water, and the NPL 14C conversion rig to generate 14C02 from a sodium bicarbonate solution. These gases will be standardised by internal gas proportional counting, transferred to cylinders and pressurised with diluent gas to achieve the required activity concentrations, comparable to those expected to be measured by the AERGMS.

Acknowledgments
The authors gratefully acknowledge funding provided by the National Measurement Office of the United Kingdom Department for Business, Innovation and Skills, through the Acoustics and Ionising Radiation Metrology Programme. This work is supported by the European Metrology Research Programme (EMRP). The EMRP is jointly funded by the EMRP participating countries within EURAMET and the European Union.

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