Separation of tritiated water using graphene oxide membrane

Sevigny, Gary J.¹  Motkuri, Radha K.¹  Gotthold, David W.¹  Fifield, Leonard S.¹  Frost, Anthony P.¹  Bratton, Wesley¹ 

[1] Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

关键词: tritium;    membrane;    separation;    graphene oxide;   

DOI  :  10.2172/1222908
RP-ID  :  PNNL--24411
PID  :  OSTI ID: 1222908
Others  :  Other: AF5805010

美国|英语

来源: SciTech Connect

【 摘 要 】

In future nuclear fuel reprocessing plants and possibly for nuclear power plants, the cleanup of tritiated water will be needed for hundreds of thousands of gallons of water with low activities of tritium. This cleanup concept utilizes graphene oxide laminar membranes (GOx) for the separation of low-concentration (10-3-10 ??Ci/g) tritiated water to create water that can be released to the environment and a much smaller waste stream with higher tritium concentrations. Graphene oxide membranes consist of hierarchically stacked, overlapping molecular layers and represent a new class of materials. A permeation rate test was performed with a 2-??m-thick cast Asbury membrane using mixed gas permeability testing with zero air (highly purified atmosphere) and with air humidified with either H2O or D2O to a nominal 50% relative humidity. The membrane permeability for both H2O and D2O was high with N2 and O2 at the system measurement limit. The membrane water permeation rate was compared to a Nafion?? membrane and the GOx permeation was approximately twice as high at room temperature. The H2O vapor permeation rate was 5.9 ?? 102 cc/m2/min (1.2 ?? 10-6 g/min-cm2), which is typical for graphene oxide membranes. To demonstrate the feasibility of such isotopic water separation through GOX laminar membranes, an experimental setup was constructed to use pressure-driven separation by heating the isotopic water mixture at one side of the membrane to create steam while cooling the other side. Several membranes were tested and were prepared using different starting materials and by different pretreatment methods. The average separation result was 0.8 for deuterium and 0.6 for tritium. Higher or lower temperatures may also improve separation efficiency but neither has been tested yet. A rough estimate of cost compared to current technology was also included as an indication of potential viability of the process. The relative process costs were based on the rough size of facility to accommodate the large surface area of the membranes and the energy needed to evaporate the water and pass through the membranes as compared to the currently used combined electrolysis and catalytic exchange process.