title: Potential of metal-organic frameworks for separation of xenon and krypton.
abstract: CONSPECTUS: The total world energy demand is predicted to rise significantly over the next few decades, primarily driven by the continuous growth of the developing world. With rapid depletion of nonrenewable traditional fossil fuels, which currently account for almost 86% of the worldwide energy output, the search for viable alternative energy resources is becoming more important from a national security and economic development standpoint. Nuclear energy, an emission-free, high-energy-density source produced by means of controlled nuclear fission, is often considered as a clean, affordable alternative to fossil fuel. However, the successful installation of an efficient and economically viable industrial-scale process to properly sequester and mitigate the nuclear-fission-related, highly radioactive waste (e.g., used nuclear fuel (UNF)) is a prerequisite for any further development of nuclear energy in the near future. Reprocessing of UNF is often considered to be a logical way to minimize the volume of high-level radioactive waste, though the generation of volatile radionuclides during reprocessing raises a significant engineering challenge for its successful implementation. The volatile radionuclides include but are not limited to noble gases (predominately isotopes of Xe and Kr) and must be captured during the process to avoid being released into the environment. Currently, energy-intensive cryogenic distillation is the primary means to capture and separate radioactive noble gas isotopes during UNF reprocessing. A similar cryogenic process is implemented during commercial production of noble gases though removal from air. In light of their high commercial values, particularly in lighting and medical industries, and associated high production costs, alternate approaches for Xe/Kr capture and storage are of contemporary research interest. The proposed pathways for Xe/Kr removal and capture can essentially be divided in two categories: selective absorption by dissolution in solvents and physisorption on porous materials. Physisorption-based separation and adsorption on highly functional porous materials are promising alternatives to the energy-intensive cryogenic distillation process, where the adsorbents are characterized by high surface areas and thus high removal capacities and often can be chemically fine-tuned to enhance the adsorbate-adsorbent interactions for optimum selectivity. Several traditional porous adsorbents such as zeolites and activated carbon have been tested for noble gas capture but have shown low capacity, selectivity, and lack of modularity. Metal-organic frameworks (MOFs) or porous coordination polymers (PCPs) are an emerging class of solid-state adsorbents that can be tailor-made for applications ranging from gas adsorption and separation to catalysis and sensing. Herein we give a concise summary of the background and development of Xe/Kr separation technologies with a focus on UNF reprocessing and the prospects of MOF-based adsorbents for that particular application.
authors.affiliation: Fundamental & Computational Sciences Directorate, Pacific Northwest National Laboratory , Richland, Washington 99352, United States.
authors.forename: Debasis
authors.initials: D
authors.lastname: Banerjee
authors.forename: Amy J
authors.initials: AJ
authors.lastname: Cairns
authors.forename: Jian
authors.initials: J
authors.lastname: Liu
authors.forename: Radha K
authors.initials: RK
authors.lastname: Motkuri
authors.forename: Satish K
authors.initials: SK
authors.lastname: Nune
authors.forename: Carlos A
authors.initials: CA
authors.lastname: Fernandez
authors.forename: Rajamani
authors.initials: R
authors.lastname: Krishna
authors.forename: Denis M
authors.initials: DM
authors.lastname: Strachan
authors.forename: Praveen K
authors.initials: PK
authors.lastname: Thallapally