Nuclear energy is among the most viable alternatives to our current fossil fuel-based energy economy. The mass deployment of nuclear energy as a low-emissions source requires the reprocessing of used nuclear fuel to recover fissile materials and mitigate radioactive waste. A major concern with reprocessing used nuclear fuel is the release of volatile radionuclides such as xenon and krypton that evolve into reprocessing facility off-gas in parts per million concentrations. The existing technology to remove these radioactive noble gases is a costly cryogenic distillation; alternatively, porous materials such as metal–organic frameworks have demonstrated the ability to selectively adsorb xenon and krypton at ambient conditions. Here we carry out a high-throughput computational screening of large databases of metal–organic frameworks and identify SBMOF-1 as the most selective for xenon. We affirm this prediction and report that SBMOF-1 exhibits by far the highest reported xenon adsorption capacity and a remarkable Xe/Kr selectivity under conditions pertinent to nuclear fuel reprocessing.
* S Supporting Information 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 appl...
A breathing 2-fold interpenetrated microporous metal-organic framework was synthesized with a flexible tetrahedral organic linker and Zn(2) clusters that sorb CO(2) preferably over N(2) and H(2).
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