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Title: Metal–organic framework with optimally selective xenon adsorption and separation

Abstract

Nuclear energy is considered among the most viable alternatives to our current fossil fuel based energy economy.1 The mass-deployment of nuclear energy as an emissions-free source requires the reprocessing of used nuclear fuel to mitigate the waste.2 One of the major concerns with reprocessing used nuclear fuel is the release of volatile radionuclides such as Xe and Kr. The most mature process for removing these radionuclides is energy- and capital-intensive cryogenic distillation. Alternatively, porous materials such as metal-organic frameworks (MOFs) have demonstrated the ability to selectively adsorb Xe and Kr at ambient conditions.3-8 High-throughput computational screening of large databases of porous materials has identified a calcium-based nanoporous MOF, SBMOF-1, as the most selective for Xe over Kr.9,10 Here, we affirm this prediction and report that SBMOF-1 exhibits by far the highest Xe adsorption capacity and a remarkable Xe/Kr selectivity under relevant nuclear reprocessing conditions. The exceptional selectivity of SBMOF-1 is attributed to its pore size tailored to Xe and its dense wall of atoms that constructs a binding site with a high affinity for Xe, as evident by single crystal X-ray diffraction and molecular simulation.

Authors:
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Publication Date:
Research Org.:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Brookhaven National Laboratory (BNL), Upton, NY (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); USDOE Office of Science (SC), Workforce Development for Teachers and Scientists (WDTS) (SC-27); National Science Foundation (NSF)
OSTI Identifier:
1340382
Alternate Identifier(s):
OSTI ID: 1290365; OSTI ID: 1379396
Report Number(s):
PNNL-SA-116761; BNL-112568-2016-JA
Journal ID: ISSN 2041-1723; AF5805020
Grant/Contract Number:
AC05-76RL01830; SC0012704; SC0001015; AC05-06OR23100; AC02-05CH11231; DMR-1231586; CHE-0840483
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 7; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
Xenon; Krypton; MOFs; 36 MATERIALS SCIENCE; 11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Inorganic chemistry; Metal-organic frameworks

Citation Formats

Banerjee, Debasis, Simon, Cory M., Plonka, Anna M., Motkuri, Radha K., Liu, Jian, Chen, Xianyin, Smit, Berend, Parise, John B., Haranczyk, Maciej, and Thallapally, Praveen K. Metal–organic framework with optimally selective xenon adsorption and separation. United States: N. p., 2016. Web. doi:10.1038/ncomms11831.
Banerjee, Debasis, Simon, Cory M., Plonka, Anna M., Motkuri, Radha K., Liu, Jian, Chen, Xianyin, Smit, Berend, Parise, John B., Haranczyk, Maciej, & Thallapally, Praveen K. Metal–organic framework with optimally selective xenon adsorption and separation. United States. doi:10.1038/ncomms11831.
Banerjee, Debasis, Simon, Cory M., Plonka, Anna M., Motkuri, Radha K., Liu, Jian, Chen, Xianyin, Smit, Berend, Parise, John B., Haranczyk, Maciej, and Thallapally, Praveen K. Mon . "Metal–organic framework with optimally selective xenon adsorption and separation". United States. doi:10.1038/ncomms11831. https://www.osti.gov/servlets/purl/1340382.
@article{osti_1340382,
title = {Metal–organic framework with optimally selective xenon adsorption and separation},
author = {Banerjee, Debasis and Simon, Cory M. and Plonka, Anna M. and Motkuri, Radha K. and Liu, Jian and Chen, Xianyin and Smit, Berend and Parise, John B. and Haranczyk, Maciej and Thallapally, Praveen K.},
abstractNote = {Nuclear energy is considered among the most viable alternatives to our current fossil fuel based energy economy.1 The mass-deployment of nuclear energy as an emissions-free source requires the reprocessing of used nuclear fuel to mitigate the waste.2 One of the major concerns with reprocessing used nuclear fuel is the release of volatile radionuclides such as Xe and Kr. The most mature process for removing these radionuclides is energy- and capital-intensive cryogenic distillation. Alternatively, porous materials such as metal-organic frameworks (MOFs) have demonstrated the ability to selectively adsorb Xe and Kr at ambient conditions.3-8 High-throughput computational screening of large databases of porous materials has identified a calcium-based nanoporous MOF, SBMOF-1, as the most selective for Xe over Kr.9,10 Here, we affirm this prediction and report that SBMOF-1 exhibits by far the highest Xe adsorption capacity and a remarkable Xe/Kr selectivity under relevant nuclear reprocessing conditions. The exceptional selectivity of SBMOF-1 is attributed to its pore size tailored to Xe and its dense wall of atoms that constructs a binding site with a high affinity for Xe, as evident by single crystal X-ray diffraction and molecular simulation.},
doi = {10.1038/ncomms11831},
journal = {Nature Communications},
number = ,
volume = 7,
place = {United States},
year = {Mon Jun 13 00:00:00 EDT 2016},
month = {Mon Jun 13 00:00:00 EDT 2016}
}

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  • Nuclear energy is considered among the most viable alternatives to our current fossil fuel based energy economy.1 The mass-deployment of nuclear energy as an emissions-free source requires the reprocessing of used nuclear fuel to mitigate the waste.2 One of the major concerns with reprocessing used nuclear fuel is the release of volatile radionuclides such as Xe and Kr. The most mature process for removing these radionuclides is energy- and capital-intensive cryogenic distillation. Alternatively, porous materials such as metal-organic frameworks (MOFs) have demonstrated the ability to selectively adsorb Xe and Kr at ambient conditions.3-8 High-throughput computational screening of large databases ofmore » porous materials has identified a calcium-based nanoporous MOF, SBMOF-1, as the most selective for Xe over Kr.9,10 Here, we affirm this prediction and report that SBMOF-1 exhibits by far the highest Xe adsorption capacity and a remarkable Xe/Kr selectivity under relevant nuclear reprocessing conditions. The exceptional selectivity of SBMOF-1 is attributed to its pore size tailored to Xe and its dense wall of atoms that constructs a binding site with a high affinity for Xe, as evident by single crystal X-ray diffraction and molecular simulation.« less
  • 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 andmore » 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.« less
  • A three-dimensional triply interpenetrated mixed metal-organic framework, Zn{sub 2}(BBA){sub 2}(CuPyen) {center_dot} G{sub x} (M'MOF-20; BBA = biphenyl-4,4'-dicarboxylate; G = guest solvent molecules), of primitive cubic net was obtained through the solvothermal reaction of Zn(NO{sub 3}){sub 2}, biphenyl-4,4'-dicarboxylic acid, and the salen precursor Cu(PyenH{sub 2})(NO{sub 3}){sub 2} by a metallo-ligand approach. The triple framework interpenetration has stabilized the framework in which the activated M'MOF-20a displays type-I N{sub 2} gas sorption behavior with a Langmuir surface area of 62 m{sup 2} g{sup -1}. The narrow pores of about 3.9 {angstrom} and the open metal sites on the pore surfaces within M'MOF-20a collaborativelymore » induce its highly selective C{sub 2}H{sub 2}/CH{sub 4} and CO{sub 2}/CH{sub 4} gas separation at ambient temperature.« less