Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 61, Issue 11, Pages -Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202117807
Keywords
Gas Separation; Krypton; Metal-Organic Frameworks; Self-Adjusting; Xenon
Categories
Funding
- Robert A. Welch Foundation [B-0027]
- US National Science Foundation [ECCS-2029800]
- National Natural Science Foundation of China [22001186]
- National Science Foundation of Jiangsu Province [BK20200853]
- National Science Foundation [DMR-1607989]
- Major Research Instrumentation Program [CHE-1531590]
- XSEDE Grant [TG-DMR090028]
- ACS Petroleum Research Fund grant [ACS PRF 56673-ND6]
- DOE-Office of Nuclear Energy
- Researchers Supporting Program at King Saud University, Riyadh, Saudi Arabia [RSP-2022/55]
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This study reports a self-adjusting metal-organic framework based on multiple weak binding interactions for capturing trace amounts of xenon and krypton from nuclear reprocessing off-gas. The self-adjusting behavior of ATC-Cu and its mechanism have been visualized and studied. The results show that ATC-Cu exhibits unprecedented high uptake capacities and record xenon capture capability from the nuclear reprocessing off-gas. This work not only provides a benchmark xenon adsorbent, but also proposes a new route for constructing smart materials for efficient separations.
The capture of the xenon and krypton from nuclear reprocessing off-gas is essential to the treatment of radioactive waste. Although various porous materials have been employed to capture Xe and Kr, the development of high-performance adsorbents capable of trapping Xe/Kr at very low partial pressure as in the nuclear reprocessing off-gas conditions remains challenging. Herein, we report a self-adjusting metal-organic framework based on multiple weak binding interactions to capture trace Xe and Kr from the nuclear reprocessing off-gas. The self-adjusting behavior of ATC-Cu and its mechanism have been visualized by the in-situ single-crystal X-ray diffraction studies and theoretical calculations. The self-adjusting behavior endows ATC-Cu unprecedented uptake capacities of 2.65 and 0.52 mmol g(-1) for Xe and Kr respectively at 0.1 bar and 298 K, as well as the record Xe capture capability from the nuclear reprocessing off-gas. Our work not only provides a benchmark Xe adsorbent but proposes a new route to construct smart materials for efficient separations.
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