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タイトル: | Benchmark Acetylene Binding Affinity and Separation through Induced Fit in a Flexible Hybrid Ultramicroporous Material |
著者: | Shivanna, Mohana Otake, Ken‐ichi Song, Bai‐Qiao Wyk, Lisa M. Yang, Qing‐Yuan Kumar, Naveen Feldmann, Wesley K. Pham, Tony Suepaul, Shanelle Space, Brian Barbour, Leonard J. Kitagawa, Susumu https://orcid.org/0000-0001-6956-9543 (unconfirmed) Zaworotko, Michael J. |
著者名の別形: | 大竹, 研一 北川, 進 |
キーワード: | coordination polymers C₂H₂/C₂H₄ and C₂H₂/CO₂ separation induced fit mechanism physisorption ultramicroporous materials |
発行日: | 6-Sep-2021 |
出版者: | Wiley |
誌名: | Angewandte Chemie International Edition |
巻: | 60 |
号: | 37 |
開始ページ: | 20383 |
終了ページ: | 20390 |
抄録: | Structural changes at the active site of an enzyme induced by binding to a substrate molecule can result in enhanced activity in biological systems. Herein, we report that the new hybrid ultramicroporous material sql-SIFSIX-bpe-Zn exhibits an induced fit binding mechanism when exposed to acetylene, C₂H₂. The resulting phase change affords exceptionally strong C₂H₂ binding that in turn enables highly selective C₂H₂/C₂H₄ and C₂H₂/CO₂ separation demonstrated by dynamic breakthrough experiments. sql-SIFSIX-bpe-Zn was observed to exhibit at least four phases: as-synthesised (α); activated (β); and C₂H₂ induced phases (β' and γ). sql-SIFSIX-bpe-Zn-β exhibited strong affinity for C₂H₂ at ambient conditions as demonstrated by benchmark isosteric heat of adsorption (Qst ) of 67.5 kJ mol⁻¹ validated through in situ pressure gradient differential scanning calorimetry (PG-DSC). Further, in situ characterisation and DFT calculations provide insight into the mechanism of the C₂H₂ induced fit transformation, binding positions and the nature of host-guest and guest-guest interactions. |
著作権等: | © 2021 The Authors. Angewandte Chemie International Edition published by Wiley-VCH GmbH This is an open access article under the terms of the Creative Commons Attribution-NonCommercial-NoDerivs License, which permits use and distribution in any medium, provided the original work is properly cited, the use is non-commercial and no modifications or adaptations are made. |
URI: | http://hdl.handle.net/2433/275723 |
DOI(出版社版): | 10.1002/anie.202106263 |
PubMed ID: | 34250717 |
出現コレクション: | 学術雑誌掲載論文等 |
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