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Nat Mater

Title:		Trace removal of benzene vapour using double-walled metal-dipyrazolate frameworks
Author(s):		He T; Kong XJ; Bian ZX; Zhang YZ; Si GR; Xie LH; Wu XQ; Huang H; Chang Z; Bu XH; Zaworotko MJ; Nie ZR; Li JR;
Address:		"Beijing Key Laboratory for Green Catalysis and Separation and Department of Environmental Chemical Engineering, Beijing University of Technology, Beijing, China. The Key Laboratory of Advanced Functional Materials, Ministry of Education, Faculty of Materials and Manufacturing, Beijing University of Technology, Beijing, China. College of Chemistry and Chemical Engineering, Qingdao University, Shandong, China. Bernal Institute and Department of Chemical Sciences, University of Limerick, Limerick, Ireland. State Key Laboratory of Separation Membranes and Membrane Processes, Tianjin Polytechnic University, Tianjin, China. School of Materials Science and Engineering and TKL of Metal and Molecule-Based Material Chemistry, Nankai University, Tianjin, China. Bernal Institute and Department of Chemical Sciences, University of Limerick, Limerick, Ireland. xtal@ul.ie. The Key Laboratory of Advanced Functional Materials, Ministry of Education, Faculty of Materials and Manufacturing, Beijing University of Technology, Beijing, China. zrnie@bjut.edu.cn. Beijing Key Laboratory for Green Catalysis and Separation and Department of Environmental Chemical Engineering, Beijing University of Technology, Beijing, China. jrli@bjut.edu.cn. The Key Laboratory of Advanced Functional Materials, Ministry of Education, Faculty of Materials and Manufacturing, Beijing University of Technology, Beijing, China. jrli@bjut.edu.cn"
Journal Title:		Nat Mater
Year:		2022
Volume:		20220428
Issue:		6
Page Number:		689 - 695
DOI:		10.1038/s41563-022-01237-x
ISSN/ISBN:		1476-4660 (Electronic) 1476-1122 (Print) 1476-1122 (Linking)
Abstract:		"In principle, porous physisorbents are attractive candidates for the removal of volatile organic compounds such as benzene by virtue of their low energy for the capture and release of this pollutant. Unfortunately, many physisorbents exhibit weak sorbate-sorbent interactions, resulting in poor selectivity and low uptake when volatile organic compounds are present at trace concentrations. Herein, we report that a family of double-walled metal-dipyrazolate frameworks, BUT-53 to BUT-58, exhibit benzene uptakes at 298 K of 2.47-3.28 mmol g(-1) at <10 Pa. Breakthrough experiments revealed that BUT-55, a supramolecular isomer of the metal-organic framework Co(BDP) (H(2)BDP = 1,4-di(1H-pyrazol-4-yl)benzene), captures trace levels of benzene, producing an air stream with benzene content below acceptable limits. Furthermore, BUT-55 can be regenerated with mild heating. Insight into the performance of BUT-55 comes from the crystal structure of the benzene-loaded phase (C(6)H(6)@BUT-55) and density functional theory calculations, which reveal that C-H...X interactions drive the tight binding of benzene. Our results demonstrate that BUT-55 is a recyclable physisorbent that exhibits high affinity and adsorption capacity towards benzene, making it a candidate for environmental remediation of benzene-contaminated gas mixtures"
Keywords:		Adsorption Benzene/chemistry Gases *Metal-Organic Frameworks *Volatile Organic Compounds;
Notes:		"MedlineHe, Tao Kong, Xiang-Jing Bian, Zhen-Xing Zhang, Yong-Zheng Si, Guang-Rui Xie, Lin-Hua Wu, Xue-Qian Huang, Hongliang Chang, Ze Bu, Xian-He Zaworotko, Michael J Nie, Zuo-Ren Li, Jian-Rong eng Research Support, Non-U.S. Gov't England 2022/04/29 Nat Mater. 2022 Jun; 21(6):689-695. doi: 10.1038/s41563-022-01237-x. Epub 2022 Apr 28"