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Trace removal of benzene vapour using double-walled metal–dipyrazolate frameworks

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journal contribution
posted on 2023-10-25, 13:28 authored by Tao He, Xiang-Jing KongXiang-Jing Kong, Zhen-Xing Bian, Yong-Zheng Zhang, Guang-Rui Si, Lin-Hua Xie, Xue-Qian Wu, Hongliang Huang, Ze Chang, Xian-He Bu, Michael ZaworotkoMichael Zaworotko, Zuo-Ren Nie, Jian Rong Li

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) (H2BDP = 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 (C6H6@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.

Funding

Ecological environment materials and preparation engineering

National Natural Science Foundation of China

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Green Adsorbents for Clean Energy (GrACE)

Science Foundation Ireland

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SYNergistic SORBents

European Research Council

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History

Publication

Nature Materials, 2022, 21,pp. 689–695

Publisher

Springer Nature

Other Funding information

J.-R.L. acknowledges support by the National Natural Science Foundation of China (22038001). J.-R.L. and Z.-R.N. acknowledge support by the National Natural Science Foundation of China (51621003). M.J.Z. acknowledges support from Science Foundation Ireland (16/IA/4624) and the European Research Council (ADG 885695). T.H. acknowledges support by the Postdoctoral Science Foundation of Chaoyang District (2020ZZ-8). We also thank Q. Chen, X. Lin, T.-C. Li and L. Tang from Beijing University of Technology and N. Kumar from the University of Limerick for their assistance with in situ PXRD and GC–MS measurements.

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  • Bernal Institute

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  • (4) Quality Education

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  • Chemical Sciences

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