Hydrogen bond unlocking-driven pore structure control for shifting multi-component gas separation function

Rong Yang, Yu Wang, Jian-Wei Cao, Zi-Ming Ye, Tony Pham, Katherine A. Forrest, Rajamani Krishna, Hongwei Chen, Libo Li, Bo-Kai Ling, Tao Zhang, Tong Gao, Xue Jiang, Xiang-Ou Xu, Qian-Hao Ye and Kai-Jie Chen ()
Additional contact information
Rong Yang: School of Chemistry and Chemical Engineering, Northwestern Polytechnical University
Yu Wang: School of Chemistry and Chemical Engineering, Northwestern Polytechnical University
Jian-Wei Cao: School of Chemistry and Chemical Engineering, Northwestern Polytechnical University
Zi-Ming Ye: Fujian Normal University
Tony Pham: University of South Florida
Katherine A. Forrest: University of South Florida
Rajamani Krishna: University of Amsterdam
Hongwei Chen: Taiyuan University of Technology
Libo Li: Taiyuan University of Technology
Bo-Kai Ling: School of Chemistry and Chemical Engineering, Northwestern Polytechnical University
Tao Zhang: School of Chemistry and Chemical Engineering, Northwestern Polytechnical University
Tong Gao: School of Chemistry and Chemical Engineering, Northwestern Polytechnical University
Xue Jiang: School of Chemistry and Chemical Engineering, Northwestern Polytechnical University
Xiang-Ou Xu: School of Chemistry and Chemical Engineering, Northwestern Polytechnical University
Qian-Hao Ye: School of Chemistry and Chemical Engineering, Northwestern Polytechnical University
Kai-Jie Chen: School of Chemistry and Chemical Engineering, Northwestern Polytechnical University

Nature Communications, 2024, vol. 15, issue 1, 1-8

Abstract: Abstract Purification of ethylene (C2H4) as the most extensive and output chemical, from complex multi-components is of great significance but highly challenging. Herein we demonstrate that precise pore structure tuning by controlling the network hydrogen bonds in two highly-related porous coordination networks can shift the efficient C2H4 separation function from C2H2/C2H4/C2H6 ternary mixture to CO2/C2H2/C2H4/C2H6 quaternary mixture system. Single-crystal X-ray diffraction revealed that the different amino groups on the triazolate ligands resulted in the change of the hydrogen bonding in the host network, which led to changes in the pore shape and pore chemistry. Gas adsorption isotherms, adsorption kinetics and gas-loaded crystal structure analysis indicated that the coordination network Zn-fa-atz (2) weakened the affinity for three C2 hydrocarbons synchronously including C2H4 but enhanced the CO2 adsorption due to the optimized CO2-host interaction and the faster CO2 diffusion, leading to effective C2H4 production from the CO2/C2H2/C2H4/C2H6 mixture in one step based on the experimental and simulated breakthrough data. Moreover, it can be shaped into spherical pellets with maintained porosity and separation performance.

Date: 2024
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DOI: 10.1038/s41467-024-45081-w

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