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Issue 6, 2018
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Enhancing light hydrocarbon storage and separation through introducing Lewis basic nitrogen sites within a carboxylate-decorated copper–organic framework

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Abstract

A novel nanoporous Cu metal–organic framework (NEM-4) with open CuII sites, Lewis basic nitrogen sites, and uncoordinated –COO groups exhibits both outstanding uptake capacities (in cm3 (STP) g−1) for C2H2 (204), C2H4 (164.1), C2H6 (172.2), C3H6 (197.4), and C3H8 (196.1) and high selectivities for C2H2/CH4 (63.2), C3H6/CH4 (174.8), and C3H8/CH4 (168.3) under ambient conditions. After eight cycles of adsorption–desorption tests, only 8.2% and 10.3% decrease in the acetylene and propene storage capacities was observed, indicating an excellent repeatability. Compared with 1 (carboxylate decorated NOTT-101), when nitrogen sites are inserted, the C2–C3 hydrocarbon uptakes of NEM-4 can be significantly enhanced. Grand Canonical Monte Carlo and first-principles calculations reveal that not only the open CuII sites but also the uncoordinated –COO groups and the nitrogen sites play significant roles in its high C2–C3 hydrocarbon uptakes. Moreover, the adsorption and separation of cationic dyes in NEM-4 are highly size and charge state dependent, and the adsorbed methylene blue (MB+) in NEM-4 can be efficiently released in an NaCl-containing CH3OH solution. This study reveals that the combination of open metal sites, carboxylate groups, Lewis basic pyridyl sites, and appropriate pore geometry is responsible for the high adsorption/separation of light hydrocarbons in NEM-4.

Graphical abstract: Enhancing light hydrocarbon storage and separation through introducing Lewis basic nitrogen sites within a carboxylate-decorated copper–organic framework

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Publication details

The article was received on 14 Mar 2018, accepted on 02 Apr 2018 and first published on 09 Apr 2018


Article type: Research Article
DOI: 10.1039/C8QM00105G
Citation: Mater. Chem. Front., 2018,2, 1146-1154
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    Enhancing light hydrocarbon storage and separation through introducing Lewis basic nitrogen sites within a carboxylate-decorated copper–organic framework

    X. Liu, W. Fan, M. Zhang, G. Li, H. Liu, D. Sun, L. Zhao, H. Zhu and W. Guo, Mater. Chem. Front., 2018, 2, 1146
    DOI: 10.1039/C8QM00105G

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