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Direct synthesis of an aliphatic amine functionalized metal-organic framework for efficient CO2 removal and CH4 purification

Abstract

Porous materials bearing free aliphatic amine groups are powerful adsorbents for carbon dioxide but generally have to be synthesized by complicated, multi-step post-synthetic modification methods due to the high activity of these functional groups. We report a crystal-engineering strategy for such metal-organic frameworks. Reactions of Zn(II) ion with diversified coordination modes and bis(4-carboxy-benzyl)amine (H2bcba) with a secondary aliphatic amine bridge at different temperatures yielded a pair of isomeric frameworks with very similar framework structures but distinctly local structures, namely α-[Zn(bcba)] (MCF-51 or α-Zn) with all amino groups coordinated and β-[Zn(bcba)] (MCF-52 or β-Zn) with uncoordinated amino groups. Single-component gas adsorption and CO2/CH4 mixture breakthrough experiments at ambient conditions showed that, the CO2 adsorption ability and CH4 purification performances of β-Zn, in terms of CO2 adsorption enthalpy (42 kJ mol-1), CO2/CH4 selectivity (32) and CH4 purity/productivity (1.49 mmol g-1 at 99.999%+), are much higher than those of α-Zn (CO2 adsorption enthalpy of 17 kJ mol-1, CO2/CH4 selectivity of 2.9 and CH4 purity/productivity of 0.088 mmol g-1 at 99%+).

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Publication details

The article was received on 11 Apr 2018, accepted on 16 May 2018 and first published on 17 May 2018


Article type: Paper
DOI: 10.1039/C8CE00574E
Citation: CrystEngComm, 2018, Accepted Manuscript
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    Direct synthesis of an aliphatic amine functionalized metal-organic framework for efficient CO2 removal and CH4 purification

    N. Huang, Z. Mo, L. Li, W. Xu, H. Zhou, D. Zhou, P. Liao, J. Zhang and X. Chen, CrystEngComm, 2018, Accepted Manuscript , DOI: 10.1039/C8CE00574E

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