Abstract
Efficient separation of acetylene (C2H2) from its byproducts, especially CO2, is difficult because of their similar physicochemical properties, including molecular dimensions and boiling point. Herein, we demonstrate trace C2H2 removal from C2H2/CO2 mixtures enabled by a new ultramicroporous metal-organic framework (MOF) adsorbent, IPM-101, which features an optimal pore size of 4 Å (close to the kinetic diameter of C2H2, 3.3 Å) and one-dimensional channels lined by Lewis basic purine groups. Single-component gas adsorption isotherms revealed a clear affinity toward C2H2 versus CO2 at low pressures with a substantial C2H2 uptake of 0.9 mmol g-1 at 3000 ppm and 298 K. Dynamic column breakthrough experiments revealed separation of C2H2 from 1:1 and 1:99 v/v C2H2/CO2 mixtures. IPM-101 exhibits one of the highest dynamic separation selectivity (αAC) values yet reported, 22.5 for 1:1 C2H2/CO2. Computational simulations indicated that the purine moiety was key to the strong C2H2 selectivity thanks to C2H2 selective N···HCCH interactions.
Original language | English |
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Pages (from-to) | 5800–5808 |
Number of pages | 9 |
Journal | Chemistry of Materials |
Volume | 33 |
Issue number | 14 |
Early online date | 9 Jul 2021 |
DOIs | |
Publication status | Published - 27 Jul 2021 |
Bibliographical note
Funding Information:S.S. and G.K.D. acknowledge the Council of Scientific and Industrial Research (CSIR) for fellowship. A.V.D. and A.J. thank IISER Pune for funding. S.M. acknowledges the Alexander von Humboldt foundation for postdoctoral research fellowship. G.K.K. thanks the University of Bath. M.V. acknowledges the Irish Centre for High-End Computing (ICHEC) for the provision of computational facilities and support. M.J.Z. acknowledges the Science Foundation Ireland (awards 13/RP/B2549 and 16/IA/4624) and the European Research Council under the European Union’s H2020 research and innovation programme (grant agreement ADG 885695). S.K.G. thanks the SERB India for project funding (Grant No. CRG/2019/000906).
Funding
S.S. and G.K.D. acknowledge the Council of Scientific and Industrial Research (CSIR) for fellowship. A.V.D. and A.J. thank IISER Pune for funding. S.M. acknowledges the Alexander von Humboldt foundation for postdoctoral research fellowship. G.K.K. thanks the University of Bath. M.V. acknowledges the Irish Centre for High-End Computing (ICHEC) for the provision of computational facilities and support. M.J.Z. acknowledges the Science Foundation Ireland (awards 13/RP/B2549 and 16/IA/4624) and the European Research Council under the European Union’s H2020 research and innovation programme (grant agreement ADG 885695). S.K.G. thanks the SERB India for project funding (Grant No. CRG/2019/000906).
ASJC Scopus subject areas
- General Chemistry
- General Chemical Engineering
- Materials Chemistry