Journal
ACS APPLIED NANO MATERIALS
Volume 3, Issue 3, Pages 2911-2919Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsanm.0c00162
Keywords
metal-organic frameworks; C2H2 separation and purification; C2H2/CO2 separation; gas separation; N-oxide
Funding
- National Natural Science Foundation of China [21771162, 21922810]
- Natural Science Foundation of Zhejiang Province, China [LR16B010001, LY17B060001]
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The development of porous metal-organic framework (MOF) solids displaying efficient separation and purification of acetylene is of cardinal significance but challenging in the chemical industry. Among the reported MOFs for such a purpose, there usually exists an issue associated with trade-off between the uptake capacity and adsorption selectivity. In this work, we employed an N-oxide-functionalized dicarboxylate ligand to successfully construct under suitable solvothermal conditions a dicopper paddlewheel-based MOF featuring two different types of nanocages and rich open oxygen atoms on the channel surface. These structural features endow the material with the promising potential for C2H2 recovery from CO2 and CH4 at ambient conditions with impressive adsorption selectivity of C2H2 over CO2 and CH4 as well as considerable C2H2 capture capacity, which have been validated by isotherm measurements, ideal adsorbed solution theory calculations, and breakthrough experiments. Furthermore, molecular modeling studies revealed the vital role that the oxygen atoms coming from both N-oxide moieties and carboxylate groups play in selectively recognizing C2H2 over CO2 and CH4.
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