title: Polar group and defect engineering in a metal-organic framework: synergistic promotion of carbon dioxide sorption and conversion.
abstract: A sulfone-functionalized metal-organic framework (MOF), USTC-253, has been synthesized that exhibits a much higher CO2 uptake capacity (168-182 %) than the corresponding unfurnished MOFs. The introduction of trifluoroacetic acid (TFA) during the synthesis of USTC-253 affords defect-containing USTC-253-TFA with exposed metal centers, which has an increased CO2 uptake (167 %) compared to pristine USTC-253. USTC-253-TFA exhibits a very high ideal adsorption solution theory selectivity (S=75) to CO2 over N2 at 298 K. In addition, USTC-253-TFA demonstrates good catalytic activity and recyclability in the cycloaddition of CO2 and epoxide at room temperature under 1 bar CO2 pressure as a result of the presence of Lewis and Brønsted acid sites, which were evaluated by diffuse reflectance infrared Fourier transform spectroscopy with a CO probe molecule. We propose that the CO2 adsorption capability has a positive correlation with the catalytic performance toward CO2 conversion.
authors: Hefei National Laboratory for Physical Sciences at the Microscale, CAS Key Laboratory of Soft Matter Chemistry, Collaborative Innovation Center of Suzhou Nano Science and Technology, School of Chemistry and Materials Science, University of Science and Technology of China, Hefei, Anhui 230026 (P.R. China).
authors: Zhuo-Rui
authors: ZR
authors: Jiang
authors: Hengwei
authors: H
authors: Wang
authors: Yingli
authors: Y
authors: Hu
authors: Junling
authors: J
authors: Lu
authors: Hai-Long
authors: HL
authors: Jiang
mesh_terms: D000327:Adsorption; D002245:Carbon Dioxide / Q000737:chemistry*; D018360:Crystallography, X-Ray; D004852:Epoxy Compounds / Q000737:chemistry; D006863:Hydrogen-Ion Concentration; D008958:Models, Molecular; D008968:Molecular Conformation; D009942:Organometallic Compounds / Q000737:chemistry*
chemical_list: D004852:Epoxy Compounds; D009942:Organometallic Compounds; D002245:Carbon Dioxide; C009068:propylene oxide
keywords: CO2 capture; aluminum; cycloaddition; heterogeneous catalysis; metal-organic frameworks