期刊
CHEMICAL ENGINEERING JOURNAL
卷 437, 期 -, 页码 -出版社
ELSEVIER SCIENCE SA
DOI: 10.1016/j.cej.2022.135363
关键词
Metal-organic frameworks; CO2 cycloaddition; Lewis acidity; Synergistic effect; Photocatalysis
资金
- National Key Research and Development Program of China [2020YFA0710301]
- National Natural Science Foundation of China [U1832145, 22172088, 51972195, 21832005, 21972078, 11374190]
- Shandong Province Natural Science Foundation [ZR2020YQ16]
- Young Scholars Program of Shandong University [2020QNQT012]
In this study, a boron-containing zirconium-based metal-organic framework was synthesized and found to exhibit synergistic effects of boron and light in enhancing the activity of CO2 cycloaddition. This provides a new strategy for designing efficient catalysts for CO2 capture and conversion under mild conditions.
Cycloaddition between CO2 and epoxides to produce cyclic carbonates is a promising approach to reach carbon neutralization. In this work, a boron-containing zirconium based metal-organic framework (UiO-67-B) pos-sessing the same topological structure with UiO-67 was prepared by replacing biphenyl-4,4'-dicarboxylic acid with 4'-borono-[1,1'-biphenyl]-4-carboxylic acid. UiO-67-B exhibits efficient activity towards the CO2 cycloaddition reaction under ambient conditions and light irradiation. Various characterizations suggest that the boron in UiO-67-B and light display synergistic effect on improving the activity. Specifically, (1) UiO-67-B displays extended light absorption; (2) UiO-67-B exhibits enhanced ligand to metal charge transfer (LMCT) process upon light irradiation; and (3) the presence of boron provides sites for the chemical adsorption and the subsequent activation of CO2, which avoids the competition with epoxide adsorption onto zirconium. This study illustrates the combination of boron and light in promoting the CO2 cycloaddition reaction, and provides a new strategy for designing efficient catalysts towards CO2 capture and conversion under mild conditions.
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