期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 58, 期 2, 页码 577-581出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201811506
关键词
carbon dioxide fixation; cyclizations; heterogeneous catalysis; metal-organic frameworks (MOFs); noble-metal-free
资金
- NSFC [21625103, 21571107, 21421001]
- 111 project [B12015]
Cyclization of propargylic alcohols with CO2 is an important reaction in industry, and noble-metal catalysts are often employed to ensure the high product yields under environmentally friendly conditions. Herein a porous noble-metal-free framework 1 with large 1D channels of 1.66 nm diameter was synthesized for this reaction. Compound 1 exhibits excellent acid/base stability, and is even stable in corrosive triethylamine for one month. Catalytic studies indicate that 1 is an effective catalyst for the cyclization of propargylic alcohols and CO2 without any solvents under mild conditions, and the turnover number (TON) can reach to a record value of 14 400. Furthermore, this MOF catalyst also has rarely seen catalytic activity when the biological macromolecule ethisterone was used as a substrate. Mechanistic studies reveal that the synergistic catalytic effect between Cu-I and In-III plays a key role in the conversion of CO2.
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