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Sibo Wang Wangshu Yao Jinliang Lin Zhengxin Ding Xinchen Wang 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2014,126(4):1052-1056
Metal–organic frameworks (MOFs) have shown great promise for CO2 capture and storage. However, the operation of chemical redox functions of framework substances and organic CO2‐trapping entities which are spatially linked together to catalyze CO2 conversion has had much less attention. Reported herein is a cobalt‐containing zeolitic imidazolate framework (Co‐ZIF‐9) which serves as a robust MOF cocatalyst to reduce CO2 by cooperating with a ruthenium‐based photosensitizer. The catalytic turnover number of Co‐ZIF‐9 was about 450 within 2.5 hours under mild reaction conditions, while still keeping its original reactivity during prolonged operation. 相似文献
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《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2017,129(48):15618-15622
The first thiocarboxylation of styrenes and acrylates with CO2 was realized by using visible light as a driving force and catalytic iron salts as promoters. A variety of important β‐thioacids were obtained in high yields. This multicomponent reaction proceeds in an atom‐ and redox‐economical manner with broad substrate scope under mild reaction conditions. Notably, high regio‐, chemo‐, and diasteroselectivity are observed. Mechanistic studies indicate that a radical pathway can account for the unusual regioselectivity. 相似文献
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《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2017,129(7):1916-1919
Herein we describe the first homogeneous non‐noble metal catalyst for the hydrogenation of CO2 to methanol. The catalyst is formed in situ from [Co(acac)3], Triphos, and HNTf2 and enables the reaction to be performed at 100 °C without a decrease in activity. Kinetic studies suggest an inner‐sphere mechanism, and in situ NMR and MS experiments reveal the formation of the active catalyst through slow removal of the acetylacetonate ligands. 相似文献
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《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2017,129(15):4251-4255
The hydrogenation of carbon dioxide involves the activation of the thermodynamically very stable molecule CO2 and formation of a C−H bond. Herein, we report that HCO2− and CO can be formed in the thermal reaction of CO2 with a diatomic metal hydride species, FeH−. The FeH− anions were produced by laser ablation, and the reaction with CO2 was analyzed by mass spectrometry and quantum‐chemical calculations. Gas‐phase HCO2− was observed directly as a product, and its formation was predicted to proceed by facile hydride transfer. The mechanism of CO2 hydrogenation in this gas‐phase study parallels similar behavior of a condensed‐phase iron catalyst. 相似文献