CO2 hydrogenation to formate catalyzed by highly stable and recyclable carbene-iridium under mild condition

被引:21
作者
Zhou, Lei [1 ]
Yao, Chenfei [1 ]
Ma, Wentao [1 ]
Hu, Jinling [1 ]
Wu, Youting [1 ]
Zhang, Zhibing [1 ]
Hu, Xingbang [1 ]
机构
[1] Nanjing Univ, Sch Chem & Chem Engn, Nanjing 210093, Peoples R China
基金
中国国家自然科学基金;
关键词
Carbon dioxide; Hydrogenation; Cyclic (alkyl)(amino)carbenes iridium; Metal-hydride; Formate; CARBON-DIOXIDE HYDROGENATION; DEFINED IRON CATALYST; FORMIC-ACID; COMPLEXES; REDUCTION; METHANOL; COBALT; ACTIVATION; RHODIUM; NANOPARTICLES;
D O I
10.1016/j.jcou.2021.101769
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
The catalytic reactivity of the metal center to H2 and the stability of the metal-hydride intermediate are vital for enhancing the CO2 hydrogenation efficiency. It was found that polymerization can bring a highly hydrophobic and stable 1,5-cyclooctadiene-iridium(I) chloride anchored on polymerized cyclic (alkyl)(amino)carbenes (PCAAC-Ir), which can protect the reactive Ir-H intermediates and the catalyst itself. Above properties makes the PCAAC-Ir superior to the un-polymerized one for the CO2 hydrogenation to formate. Up to 195,600 TON can be achieved, being 38.7 times higher than that of the un-polymerized CAAC-Ir. Besides, the CO2 hydrogenation catalyzed by P-CAAC-Ir performs quite well in water, whereas that catalysed by un-polymerized CAAC-Ir does work under the same condition. In addition, the polymerized catalyst can be easily recycled without significant loss of activity.
引用
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页数:6
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