期刊
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
卷 141, 期 1, 页码 138-142出版社
AMER CHEMICAL SOC
DOI: 10.1021/jacs.8b12138
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资金
- National Natural Science Foundation of China [21602237, 21732007, 21890721, 21821002]
- Program of Shanghai Academic Research Leader
- Strategic Priority Research Program of the Chinese Academy of Sciences [XDB20000000]
- Fujian Institute of Innovation, Chinese Academy of Sciences
- Chinese Academy of Sciences President's International Fellowship Initiative
Redistribution of primary silanes through C-Si and Si-H bond cleavage and reformation provides a straightforward synthesis of secondary silanes, but the poor selectivity and low efficiency severely hinders the application of this synthetic protocol. Here, we show that a newly synthesized divalent ytterbium alkyl complex exhibits unprecedentedly high catalytic activity toward the selective redistribution of primary arylsilanes to secondary arylsilanes. More significantly, this complex also effectively catalyzes the cross-coupling between electron-withdrawing substituted primary arylsilanes and electron-donating substituted primary arylsilanes to secondary arylsilanes containing two different aryls. DFT calculation indicates that the reaction always involve the exothermic formation of a hypervalent silicon upon facile addition of PhSiH3 to the Yb-E (E = C, H) bond. This hypervalent compound can easily either generate directly the Yb-Ph complex, or indirectly through the formation of Yb-H, that is the key complex for the formation of Ph2SiH2.
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