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Synthesis of cobalt single atom catalyst by a solid-state transformation strategy for direct c-c cross-coupling of primary and secondary alcohols

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Nano Research 2022年第5期15卷 4023-4031页

作者： Zhijun Li Yuying chen Xiaowen Lu Honghong Li Leipeng Leng Tinglei zhang JHugh Horton Joint International Research Laboratory of Advanced chemical catalytic Materials&Surface Science College of Chemistry and Chemical EngineeringNortheast Petroleum UniversityDaqing 163318China Department of chemistry Queen’s UniversityKingston K7L 3N6Canada

Atomic engineering of single atom catalysts(SAcs)with high-density available active sites and optimized electronic properties can substantially boost catalytic ***,we report a solid-state transformation strategy to access co SAcs by introducing co species from commercial cO_(2)O3 powders into nitrogen-doped carbon *** catalyst exhibited excellent catalytic activity,with a turnover frequency(TOF)of 2,307 h^(-1)and yield of 95%,in the direct c-c cross-coupling of benzyl alcohol and 1-phenylethanol(1 atm O2@80℃)to yield *** functional theory(DFT)calculations demonstrate the coordination environment and electronic metal-support interaction impact the catalytic *** particular,a wide substrate scope and a broad functional-group tolerance of this SAc were validated,and the employment of this strategy for large-scale synthesis was also shown to be *** work might shed light on the facile and scalable synthesis of highly active,selective,and stable SAcs for heterogeneous catalysis.

关键词： single atom catalysis solid-state transformation c-c cross-coupling a,β-unsaturated ketones catalytic activity

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cooperation of SET and cMD mechanisms of cobalt-catalyzed dual c-H activation and cross-coupling reactions: A DFT study

Cooperation of SET and CMD mechanisms of cobalt-catalyzed du...

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第十三届全国量子化学会议

作者： Xue Li Donghui Wei Zhongjun Li The college of chemistry and Molecular Engineering Center of Computational ChemistryZhengzhou University

Almost all the co-catalyzed c-H functionalizations have been achieved based on either single electron transfer(SET) or the concerted-metalation deprotonation(cMD) mechanism.[1-2] Recently, Du et al. reporeted the novel cobalt-catalyzed c-H activation cross-coupling reaction between two aromatic rings by using different directing groups.[3] Interestingly, both SET and cMD mechanism would be invloved in this kind of dual c-H activations, which is remarkably different from the previous references.[1-2]Herein, we first investigate the detailed mechanism of the co-catalyzed c-H/c-H activation/arylation reaction between the 8-aminoquinoline amide and 2-phenylpyridine at the M06-L/6-31G(d,p)//LanL2DZ level. The calculated results indicated that the whole catalytic reaction contains two stages: c-H/c-H activations and c-c *** two c-H activations were proceeding via the SET and cMD mechanisms,respectively. The rate-determining step of entire reaction is the c-c bond formation rather than the c-H activations, which is well consistent with the kinetic experiments.[3]The mechanistic insights obtained in the present study should be useful for understanding the novel metal-catalyzed c-H activation/arylation, and thus provide valuable clues on rational design of efficient metal catalysts for the metal-catalyzed cross-coupling reactions.

关键词： c-H activation c-c cross-coupling cobalt catalysis SET/cMD mechanism

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