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Atomic engineering of single atom catalysts (SACs) with high-density available active sites and optimized electronic properties can substantially boost catalytic efficacy. Herein, we report a solid-state transformation strategy to access Co SACs by introducing Co species from commercial Co2O3 powders into nitrogen-doped carbon support. The 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 °C) to yield chalcone. Density functional theory (DFT) calculations demonstrate the coordination environment and electronic metal–support interaction impact the catalytic pathway. In 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 feasible. This work might shed light on the facile and scalable synthesis of highly active, selective, and stable SACs for heterogeneous catalysis.
This work was supported by the China Postdoctoral Science Foundation (Nos. 2019M661247 and 2020T130091), Postdoctoral Science Foundation of Heilongjiang Province (No. LBH-Z19047), Scientific Research Foundation for Returned Scholars of Heilongjiang Province of China (No. 719900091), and Heilongjiang Touyan Innovation Team Program.