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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.
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