Regulating electron configuration of single Cu sites via unsaturated N,O-coordination for selective oxidation of benzene

Developing highly efficient catalyst for selective oxidation of benzene to phenol (SOBP) with low H(2)O(2) consumption is highly desirable for practical application, but challenge remains. Herein, we report unique single-atom Cu(1)-N(1)O(2) coordination-structure on N/C material (Cu-N(1)O(2) SA/CN), prepared by water molecule-mediated pre-assembly-pyrolysis method, can efficiently boost SOBP reaction at a 2:1 of low H(2)O(2)/benzene molar ratio, showing 83.7% of high benzene conversion with 98.1% of phenol selectivity. The Cu(1)-N(1)O(2) sites can provide a preponderant reaction pathway for SOBP reaction with less steps and lower energy barrier. As a result, it shows an unexpectedly higher turnover frequency (435 h(−1)) than that of Cu(1)-N(2) (190 h(−1)), Cu(1)-N(3) (90 h(−1)) and Cu nanoparticle (58 h(−1)) catalysts, respectively. This work provides a facile and efficient method for regulating the electron configuration of single-atom catalyst and generates a highly active and selective non-precious metal catalyst for industrial production of phenol through selective oxidation of benzene.