Intramolecular hydroxyl nucleophilic attack pathway by a polymeric water oxidation catalyst with single cobalt sites

Abstract Exploration of efficient water oxidation catalysts (WOCs) is the primary challenge in conversion of renewable energy into fuels. Here we report a molecularly well-defined heterogeneous WOC with Aza-fused, π-conjugated, microporous polymer (Aza-CMP) coordinated single cobalt sites (Aza-CMP-Co). The single cobalt sites in Aza-CMP-Co exhibited superior activity under alkaline and near-neutral conditions. Moreover, the molecular nature of the isolated catalytic sites makes Aza-CMP-Co a reliable model for studying the heterogeneous water oxidation mechanism. By a combination of experimental and theoretical results, a pH-dependent nucleophilic attack pathway for O-O bond formation was proposed. Under…

• WU
  Westlake University
• NN
  National Natural Science Foundation of China

  Awards: 22172011, 22088102
• KT
  Kungliga Tekniska Högskolan
• V
  Vetenskapsrådet

  Award: 2017-00935
• CS
  China Scholarship Council
• NN
  National Natural Science Foundation of China-Yunnan Joint Fund
• NS
  National Supercomputing Center, Korea Institute of Science and Technology Information