O‐, N‐Atoms‐Coordinated Mn Cofactors within a Graphene Framework as Bioinspired Oxygen Reduction Reaction Electrocatalysts

• DOI: 10.1002/adma.201801732
• Publication Date: 2018-05-28T07:01:59Z
• Authors: Yang Yang; Kaitian Mao; Shiqi Gao; Hao Huang; Guoliang Xia; Zhiyu Lin; Peng Jiang; Changlai Wang; Hui Wang; Qianwang Chen
• Keywords: Oxygen; Manganese; Nitrogen; Graphite; Oxidation-Reduction; 01 natural sciences; 7. Clean energy; Catalysis; 0104 chemical sciences

Manganese (Mn) is generally regarded as not being sufficiently active for the oxygen reduction reaction (ORR) compared to other transition metals such Fe and Co. However, in biology, manganese-containing enzymes can catalyze oxygen-evolving reactions efficiently with a relative low onset potential. Here, atomically dispersed O N atoms coordinated Mn sites are incorporated within graphene frameworks emulate both structure function of cofactors heme-copper oxidases superfamily. Unlike previous single-metal catalysts general M-N-C structures, here, it proved that atom also play significant role tuning intrinsic catalytic activities metals. The biomimetic electrocatalyst exhibits superior performance ORR zinc-air batteries under alkaline conditions, which even better than commercial Pt/C. excellent be ascribed abundant frameworks, confirmed by various characterization methods. Theoretical calculations reveal activity metal significantly improved via changing local geometry nearest atoms. Especially, containing Mn-N3 O1 cofactor demonstrate fastest kinetics due d electronic states reasonable state.