Atomically dispersed Mn–Nx catalysts derived from Mn‐hexamine coordination frameworks for oxygen reduction reaction
Guoyu Zhong,
Liuyong Zou,
Xiao Chi,
Zhen Meng,
Zehong Chen,
Tingzhen Li,
Yongfa Huang,
Xiaobo Fu,
Wenbo Liao,
Shaona Zheng,
Yongjun Xu,
Feng Peng,
Xinwen Peng
Affiliations
Guoyu Zhong
Guangdong Provincial Key Laboratory of Distributed Energy Systems School of Chemical Engineering and Energy Technology, Dongguan University of Technology Dongguan China
Liuyong Zou
Guangdong Provincial Key Laboratory of Distributed Energy Systems School of Chemical Engineering and Energy Technology, Dongguan University of Technology Dongguan China
Xiao Chi
State Key Laboratory of Pulp and Paper Engineering South China University of Technology Guangzhou China
Zhen Meng
Guangdong Provincial Key Laboratory of Distributed Energy Systems School of Chemical Engineering and Energy Technology, Dongguan University of Technology Dongguan China
Zehong Chen
State Key Laboratory of Pulp and Paper Engineering South China University of Technology Guangzhou China
Tingzhen Li
State Key Laboratory of Pulp and Paper Engineering South China University of Technology Guangzhou China
Yongfa Huang
State Key Laboratory of Pulp and Paper Engineering South China University of Technology Guangzhou China
Xiaobo Fu
Guangdong Provincial Key Laboratory of Distributed Energy Systems School of Chemical Engineering and Energy Technology, Dongguan University of Technology Dongguan China
Wenbo Liao
Guangdong Provincial Key Laboratory of Distributed Energy Systems School of Chemical Engineering and Energy Technology, Dongguan University of Technology Dongguan China
Shaona Zheng
Guangdong Provincial Key Laboratory of Distributed Energy Systems School of Chemical Engineering and Energy Technology, Dongguan University of Technology Dongguan China
Yongjun Xu
Guangdong Provincial Key Laboratory of Distributed Energy Systems School of Chemical Engineering and Energy Technology, Dongguan University of Technology Dongguan China
Feng Peng
School of Chemistry and Chemical Engineering Guangzhou University Guangzhou China
Xinwen Peng
State Key Laboratory of Pulp and Paper Engineering South China University of Technology Guangzhou China
Abstract Metal‐organic frameworks recently have been burgeoning and used as precursors to obtain various metal–nitrogen–carbon catalysts for oxygen reduction reaction (ORR). Although rarely studied, Mn–N–C is a promising catalyst for ORR due to its weak Fenton reaction activity and strong graphitization catalysis. Here, we developed a facile strategy for anchoring the atomically dispersed nitrogen‐coordinated single Mn sites on carbon nanosheets (MnNCS) from an Mn‐hexamine coordination framework. The atomically dispersed Mn–N4 sites were dispersed on ultrathin carbon nanosheets with a hierarchically porous structure. The optimized MnNCS displayed an excellent ORR performance in half‐cells (0.89 V vs. reversible hydrogen electrode (RHE) in base and 0.76 V vs. RHE in acid in half‐wave potential) and Zn–air batteries (233 mW cm−2 in peak power density), along with significantly enhanced stability. Density functional theory calculations further corroborated that the Mn–N4–C12 site has favorable adsorption of *OH as the rate‐determining step. These findings demonstrate that the metal‐hexamine coordination framework can be used as a model system for the rational design of highly active atomic metal catalysts for energy applications.
