Issue 11, 2023

Atomically dispersed Mn atoms coordinated with N and O within an N-doped porous carbon framework for boosted oxygen reduction catalysis

Abstract

Developing efficient and robust catalysts to replace Pt group metals for the oxygen reduction reaction (ORR) is conducive to achieving highly efficient energy conversion. Here, we develop a general ion exchange strategy to construct highly efficient ORR catalysts consisting of various atomically dispersed metal atoms anchored on N-doped porous carbon (M–SAs/NC) to investigate the atomic structure–catalytic activity relationship. The structure characterization results demonstrated that the achieved atomic structure varied due to the presence of different metal centers. Mn–SAs/NC consists of MnN3O1 centers, in which the Mn single atoms are stabilized by 3 N and 1 O. In contrast, the center metals in Fe-/Co-/Cu single-atom catalysts are coordinated by merely N atoms. Mn–SAs/NC delivers superior performance for the ORR with a half-wave potential (E1/2) of 0.91 V vs. RHE in 0.1 M KOH solution, outperforming that of the commercial Pt/C catalyst and the control Fe-/Co-/Cu single-atom catalysts. Furthermore, Mn–SAs/NC also shows excellent methanol tolerance and stability up to 5000 cycles. Density functional theory (DFT) calculations reveal that Mn single atom catalysts with MnN3O1 centers contributed to the superior ORR performance with lower energy barriers and optimized adsorption capacity of intermediates. These findings provide insights into the design and development of specific coordinated structures of atomically dispersed catalysts to facilitate the practical applications of energy conversion.

Graphical abstract: Atomically dispersed Mn atoms coordinated with N and O within an N-doped porous carbon framework for boosted oxygen reduction catalysis

Supplementary files

Article information

Article type
Paper
Submitted
01 noy 2022
Accepted
02 fev 2023
First published
02 fev 2023

Nanoscale, 2023,15, 5448-5457

Atomically dispersed Mn atoms coordinated with N and O within an N-doped porous carbon framework for boosted oxygen reduction catalysis

J. Huo, X. Cao, Y. Tian, L. Li, J. Qu, Y. Xie, X. Nie, Y. Zhao, J. Zhang and H. Liu, Nanoscale, 2023, 15, 5448 DOI: 10.1039/D2NR06096E

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