Ferromagnetic ordering correlated strong metal–oxygen hybridization for superior oxygen reduction reaction activity

Author:

Li Jisi1ORCID,Zheng Caiyan2,Zhao Erling1,Mao Jing1,Cheng Yahui3,Liu Hui1,Hu Zhenpeng2,Ling Tao1

Affiliation:

1. School of Materials Science and Engineering, Tianjin University, Tianjin 300072, China

2. School of Physics, Nankai University, Tianjin 300071, China

3. Department of Electronics, Nankai University, Tianjin 300350, China

Abstract

The efficiency of transition-metal oxide materials toward oxygen-related electrochemical reactions is classically controlled by metal–oxygen hybridization. Recently, the unique magnetic exchange interactions in transition-metal oxides are proposed to facilitate charge transfer and reduce activation barrier in electrochemical reactions. Such spin/magnetism-related effects offer a new and rich playground to engineer oxide electrocatalysts, but their connection with the classical metal–oxygen hybridization theory remains an open question. Here, using the Mn x V y O z family as a platform, we show that ferromagnetic (FM) ordering is intrinsically correlated with the strong manganese (Mn)–oxygen (O) hybridization of Mn oxides, thus significantly increasing the oxygen reduction reaction (ORR) activity. We demonstrate that this enhanced Mn–O hybridization in FM Mn oxides is closely associated with the generation of active Mn sites on the oxide surface and obtaining favorable reaction thermodynamics under operating conditions. As a result, FM-Mn 2 V 2 O 7 with a high degree of Mn–O hybridization achieves a record high ORR activity. Our work highlights the potential applications of magnetic oxide materials with strong metal–oxygen hybridization in energy devices.

Funder

MOST | National Natural Science Foundation of China

天津市科学技术局 | Natural Science Foundation of Tianjin Municipality

Publisher

Proceedings of the National Academy of Sciences

Subject

Multidisciplinary

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