A Janus dual-atom catalyst for electrocatalytic oxygen reduction and evolution

Bing Tang, Yanan Zhou, Qianqian Ji, Zechao Zhuang, Lei Zhang, Chao Wang, Haibo Hu, Huijuan Wang, Bingbao Mei, Fei Song, Shuang Yang, Bert. M. Weckhuysen, Hao Tan, Dingsheng Wang, Wensheng Yan

Research output: Contribution to journalArticleAcademicpeer-review

Abstract

Dual-atom catalysts, which exhibit high activity and atom utilization, show promise for sustainable energy conversion and storage technologies. However, the rational design and synthesis of a dual-atom catalyst with structurally homogeneous and flexible active sites remains challenging. In this work, we developed a strategy for the synthesis of a carbon-based catalyst with diatomic Fe–Co sites in which the Fe and Co atoms are coordinated to N and O atoms, respectively, and linked through bridging N and O atoms (FeCo–N3O3@C). The Janus FeCo–N3O3@C quaternary dimer is a stable and efficient bifunctional catalyst in the electrocatalytic oxygen reduction reaction (half-wave potential E1/2 = 0.936 V) and oxygen evolution reaction (potential E = 1.528 V at 10 mA cm−2). When assembled in a Zn–air battery, it exhibits superior performance over a benchmark Pt/C + RuO2 air cathode. A series of ex situ and in situ characterizations, combined with theoretical calculations, revealed that the bifunctional performance of the catalyst originates from the strong coupling of the Fe–N3 and Co–O3 moieties, which alters the d-orbital energy level of the metal atoms, optimizing the adsorption–desorption of oxygenated intermediates and improving the reaction kinetics of the oxygen reduction and evolution reactions. The in-depth insights gained into the fundamental mechanism of this dual-atom catalyst at the atomic and electronic level will facilitate the rational design of further highly efficient multifunctional catalysts with customized activities for specific reactions. (Figure presented.)

Original languageEnglish
Number of pages13
JournalNature Synthesis
Issue number7
DOIs
Publication statusE-pub ahead of print - 3 Jun 2024

Keywords

  • Carbon
  • Generalized gradient approximation
  • Spectroscopy
  • X-ray-emission

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