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

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...

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Veröffentlicht in:Nature Synthesis Jg. 3; H. 7; S. 878 - 890
Hauptverfasser: Tang, Bing, Zhou, Yanan, Ji, Qianqian, Zhuang, Zechao, Zhang, Lei, Wang, Chao, Hu, Haibo, Wang, Huijuan, Mei, Bingbao, Song, Fei, Yang, Shuang, Weckhuysen, Bert. M., Tan, Hao, Wang, Dingsheng, Yan, Wensheng
Format: Journal Article
Sprache:Englisch
Veröffentlicht: London Nature Publishing Group 01.07.2024
Schlagworte:
Adsorption
Carbon
Catalysis
Catalysts
Chemical reduction
Chemical synthesis
Cobalt
Energy conversion
Energy levels
Evolution
Fourier transforms
Intermediates
Iron
Ligands
Metal air batteries
Metals
Nanoparticles
Oxygen
Oxygen evolution reactions
Oxygen reduction reactions
Reaction kinetics
Spectrum analysis
Statistical analysis
Transmission electron microscopy
Zinc-oxygen batteries
ISSN:2731-0582, 2731-0582
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Zusammenfassung: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.The rational design and synthesis of dual-atom catalysts with structurally uniform and flexible active sites remains challenging. Now the tailored synthesis of a Janus Fe–Co dual-metal catalyst is reported in which the Fe and Co atoms are coordinated to N and O, respectively, and linked through bridging N and O atoms.
Bibliographie:ObjectType-Article-1
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ISSN:2731-0582
2731-0582
DOI:10.1038/s44160-024-00545-1