Understanding Synergistic Catalysis on Cu‐Se Dual Atom Sites via Operando X‐ray Absorption Spectroscopy in Oxygen Reduction Reaction

The construction and understanding of synergy in well‐defined dual‐atom active sites is an available avenue to promote multistep tandem catalytic reactions. Herein, we construct a dual‐hetero‐atom catalyst that comprises adjacent Cu‐N4 and Se‐C3 active sites for efficient oxygen reduction reaction (...

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Published in:Angewandte Chemie 2023-03, Vol.135 (13), p.n/a
Main Authors: Sun, Zhiguo, Zhang, Huijuan, Cao, Linlin, Liu, Xiaokang, Wu, Dan, Shen, Xinyi, Zhang, Xue, Chen, Zihang, Ru, Sen, Zhu, Xiangyu, Xia, Zhiyuan, Luo, Qiquan, Xu, Faqiang, Yao, Tao
Format: Article
Language:English
Subjects:
Absorption spectroscopy
Cascade chemical reactions
Catalysis
Catalysts
Charge distribution
Chemical reduction
Chemistry
Copper
Dual-Atom Sites
Maximum power density
Metal air batteries
Operando X-Ray Absorption Spectroscopy
Oxygen
Oxygen Reduction Reaction
Oxygen reduction reactions
Synergic Catalysis
Zinc-oxygen batteries
Zn-Air Battery
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Summary:The construction and understanding of synergy in well‐defined dual‐atom active sites is an available avenue to promote multistep tandem catalytic reactions. Herein, we construct a dual‐hetero‐atom catalyst that comprises adjacent Cu‐N4 and Se‐C3 active sites for efficient oxygen reduction reaction (ORR) activity. Operando X‐ray absorption spectroscopy coupled with theoretical calculations provide in‐depth insights into this dual‐atom synergy mechanism for ORR under realistic device operation conditions. The heteroatom Se modulator can efficiently polarize the charge distribution around symmetrical Cu‐N4 moieties, and serve as synergistic site to facilitate the second oxygen reduction step simultaneously, in which the key OOH*‐(Cu1‐N4) transforms to O*‐(Se1‐C2) intermediate on the dual‐atom sites. Therefore, this designed catalyst achieves satisfied alkaline ORR activity with a half‐wave potential of 0.905 V vs. RHE and a maximum power density of 206.5 mW cm−2 in Zn‐air battery. The synergistic oxygen reduction reaction that occurs on the Cu1‐N4 and Se1‐C3 dual‐hetero‐atom sites is revealed by the operando X‐ray absorption spectroscopy under realistic Zn‐air battery conditions, in which OOH*‐(Cu1‐N4) obtains one electron and is further transformed into the O*‐(Se1‐C2) intermediate.
ISSN:0044-8249
1521-3757
DOI:10.1002/ange.202217719