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Understanding Synergistic Catalysis on Cu-Se Dual Atom Sites via Operando X-ray Absorption Spectroscopy in Oxygen Reduction Reaction |
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| Authors: | Zhiguo Sun Huijuan Zhang Linlin Cao Xiaokang Liu Dan Wu Xinyi Shen Xue Zhang Zihang Chen Sen Ru Xiangyu Zhu Zhiyuan Xia Qiquan Luo Faqiang Xu Prof Tao Yao |
| Institution: | 1. National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei, 230029 P. R. China
These authors contributed equally to this work.;2. National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei, 230029 P. R. China;3. Institutes of Physical Science and Information Technology, Anhui University, Hefei, 230601 P. R. China |
| Abstract: | 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. |
| Keywords: | Dual-Atom Sites Operando X-Ray Absorption Spectroscopy Oxygen Reduction Reaction Synergic Catalysis Zn-Air Battery |