Atomic interface effect of a single atom copper catalyst for enhanced oxygen reduction reactions

Zhuoli Jiang; Wenming Sun; Huishan Shang; Wenxing Chen; Tingting Sun; Haijing Li; Juncai Dong; Jing Zhou; Zhi Li; Yu Wang; Rui Cao; Ritimukta Sarangi; Zhengkun Yang; Dingsheng Wang; Jiatao Zhang; Yadong Li

doi:10.1039/C9EE02974E

Atomic interface effect of a single atom copper catalyst for enhanced oxygen reduction reactions†

Zhuoli Jiang,‡^a Wenming Sun,‡^b Huishan Shang,‡^a Wenxing Chen,*^a Tingting Sun,^c Haijing Li,^d Juncai Dong,^d Jing Zhou,^e Zhi Li,^f Yu Wang,^e Rui Cao,^g Ritimukta Sarangi,^g Zhengkun Yang,^h Dingsheng Wang,

*^f Jiatao Zhang

*^a and Yadong Li

*^f

Author affiliations

* Corresponding authors

^a Beijing Key Laboratory of Construction Tailorable Advanced Functional Materials and Green Applications, School of Materials Science and Engineering, Beijing Institute of Technology, Beijing 100081, China
E-mail: wxchen@bit.edu.cn, zhangjt@bit.edu.cn

^b College of Science, China Agricultural University, Beijing 100193, China

^c Beijing Key Laboratory for Science and Application of Functional Molecular and Crystalline Materials, Department of Chemistry, University of Science and Technology Beijing, Beijing 100083, China

^d Beijing Synchrotron Radiation Facility, Institute of High Energy Physics, Chinese Academy of Sciences, Beijing 100049, China

^e Shanghai Synchrotron Radiation Facility, Shanghai Institute of Applied Physics, Chinese Academy of Science, Shanghai 201800, China

^f Department of Chemistry, Tsinghua University, Beijing 100084, China
E-mail: wangdingsheng@mail.tsinghua.edu.cn, ydli@mail.tsinghua.edu.cn

^g Stanford Synchrotron Radiation Lightsource, SLAC National Accelerator Laboratory, Menlo Park, CA, USA

^h Department of Chemistry, Collaborative Innovation Center of Chemistry for Energy Materials, University of Science and Technology of China, Hefei 230026, China

Abstract

The regulation of catalytic activity in the oxygen reduction reaction (ORR) is significant to the development of metal–air batteries and other oxygen involving energy conversion devices. Herein, we propose an atomic interface strategy to construct a single atom copper catalyst (denoted as Cu-SA/SNC) which exhibits enhanced ORR activity with a half-wave potential of 0.893 V vs. RHE in alkaline media. Moreover, synchrotron-radiation-based X-ray absorption fine structure (XAFS) investigations together with density functional theory (DFT) calculations reveal that the isolated bond-shrinking low-valence Cu (+1)–N₄–C₈S₂ atomic interface moiety serves as an active site during the ORR process, and the synergistic mechanism between the Cu species and the carbon matrix at the atomic interface plays a critical role in boosting the ORR efficiency, by adjusting the reaction free energy of intermediate adsorption. This atomic interface concept may provide an alternative methodology for the rational design of advanced oxygen electrode materials and new probability to improve their catalytic performance.

Energy & Environmental Science

Atomic interface effect of a single atom copper catalyst for enhanced oxygen reduction reactions†

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