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

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)–N 4–C 8S 2 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. Furthermore, 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.

Authors:
 [1];  [2];  [1];  [1];  [3];  [4];  [4];  [5];  [6];  [5];  [7];  [7];  [8]; ORCiD logo [6]; ORCiD logo [1]; ORCiD logo [9]
  1. Beijing Inst. of Technology, Beijing (China)
  2. China Agricultural Univ., Beijing (China)
  3. Univ. of Science and Technology Beijing, Beijing (China)
  4. Chinese Academy of Sciences (CAS), Beijing (China)
  5. Chinese Academy of Sciences (CAS), Shanghai (China)
  6. Tsinghua Univ., Beijing (China)
  7. SLAC National Accelerator Lab., Menlo Park, CA (United States)
  8. Univ. of Science and Technology of China, Hefei (China)
  9. Department of Chemistry; Tsinghua University; Beijing 100084; China
Publication Date:
Research Org.:
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1595249
Grant/Contract Number:  
AC02-76SF00515; 21643003; 21671117; 21703219; 21801015; 21871159; 51501010; 51631001; 51702016; 51872030
Resource Type:
Accepted Manuscript
Journal Name:
Energy & Environmental Science
Additional Journal Information:
Journal Volume: 12; Journal Issue: 12; Journal ID: ISSN 1754-5692
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Jiang, Zhuoli, Sun, Wenming, Shang, Huishan, Chen, Wenxing, Sun, Tingting, Li, Haijing, Dong, Juncai, Zhou, Jing, Li, Zhi, Wang, Yu, Cao, Rui, Sarangi, Ritimukta, Yang, Zhengkun, Wang, Dingsheng, Zhang, Jiatao, and Li, Yadong. Atomic interface effect of a single atom copper catalyst for enhanced oxygen reduction reactions. United States: N. p., 2019. Web. doi:10.1039/c9ee02974e.
Jiang, Zhuoli, Sun, Wenming, Shang, Huishan, Chen, Wenxing, Sun, Tingting, Li, Haijing, Dong, Juncai, Zhou, Jing, Li, Zhi, Wang, Yu, Cao, Rui, Sarangi, Ritimukta, Yang, Zhengkun, Wang, Dingsheng, Zhang, Jiatao, & Li, Yadong. Atomic interface effect of a single atom copper catalyst for enhanced oxygen reduction reactions. United States. doi:10.1039/c9ee02974e.
Jiang, Zhuoli, Sun, Wenming, Shang, Huishan, Chen, Wenxing, Sun, Tingting, Li, Haijing, Dong, Juncai, Zhou, Jing, Li, Zhi, Wang, Yu, Cao, Rui, Sarangi, Ritimukta, Yang, Zhengkun, Wang, Dingsheng, Zhang, Jiatao, and Li, Yadong. Fri . "Atomic interface effect of a single atom copper catalyst for enhanced oxygen reduction reactions". United States. doi:10.1039/c9ee02974e.
@article{osti_1595249,
title = {Atomic interface effect of a single atom copper catalyst for enhanced oxygen reduction reactions},
author = {Jiang, Zhuoli and Sun, Wenming and Shang, Huishan and Chen, Wenxing and Sun, Tingting and Li, Haijing and Dong, Juncai and Zhou, Jing and Li, Zhi and Wang, Yu and Cao, Rui and Sarangi, Ritimukta and Yang, Zhengkun and Wang, Dingsheng and Zhang, Jiatao and Li, Yadong},
abstractNote = {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. Furthermore, 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.},
doi = {10.1039/c9ee02974e},
journal = {Energy & Environmental Science},
number = 12,
volume = 12,
place = {United States},
year = {2019},
month = {11}
}

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