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Title: Quasi-Paired Pt Atomic Sites on Mo2C Promoting Selective Four-Electron Oxygen Reduction
Authors: Zhang, Lei 
Yang, Tong 
Zang, Wenjie 
Kou, Zongkui
Ma, Yuanyuan 
Waqar, Moaz
Liu, Ximeng 
Zheng, Lirong
Pennycook, Stephen J. 
Liu, Zhaolin
Loh, Xian Jun
Shen, Lei 
Wang, John 
Keywords: cleavage of O?O bond
oxygen reduction reaction
quasi-paired Pt atoms
single atom catalysts
Issue Date: 14-Jul-2021
Publisher: John Wiley and Sons Inc
Citation: Zhang, Lei, Yang, Tong, Zang, Wenjie, Kou, Zongkui, Ma, Yuanyuan, Waqar, Moaz, Liu, Ximeng, Zheng, Lirong, Pennycook, Stephen J., Liu, Zhaolin, Loh, Xian Jun, Shen, Lei, Wang, John (2021-07-14). Quasi-Paired Pt Atomic Sites on Mo2C Promoting Selective Four-Electron Oxygen Reduction. Advanced Science 8 (18) : 2101344. ScholarBank@NUS Repository.
Rights: Attribution 4.0 International
Abstract: Atomically dispersed Pt species are advocated as a promising electrocatalyst for the oxygen reduction reaction (ORR) to boost noble metal utilization efficiency. However, when assembled on various substrates, isolated Pt single atoms are often demonstrated to proceed through the two-electron ORR pathway due to the unfavorable O?O bond cleavage thermodynamics in the absence of catalytic ensemble sites. In addition, although their distinct local coordination environments at the exact single active sites are intensively explored, the interactions and synergy between closely neighboring single atom sites remain elusive. Herein, atomically dispersed Pt monomers strongly interacting on a Mo2C support is demonstrated as a model catalyst in the four-electron ORR, and the beneficial interactions between two closely neighboring and yet non-contiguous Pt single atom sites (named as quasi-paired Pt single atoms) are shown. Compared to isolated Pt single atom sites, the quasi-paired Pt single atoms deliver a superior mass activity of 0.224 A mg?1Pt and near-100% selectivity toward four-electron ORR due to the synergistic interaction from the two quasi-paired Pt atom sites in modulating the binding mode of reaction intermediates. Our first-principles calculations reveal a unique mechanism of such quasi-paired configuration for promoting four-electron ORR. © 2021 The Authors. Advanced Science published by Wiley-VCH GmbH
Source Title: Advanced Science
ISSN: 2198-3844
DOI: 10.1002/advs.202101344
Rights: Attribution 4.0 International
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