Activating Single‐Atom Ni Site via First‐Shell Si Modulation Boosts Oxygen Reduction Reaction

Wang, Fangqing; Li, Ying; Zhang, Rui; Liu, Hui; Zhang, Yangyang; Zheng, Xuerong; Zhang, Jun; Chen, Cong; Zheng, Shijian; Xin, Huolin L.

doi:10.1002/smll.202206071

Activating Single‐Atom Ni Site via First‐Shell Si Modulation Boosts Oxygen Reduction Reaction

Journal Article · Sun Dec 11 04:00:00 EST 2022 · Small

DOI:https://doi.org/10.1002/smll.202206071· OSTI ID:2425448

Wang, Fangqing ^[1]; Li, Ying ^[1]; Zhang, Rui ^[2]; ^[1]; Zhang, Yangyang ^[1]; Zheng, Xuerong ^[3]; Zhang, Jun ^[1]; Chen, Cong ^[1]; Zheng, Shijian ^[1]; Xin, Huolin L. ^[2]

Key Laboratory of Special Functional Materials for Ecological Environment and Information Ministry of Education School of Material Science and Engineering Hebei University of Technology Tianjin 300130 P. R. China
Department of Physics and Astronomy University of California Irvine CA 92697 USA
School of Materials Science and Engineering Tianjin University Tianjin Haihe Education Park Tianjin 300072 P. R. China

Abstract

Atomically dispersed nitrogen‐coordinated 3d transition‐metal site on carbon support (M‐NC) are promising alternatives to Pt group metal‐based catalysts toward oxygen reduction reaction (ORR). However, despite the excellent activities of most of M‐NC catalysts, such as Fe‐NC, Co‐NC et al., their durability is far from satisfactory due to Fenton reaction. Herein, this work reports a novel Si‐doped Ni‐NC catalyst (Ni‐SiNC) that possesses high activity and excellent stability. X‐ray absorption fine structure and aberration‐corrected transmission electron microscopy uncover that the single‐atom Ni site is coordinated with one Si atom and three N atoms, constructing Ni‐Si₁N₃ moiety. The Ni‐SiNC catalyst exhibits a half‐wave potential (E_1/2) of 0.866 V versus RHE, with a distinguished long‐term durability in alkaline media of only 10 mV negative shift in E_1/2 after 35 000 cycles, which is also validated in Zn‐air battery. Density functional theory calculations reveal that the Ni‐Si₁N₃ moiety facilitates ORR kinetics through optimizing the adsorption of intermediates.

Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)

Sponsoring Organization:: USDOE Office of Science (SC)

DOE Contract Number:: SC0012704

OSTI ID:: 2425448

Journal Information:: Small, Journal Name: Small Journal Issue: 8 Vol. 19; ISSN 1613-6810

Publisher:: Wiley

Country of Publication:: United States

Language:: English

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