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author:

Bi, M. (Bi, M..) [1] | Yao, Y. (Yao, Y..) [2] | Kang, J. (Kang, J..) [3] | Wang, Y. (Wang, Y..) [4] | Shi, T. (Shi, T..) [5] | Zhu, Z. (Zhu, Z..) [6] | Wu, Y. (Wu, Y..) [7] | Tang, Z. (Tang, Z..) [8] | Chen, S. (Chen, S..) [9] | Liu, P. (Liu, P..) [10] | Yin, H. (Yin, H..) [11] | Zhao, H. (Zhao, H..) [12]

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Scopus

Abstract:

Atomically dispersed, non-noble-metal catalysts represent promising alternatives to costly platinum-group electrocatalysts, yet precise control over metal site proximity remains challenging. Herein, we report the synthesis of ultrathin (∼1.5 nm) N-doped carbon nanosheets decorated with densely packed single-atom copper sites (Cu SAs/N-CS), achieved via controlled pyrolysis of a Cu–1H-1,2,4-triazole complex precursor. The resulting Cu SAs/N-CS exhibits a high copper loading (3.17 wt %) with a remarkably short average interatomic distance (∼3.1 Å) between adjacent Cu atoms. Inspired by multicopper oxidase enzymes, these closely spaced Cu active sites facilitate efficient four-electron (4e–) oxygen reduction reactions (ORRs), displaying superior catalytic performance and long-term stability in both neutral and alkaline media. Specifically, Cu SAs/N-CS achieves impressive half-wave potentials of 0.68 V (neutral) and 0.91 V (alkaline) vs RHE, rivaling commercial Pt/C under neutral conditions and outperforming it in alkaline electrolytes. Density functional theory (DFT) analyses indicate that short-range Cu site proximity upshifts the d-band center, strengthens O2adsorption, and significantly lowers the activation barrier for the 4e–ORR pathway, thus elucidating the mechanism behind its exceptional catalytic activity. © 2025 American Chemical Society

Keyword:

copper single-atom catalysts DFT calculation electrocatalysts oxygen reduction reaction two-dimensional materials

Community:

  • [ 1 ] [Bi M.]Key Laboratory of Materials Physics, Center for Environmental and Energy Nanomaterials, Anhui Key Laboratory of Nanomaterials and Nanotechnology, CAS Center for Excellence in Nanoscience, Institute of Solid State Physics, Hefei Institutes of Physical Science, Chinese Academy of Sciences, Anhui, Hefei, 230031, China
  • [ 2 ] [Bi M.]University of Science and Technology of China, Anhui, Hefei, 230026, China
  • [ 3 ] [Yao Y.]Key Laboratory of Micro-Nano Energy Materials and Application Technologies, Hengyang Normal University, Hengyang, 421002, China
  • [ 4 ] [Kang J.]Key Laboratory of Materials Physics, Center for Environmental and Energy Nanomaterials, Anhui Key Laboratory of Nanomaterials and Nanotechnology, CAS Center for Excellence in Nanoscience, Institute of Solid State Physics, Hefei Institutes of Physical Science, Chinese Academy of Sciences, Anhui, Hefei, 230031, China
  • [ 5 ] [Wang Y.]College of Environment and Safety Engineering, Fuzhou University, Fuzhou, 350108, China
  • [ 6 ] [Shi T.]Key Laboratory of Materials Physics, Center for Environmental and Energy Nanomaterials, Anhui Key Laboratory of Nanomaterials and Nanotechnology, CAS Center for Excellence in Nanoscience, Institute of Solid State Physics, Hefei Institutes of Physical Science, Chinese Academy of Sciences, Anhui, Hefei, 230031, China
  • [ 7 ] [Shi T.]University of Science and Technology of China, Anhui, Hefei, 230026, China
  • [ 8 ] [Zhu Z.]Key Laboratory for Ultrafine Materials of Ministry of Education, School of Materials Science and Engineering, East China University of Science and Technology, Shanghai, 200237, China
  • [ 9 ] [Wu Y.]Key Laboratory of Materials Physics, Center for Environmental and Energy Nanomaterials, Anhui Key Laboratory of Nanomaterials and Nanotechnology, CAS Center for Excellence in Nanoscience, Institute of Solid State Physics, Hefei Institutes of Physical Science, Chinese Academy of Sciences, Anhui, Hefei, 230031, China
  • [ 10 ] [Tang Z.]Key Laboratory of Micro-Nano Energy Materials and Application Technologies, Hengyang Normal University, Hengyang, 421002, China
  • [ 11 ] [Chen S.]Key Laboratory of Materials Physics, Center for Environmental and Energy Nanomaterials, Anhui Key Laboratory of Nanomaterials and Nanotechnology, CAS Center for Excellence in Nanoscience, Institute of Solid State Physics, Hefei Institutes of Physical Science, Chinese Academy of Sciences, Anhui, Hefei, 230031, China
  • [ 12 ] [Liu P.]Centre for Catalysis and Clean Energy, School of Environment and Science, Griffith University, Gold Coast Campus, Gold Coast, 4222, QLD, Australia
  • [ 13 ] [Yin H.]Key Laboratory of Materials Physics, Center for Environmental and Energy Nanomaterials, Anhui Key Laboratory of Nanomaterials and Nanotechnology, CAS Center for Excellence in Nanoscience, Institute of Solid State Physics, Hefei Institutes of Physical Science, Chinese Academy of Sciences, Anhui, Hefei, 230031, China
  • [ 14 ] [Yin H.]University of Science and Technology of China, Anhui, Hefei, 230026, China
  • [ 15 ] [Zhao H.]Centre for Catalysis and Clean Energy, School of Environment and Science, Griffith University, Gold Coast Campus, Gold Coast, 4222, QLD, Australia

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Source :

ACS Applied Materials and Interfaces

ISSN: 1944-8244

Year: 2025

Issue: 31

Volume: 17

Page: 44541-44551

8 . 5 0 0

JCR@2023

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ESI Highly Cited Papers on the List: 0 Unfold All

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30 Days PV: 0

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