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author:

Bi, Mengfan (Bi, Mengfan.) [1] | Yao, Yongsheng (Yao, Yongsheng.) [2] | Kang, Jian (Kang, Jian.) [3] | Wang, Yonghao (Wang, Yonghao.) [4] | Shi, Tongfei (Shi, Tongfei.) [5] | Zhu, Zhengju (Zhu, Zhengju.) [6] | Wu, Yijin (Wu, Yijin.) [7] | Tang, Zhenkun (Tang, Zhenkun.) [8] | Chen, Shan (Chen, Shan.) [9] | Liu, Porun (Liu, Porun.) [10] | Yin, Huajie (Yin, Huajie.) [11] | Zhao, Huijun (Zhao, Huijun.) [12]

Indexed by:

SCIE

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 (similar to 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 (similar to 3.1 & Aring;) 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 O2 adsorption, and significantly lowers the activation barrier for the 4e- ORR pathway, thus elucidating the mechanism behind its exceptional catalytic activity.

Keyword:

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

Community:

  • [ 1 ] [Bi, Mengfan]Chinese Acad Sci, Ctr Environm & Energy Nanomat,CAS Ctr Excellence N, Key Lab Mat Phys,Anhui Key Lab Nanomat & Nanotech, CAS Ctr Excellence Nanosci,Inst Solid State Phys,H, Hefei 230031, Anhui, Peoples R China
  • [ 2 ] [Kang, Jian]Chinese Acad Sci, Ctr Environm & Energy Nanomat,CAS Ctr Excellence N, Key Lab Mat Phys,Anhui Key Lab Nanomat & Nanotech, CAS Ctr Excellence Nanosci,Inst Solid State Phys,H, Hefei 230031, Anhui, Peoples R China
  • [ 3 ] [Shi, Tongfei]Chinese Acad Sci, Ctr Environm & Energy Nanomat,CAS Ctr Excellence N, Key Lab Mat Phys,Anhui Key Lab Nanomat & Nanotech, CAS Ctr Excellence Nanosci,Inst Solid State Phys,H, Hefei 230031, Anhui, Peoples R China
  • [ 4 ] [Wu, Yijin]Chinese Acad Sci, Ctr Environm & Energy Nanomat,CAS Ctr Excellence N, Key Lab Mat Phys,Anhui Key Lab Nanomat & Nanotech, CAS Ctr Excellence Nanosci,Inst Solid State Phys,H, Hefei 230031, Anhui, Peoples R China
  • [ 5 ] [Chen, Shan]Chinese Acad Sci, Ctr Environm & Energy Nanomat,CAS Ctr Excellence N, Key Lab Mat Phys,Anhui Key Lab Nanomat & Nanotech, CAS Ctr Excellence Nanosci,Inst Solid State Phys,H, Hefei 230031, Anhui, Peoples R China
  • [ 6 ] [Yin, Huajie]Chinese Acad Sci, Ctr Environm & Energy Nanomat,CAS Ctr Excellence N, Key Lab Mat Phys,Anhui Key Lab Nanomat & Nanotech, CAS Ctr Excellence Nanosci,Inst Solid State Phys,H, Hefei 230031, Anhui, Peoples R China
  • [ 7 ] [Bi, Mengfan]Univ Sci & Technol China, Hefei 230026, Anhui, Peoples R China
  • [ 8 ] [Shi, Tongfei]Univ Sci & Technol China, Hefei 230026, Anhui, Peoples R China
  • [ 9 ] [Yin, Huajie]Univ Sci & Technol China, Hefei 230026, Anhui, Peoples R China
  • [ 10 ] [Yao, Yongsheng]Hengyang Normal Univ, Key Lab Micronano Energy Mat & Applicat Technol, Hengyang 421002, Peoples R China
  • [ 11 ] [Tang, Zhenkun]Hengyang Normal Univ, Key Lab Micronano Energy Mat & Applicat Technol, Hengyang 421002, Peoples R China
  • [ 12 ] [Liu, Porun]Griffith Univ, Ctr Catalysis & Clean Energy, Sch Environm & Sci, Gold Coast Campus, Gold Coast, Qld 4222, Australia
  • [ 13 ] [Zhao, Huijun]Griffith Univ, Ctr Catalysis & Clean Energy, Sch Environm & Sci, Gold Coast Campus, Gold Coast, Qld 4222, Australia
  • [ 14 ] [Wang, Yonghao]Fuzhou Univ, Coll Environm & Safety Engn, Fuzhou 350108, Peoples R China
  • [ 15 ] [Zhu, Zhengju]East China Univ Sci & Technol, Sch Mat Sci & Engn, Key Lab Ultrafine Mat, Minist Educ, Shanghai 200237, Peoples R China

Reprint 's Address:

  • [Yin, Huajie]Chinese Acad Sci, Ctr Environm & Energy Nanomat,CAS Ctr Excellence N, Key Lab Mat Phys,Anhui Key Lab Nanomat & Nanotech, CAS Ctr Excellence Nanosci,Inst Solid State Phys,H, Hefei 230031, Anhui, Peoples R China;;[Yin, Huajie]Univ Sci & Technol China, Hefei 230026, Anhui, Peoples R China;;[Zhao, Huijun]Griffith Univ, Ctr Catalysis & Clean Energy, Sch Environm & Sci, Gold Coast Campus, Gold Coast, Qld 4222, Australia;;[Wang, Yonghao]Fuzhou Univ, Coll Environm & Safety Engn, Fuzhou 350108, Peoples R China

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Source :

ACS APPLIED MATERIALS & INTERFACES

ISSN: 1944-8244

Year: 2025

8 . 5 0 0

JCR@2023

Cited Count:

WoS CC Cited Count:

SCOPUS Cited Count:

ESI Highly Cited Papers on the List: 0 Unfold All

WanFang Cited Count:

Chinese Cited Count:

30 Days PV: 0

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