文献类型：期刊文献

英文题名：High-Density Atomically Dispersed Copper Sites with Close Distances on Ultrathin N-Doped Carbon Nanosheets as an Efficient Oxygen Reduction Catalyst

作者：Bi, Mengfan[1,2];Yao, Yongsheng[3];Kang, Jian[1];Wang, Yonghao[5];Shi, Tongfei[1,2];Zhu, Zhengju[6];Wu, Yijin[1];Tang, Zhenkun[3];Chen, Shan[1];Liu, Porun[4];Yin, Huajie[1,2];Zhao, Huijun[4]

机构：[1]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]Univ Sci & Technol China, Hefei 230026, Anhui, Peoples R China;[3]Hengyang Normal Univ, Key Lab Micronano Energy Mat & Applicat Technol, Hengyang 421002, Peoples R China;[4]Griffith Univ, Ctr Catalysis & Clean Energy, Sch Environm & Sci, Gold Coast Campus, Gold Coast, Qld 4222, Australia;[5]Fuzhou Univ, Coll Environm & Safety Engn, Fuzhou 350108, Peoples R China;[6]East China Univ Sci & Technol, Sch Mat Sci & Engn, Key Lab Ultrafine Mat, Minist Educ, Shanghai 200237, Peoples R China

年份：2025

卷号：17

期号：31

起止页码：44541

外文期刊名：ACS APPLIED MATERIALS & INTERFACES

收录：;EI(收录号：20253419010370);WOS:【SCI-EXPANDED(收录号:WOS:001533115000001)】；

基金：This work was financially supported by the National Natural Science Foundation of China (grant nos. 52472263 and 52303340). Numerical computations were performed at Hefei Advanced Computing Center. In situ synchrotron radiation infrared adsorption spectroscopy was performed at Hefei Synchrotron Radiation Facility (31131. 02. HLS. IRSM).

语种：英文

外文关键词：oxygen reduction reaction; copper single-atom catalysts; two-dimensional materials; electrocatalysts; DFT calculation

摘要：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.