原位
蚀刻(微加工)
热的
碳纤维
材料科学
催化作用
金属
透射电子显微镜
Atom(片上系统)
氧气
化学工程
纳米技术
化学
计算机科学
工程类
物理
冶金
复合数
复合材料
有机化学
气象学
嵌入式系统
生物化学
图层(电子)
作者
Shengjie Wei,Lei Li,Ang Li,Lei Zhang,Haibo Hu,Dawei Pang,Qinghua Zhang,Hai Xiao,Wenxing Chen
标识
DOI:10.1016/j.cej.2023.142820
摘要
Designing atomic defects engineering is significant for boosting the activity of metal catalytic sites. Herein, we constructed Fe-N4 sites on defective N-doped carbon catalyst (Fe-N4/def-CN) by in-situ ZnO thermal etching strategy. Compared with defect-free Fe-N4/CN, Fe-N4/def-CN had a half-wave potential (E1/2) of 0.920 V vs RHE for alkaline ORR with 50 mV increasing. We directly observed the ZnO in-situ disappearance, studied ZnO thermal etching effect on CN substrate and revealed the mechanism of carbon defect formation by in-situ environmental transmission electron microscopy (ETEM) and in-situ X-ray diffraction (XRD) measurements. Density functional theory (DFT) calculations demonstrated the easier formation of double carbon-atoms defects adjacent to Fe-N4 sites. The carbon-atoms defects and Zn-atom vacancies synergistically improved the ORR activity of Fe-N4 sites. This work provides a atomic-level insight to optimize the atomic defects engineering of metal-N4 sites, such as carbon-atoms defects and metal-atoms vacancies by in-situ ZnO thermal etching strategy.
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