Atomic Tuning of Single-Atom Fe-N-C Catalysts with Phosphorus for Robust Electrochemical CO2 Reduction
文献类型：期刊论文
| 作者 | Li, Ke3; Zhang, Shengbo2; Zhang, Xiuli1; Liu, Shuang3; Jiang, Haosong3; Jiang, Taoli3; Shen, Chunyue3; Yu, Yi1; Chen, Wei3 |
| 刊名 | NANO LETTERS
 |
| 出版日期 | 2022-02-23 |
| 卷号 | 22 |
| ISSN号 | 1530-6984 |
| 关键词 | CO2RR single-atom catalyst Fe-N/P-C ex-situ XAS DFT calculations |
| DOI | 10.1021/acs.nanolett.1c04382 |
| 通讯作者 | Chen, Wei(weichen1@ustc.edu.cn) |
| 英文摘要 | The electrochemical reduction of CO2 to produce carbon-based fuels and chemicals possesses huge potentials to alleviate current environmental problems. However, it is confronted by great challenges in the design of active electrocatalysts with low overpotentials and high product selectivity. Here we report the atomic tuning of a single-Fe-atom catalyst with phosphorus (Fe-N/P-C) on commercial carbon black as a robust electrocatalyst for CO2 reduction. The Fe-N/P-C catalyst exhibits impressive performance in the electrochemical reduction of CO2 to CO, with a high Faradaic efficiency of 98% and a high mass-normalized turnover frequency of 508.8 h(-1) at a low overpotential of 0.34 V. On the basis of ex-situ X-ray absorption spectroscopy measurements and DFT calculations, we reveal that the tuning of P in single-Fe-atom catalysts reduces the oxidation state of the Fe center and decreases the free-energy barrier of *CO intermediate formation, consequently maintaining the electrocatalytic activity and stability of single-Fe-atom catalysts. |
| WOS关键词 | ELECTROCATALYTIC REDUCTION ; ELECTROREDUCTION ; NITROGEN ; GRAPHENE ; SITES |
| 资助项目 | USTC[KY2060000150] ; USTC Center for Micro and Nanoscale Research ; Center for High-Resolution Electron Microscopy (C.EM) at ShanghaiTech University ; National Natural Science Foundation of China[52102191] |
| WOS研究方向 | Chemistry ; Science & Technology - Other Topics ; Materials Science ; Physics |
| 语种 | 英语 |
| 出版者 | AMER CHEMICAL SOC |
| WOS记录号 | WOS:000776700100014 |
| 资助机构 | USTC ; USTC Center for Micro and Nanoscale Research ; Center for High-Resolution Electron Microscopy (C.EM) at ShanghaiTech University ; National Natural Science Foundation of China |
| 源URL | [http://ir.hfcas.ac.cn:8080/handle/334002/128601]  |
| 专题 | 中国科学院合肥物质科学研究院 |
| 通讯作者 | Chen, Wei |
| 作者单位 | 1.ShanghaiTech Univ, Sch Phys Sci & Technol, Shanghai 201210, Peoples R China 2.Chinese Acad Sci, Ctr Environm & Energy Nanomat, Key Lab Mat Phys,HFIPS,Anhui Key Lab Nanomat & Na, Inst Solid State Phys,CAS Ctr Excellence Nanosci, Hefei 230031, Peoples R China 3.Univ Sci & Technol China, Sch Chem & Mat Sci, Dept Appl Chem, Hefei Natl Lab Phys Sci Microscale, Hefei 230026, Anhui, Peoples R China |
| 推荐引用方式 GB/T 7714 | Li, Ke,Zhang, Shengbo,Zhang, Xiuli,et al. Atomic Tuning of Single-Atom Fe-N-C Catalysts with Phosphorus for Robust Electrochemical CO2 Reduction[J]. NANO LETTERS,2022,22. |
| APA | Li, Ke.,Zhang, Shengbo.,Zhang, Xiuli.,Liu, Shuang.,Jiang, Haosong.,...&Chen, Wei.(2022).Atomic Tuning of Single-Atom Fe-N-C Catalysts with Phosphorus for Robust Electrochemical CO2 Reduction.NANO LETTERS,22. |
| MLA | Li, Ke,et al."Atomic Tuning of Single-Atom Fe-N-C Catalysts with Phosphorus for Robust Electrochemical CO2 Reduction".NANO LETTERS 22(2022). |
入库方式： OAI收割
来源：合肥物质科学研究院
浏览0
下载0
收藏0
其他版本
除非特别说明，本系统中所有内容都受版权保护，并保留所有权利。