Atomic Tuning of Single-Atom Fe-N-C Catalysts with Phosphorus for Robust Electrochemical CO2 Reduction

doi:10.1021/acs.nanolett.1c04382

	Atomic Tuning of Single-Atom Fe-N-C Catalysts with Phosphorus for Robust Electrochemical CO2 Reduction
	Li, Ke 1; Zhang, Shengbo 2; Zhang, Xiuli 3; Liu, Shuang 1; Jiang, Haosong 1; Jiang, Taoli 1; Shen, Chunyue 1; Yu, Yi 3; Chen, Wei 1
刊名	NANO LETTERS
	2022-02-23
卷号	22
关键词	CO2RR single-atom catalyst Fe-N/P-C ex-situ XAS DFT calculations
ISSN号	1530-6984
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.
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关键词	ELECTROCATALYTIC REDUCTION ; ELECTROREDUCTION ; NITROGEN ; GRAPHENE ; SITES
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
内容类型	期刊论文
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.Univ Sci & Technol China, Sch Chem & Mat Sci, Dept Appl Chem, Hefei Natl Lab Phys Sci Microscale, Hefei 230026, Anhui, 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.ShanghaiTech Univ, Sch Phys Sci & Technol, Shanghai 201210, 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).