中文版 | English
Title

Si-doping induced electronic structure regulation of single-atom Fe sites for boosted CO2 electroreduction at low overpotentials

Author
Corresponding AuthorCao, Changsheng
Publication Years
2023-02-01
Source Title
ISSN
2096-5168
EISSN
2639-5274
Volume2023
Abstract
Transition metal-based single-atom catalysts (TM-SACs) are promising alternatives to Au-and Ag-based electrocatalysts for CO production through CO2 reduction reaction. However, developing TM-SACs with high activity and selectivity at low overpotentials is challenging. Herein, a novel Fe-based SAC with Si doping (Fe-N-C-Si) was prepared, which shows a record-high electrocatalytic performance toward the CO2-to-CO conversion with exceptional current density (> 350.0 mA cm(-2)) and similar to 100% Faradaic efficiency (FE) at the overpotentials of < 400 mV, far superior to the reported Fe-based SACs. Further assembling Fe-N-C-Si as the cathode in a rechargeable Zn-CO2 battery delivers an outstanding performance with a maximal power density of 2.44 mW cm(-2) at the output voltage of 0.30 V, as well as the high cycling stability and FE (> 90%) for CO production. Experimental combined with theoretical analysis unraveled that the nearby Si dopants in the form of Si-C/N bonds modulates the electronic structure of the atomic Fe sites in Fe-N-C-Si to significantly accelerate the key pathway involving *CO intermediate desorption, inhibiting the poisoning of the Fe sites under high CO coverage and thus boosting the CO2RR performance. This work provides an efficient strategy to tune the adsorption/desorption behaviors of intermediates on single-atom sites to improve their electrocatalytic performance.
URL[Source Record]
Indexed By
Language
English
SUSTech Authorship
Others
Funding Project
National Key R&D Program of China[2021YFA1500402] ; National Natural Science Foundation of China (NSFC)["22105203","22175174"] ; Natural Science Foundation of Fujian Province["2020J01116","2021J06033"] ; China Postdoctoral Science Foundation["2021TQ0332","2021M703215"]
WOS Research Area
Science & Technology - Other Topics
WOS Subject
Multidisciplinary Sciences
WOS Accession No
WOS:000928828300001
Publisher
Data Source
Web of Science
Citation statistics
Cited Times [WOS]:3
Document TypeJournal Article
Identifierhttp://kc.sustech.edu.cn/handle/2SGJ60CL/489998
DepartmentSouthern University of Science and Technology
工学院_材料科学与工程系
Affiliation
1.Chinese Acad Sci, Fujian Inst Res Struct Matter, State Key Lab Struct Chem, Fuzhou 350002, Peoples R China
2.Fujian Sci & Technol Innovat Lab Optoelect Informa, Fuzhou 350108, Peoples R China
3.Univ Chinese Acad Sci, Beijing 100049, Peoples R China
4.King Abdullah Univ Sci & Technol KAUST, KAUST Catalysis Ctr KCC, Thuwal 239556900, Saudi Arabia
5.City Univ Hong Kong, Dept Chem, Hong Kong 999077, Peoples R China
6.Chinese Acad Sci, CAS Key Lab Design & Assembly Funct Nanostruct, Fujian Struct Matter, Fuzhou 350002, Peoples R China
7.Kyoto Univ, Inst Integrated Cell Mat Sci iCeMS, Kyoto 6068501, Japan
8.SUSTech Kyoto Univ Adv Energy Mat Joint Innovat La, Shenzhen Key Lab Micro Nanoporous Funct Mat SKLPM, Shenzhen 518055, Peoples R China
9.Southern Univ Sci & Technol SUSTech, Dept Mat Sci & Engn, Shenzhen 518055, Peoples R China
Recommended Citation
GB/T 7714
Cao, Changsheng,Zhou, Shenghua,Zuo, Shouwei,et al. Si-doping induced electronic structure regulation of single-atom Fe sites for boosted CO2 electroreduction at low overpotentials[J]. RESEARCH,2023,2023.
APA
Cao, Changsheng.,Zhou, Shenghua.,Zuo, Shouwei.,Zhang, Huabin.,Chen, Bo.,...&Zhu, Qi-Long.(2023).Si-doping induced electronic structure regulation of single-atom Fe sites for boosted CO2 electroreduction at low overpotentials.RESEARCH,2023.
MLA
Cao, Changsheng,et al."Si-doping induced electronic structure regulation of single-atom Fe sites for boosted CO2 electroreduction at low overpotentials".RESEARCH 2023(2023).
Files in This Item:
There are no files associated with this item.
Related Services
Fulltext link
Recommend this item
Bookmark
Usage statistics
Export to Endnote
Export to Excel
Export to Csv
Altmetrics Score
Google Scholar
Similar articles in Google Scholar
[Cao, Changsheng]'s Articles
[Zhou, Shenghua]'s Articles
[Zuo, Shouwei]'s Articles
Baidu Scholar
Similar articles in Baidu Scholar
[Cao, Changsheng]'s Articles
[Zhou, Shenghua]'s Articles
[Zuo, Shouwei]'s Articles
Bing Scholar
Similar articles in Bing Scholar
[Cao, Changsheng]'s Articles
[Zhou, Shenghua]'s Articles
[Zuo, Shouwei]'s Articles
Terms of Use
No data!
Social Bookmark/Share
No comment.

Items in the repository are protected by copyright, with all rights reserved, unless otherwise indicated.