Fe-N4O-C Nanoplates Covalently Bonding on Graphene for Efficient CO 2 Electroreduction and Zn-CO2 Batteries
Abstract
Electrochemical carbon dioxide (CO2) reduction into value-added products holds great promise in moving toward carbon neutrality but remains a grand challenge due to lack of efficient electrocatalysts. Herein, the nucleophilic substitution reaction is elaborately harnessed to synthesize carbon nanoplates with a Fe-N4O configuration anchored onto graphene substrate (Fe-N4O-C/Gr) through covalent linkages. Density functional theory calculations demonstrate the unique configuration of Fe-N4O with one oxygen (O) atom in the axial direction not only suppresses the competing hydrogen evolution reaction, but also facilitates the desorption of *CO intermediate compared with the commonly planar single-atomic Fe sites. The Fe-N4O-C/Gr shows excellent performance in the electroreduction of CO2 into carbon monoxide (CO) with an impressive Faradaic efficiency of 98.3% at -0.7 V versus reversible hydrogen electrode (RHE) and a high turnover frequency of 3511 h-1. Furthermore, as a cathode catalyst in an aqueous zinc (Zn)-CO2 battery, the Fe-N4O-C/Gr achieves a high CO Faradaic efficiency (≈91%) at a discharge current density of 3 mA cm-2 and long-term stability over 74 h. Here this work opens up a new route to simultaneously modulate the geometric and electronic structure of single-atomic catalysts toward efficient CO2 conversion.
- Authors:
-
[1];
[2];
[1];
[1]
- Nankai University, Tianjin (China)
- Brookhaven National Laboratory (BNL), Upton, NY (United States). Dept. of Chemistry
- Publication Date:
- Research Org.:
- Brookhaven National Laboratory (BNL), Upton, NY (United States)
- Sponsoring Org.:
- USDOE Office of Energy Efficiency and Renewable Energy (EERE), Office of Sustainable Transportation. Vehicle Technologies Office (VTO); National Natural Science Foundation of China (NSFC); Ministry of Science and Technology of China; Central Universities
- OSTI Identifier:
- 1963587
- Report Number(s):
- BNL-224189-2023-JAAM
Journal ID: ISSN 1616-301X
- Grant/Contract Number:
- SC0012704; 22105107; 2021YFA1201900; 020/C029201005
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Advanced Functional Materials
- Additional Journal Information:
- Journal Volume: 33; Journal Issue: 27; Journal ID: ISSN 1616-301X
- Publisher:
- Wiley
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 25 ENERGY STORAGE; Zn-CO2 battery; atomically dispersed Fe-N4O; axial coordinations; covalent interactions; electrochemical CO2 reductions
Citation Formats
Chen, Shan, Chen, Jialei, Li, Youzeng, Tan, Sha, Liao, Xuelong, Zhao, Tete, Zhang, Kai, Hu, Enyuan, Cheng, Fangyi, and Wang, Huan. Fe-N4O-C Nanoplates Covalently Bonding on Graphene for Efficient CO 2 Electroreduction and Zn-CO2 Batteries. United States: N. p., 2023.
Web. doi:10.1002/adfm.202300801.
Chen, Shan, Chen, Jialei, Li, Youzeng, Tan, Sha, Liao, Xuelong, Zhao, Tete, Zhang, Kai, Hu, Enyuan, Cheng, Fangyi, & Wang, Huan. Fe-N4O-C Nanoplates Covalently Bonding on Graphene for Efficient CO 2 Electroreduction and Zn-CO2 Batteries. United States. https://doi.org/10.1002/adfm.202300801
Chen, Shan, Chen, Jialei, Li, Youzeng, Tan, Sha, Liao, Xuelong, Zhao, Tete, Zhang, Kai, Hu, Enyuan, Cheng, Fangyi, and Wang, Huan. Fri .
"Fe-N4O-C Nanoplates Covalently Bonding on Graphene for Efficient CO 2 Electroreduction and Zn-CO2 Batteries". United States. https://doi.org/10.1002/adfm.202300801. https://www.osti.gov/servlets/purl/1963587.
@article{osti_1963587,
title = {Fe-N4O-C Nanoplates Covalently Bonding on Graphene for Efficient CO 2 Electroreduction and Zn-CO2 Batteries},
author = {Chen, Shan and Chen, Jialei and Li, Youzeng and Tan, Sha and Liao, Xuelong and Zhao, Tete and Zhang, Kai and Hu, Enyuan and Cheng, Fangyi and Wang, Huan},
abstractNote = {Electrochemical carbon dioxide (CO2) reduction into value-added products holds great promise in moving toward carbon neutrality but remains a grand challenge due to lack of efficient electrocatalysts. Herein, the nucleophilic substitution reaction is elaborately harnessed to synthesize carbon nanoplates with a Fe-N4O configuration anchored onto graphene substrate (Fe-N4O-C/Gr) through covalent linkages. Density functional theory calculations demonstrate the unique configuration of Fe-N4O with one oxygen (O) atom in the axial direction not only suppresses the competing hydrogen evolution reaction, but also facilitates the desorption of *CO intermediate compared with the commonly planar single-atomic Fe sites. The Fe-N4O-C/Gr shows excellent performance in the electroreduction of CO2 into carbon monoxide (CO) with an impressive Faradaic efficiency of 98.3% at -0.7 V versus reversible hydrogen electrode (RHE) and a high turnover frequency of 3511 h-1. Furthermore, as a cathode catalyst in an aqueous zinc (Zn)-CO2 battery, the Fe-N4O-C/Gr achieves a high CO Faradaic efficiency (≈91%) at a discharge current density of 3 mA cm-2 and long-term stability over 74 h. Here this work opens up a new route to simultaneously modulate the geometric and electronic structure of single-atomic catalysts toward efficient CO2 conversion.},
doi = {10.1002/adfm.202300801},
journal = {Advanced Functional Materials},
number = 27,
volume = 33,
place = {United States},
year = {Fri Mar 24 00:00:00 EDT 2023},
month = {Fri Mar 24 00:00:00 EDT 2023}
}
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