Fe-N4O-C Nanoplates Covalently Bonding on Graphene for Efficient CO 2 Electroreduction and Zn-CO2 Batteries

Chen, Shan; Chen, Jialei; Li, Youzeng; Tan, Sha; Liao, Xuelong; Zhao, Tete; Zhang, Kai; Hu, Enyuan; Cheng, Fangyi; Wang, Huan

doi:10.1002/adfm.202300801

Fe-N₄O-C Nanoplates Covalently Bonding on Graphene for Efficient CO ₂ Electroreduction and Zn-CO₂ Batteries

Journal Article · Fri Mar 24 00:00:00 EDT 2023 · Advanced Functional Materials

DOI:https://doi.org/10.1002/adfm.202300801· OSTI ID:1963587

Chen, Shan ^[1]; Chen, Jialei ^[1]; Li, Youzeng ^[1]; Tan, Sha ^[2]; Liao, Xuelong ^[1]; Zhao, Tete ^[1]; ^[1]; ^[2]; ^[1]; ^[1]

Nankai University, Tianjin (China)
Brookhaven National Laboratory (BNL), Upton, NY (United States). Dept. of Chemistry

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.

View Accepted Manuscript (DOE)

Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sponsoring Organization:: Central Universities; Ministry of Science and Technology of China; National Natural Science Foundation of China; USDOE Office of Energy Efficiency and Renewable Energy (EERE), Office of Sustainable Transportation. Vehicle Technologies Office (VTO)

Grant/Contract Number:: SC0012704

OSTI ID:: 1963587

Report Number(s):: BNL-224189-2023-JAAM

Journal Information:: Advanced Functional Materials, Journal Name: Advanced Functional Materials Journal Issue: 27 Vol. 33; ISSN 1616-301X

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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Fe-N₄O-C Nanoplates Covalently Bonding on Graphene for Efficient CO ₂ Electroreduction and Zn-CO₂ Batteries