Surface area‐enhanced cerium and sulfur‐modified hierarchical bismuth oxide nanosheets for electrochemical carbon dioxide reduction to formate.

Palanimuthu, Naveenkumar; Subramaniam, Mohan Raj; P., Muthu Austeria; Sharma, Preetam Kumar; Ramalingam, Vinoth; Peramaiah, Karthik; Ramakrishnan, Shanmugam; Gu, Geun Ho; Yu, Eileen Hao; Yoo, Dong Jin

Abstract

Electrochemical carbon dioxide reduction reaction (ECO2RR) is a promising approach to synthesize fuels and value-added chemical feedstocks while reducing atmospheric CO2 levels. Here, high surface area cerium and sulfur-doped hierarchical bismuth oxide nanosheets (Ce@S-Bi2O3) are develpoed by a solvothermal method. The resulting Ce@S-Bi2O3 electrocatalyst shows a maximum formate Faradaic efficiency (FE) of 92.5% and a current density of 42.09 mA cm−2 at −1.16 V versus RHE using a traditional H-cell system. Furthermore, using a three-chamber gas diffusion electrode (GDE) reactor, a maximum formate FE of 85% is achieved in a wide range of applied potentials (−0.86 to −1.36 V vs RHE) using Ce@S-Bi2O3. The density functional theory (DFT) results show that doping of Ce and S in Bi2O3 enhances formate production by weakening the OH* and H* species. Moreover, DFT calculations reveal that *OCHO is a dominant pathway on Ce@S-Bi2O3 that leads to efficient formate production. This study opens up new avenues for designing metal and element-doped electrocatalysts to improve the catalytic activity and selectivity for ECO2RR.

Citation

PALANTIMUTHU, N., SUBRAMANIAM, M.R., P, M.A., SHARMA, P.K., RAMALINGAM, V., PERAMAIAH, K., RAMAKRISHNAN, S., GU, G.H., YU, E.H. and YOO, D.J. 2024. Surface area-enhanced cerium and sulfur-modified hierarchical bismuth oxide nanosheets for electrochemical carbon dioxide reduction to formate. Small [online], Early View. Available from: https://doi.org/10.1002/smll.202400913

• Journal Article Type: Article
• Acceptance Date: May 21, 2024
• Online Publication Date: Jun 7, 2024
• Deposit Date: Jun 10, 2024
• Publicly Available Date: Jun 11, 2024
• Journal: Small
• Print ISSN: 1613-6810
• Electronic ISSN: 1613-6829
• Publisher: Wiley
• Peer Reviewed: Peer Reviewed
• DOI: https://doi.org/10.1002/smll.202400913
• Keywords: Bismuth oxide; Density functional theory; Electrochemical CO2 reduction; Formate; Surface area
• Public URL: https://rgu-repository.worktribe.com/output/2372354
• Additional Information: This article has been published with separate supporting information. This supporting information has been incorporated into a single file on this repository and can be found at the end of the file associated with this output.