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

Palanimuthu, Naveenkumar, Subramaniam, Mohan Raj, Muthu Austeria, P., Sharma, Preetam Kumar, Ramalingam, Vinoth, Peramaiah, Karthik, Ramakrishnan, Shanmugam, Gu, Geun Ho, Yu, Eileen Hao and Yoo, Dong Jin (2024) Surface area-enhanced cerium and sulfur-modified hierarchical bismuth oxide nanosheets for electrochemical carbon dioxide reduction to formate. Small, 20 (40), [2400913]. (doi:10.1002/smll.202400913).

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.

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Contributors

Author: Eileen Hao Yu

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