Surface Area‐Enhanced Cerium and Sulfur‐Modified Hierarchical Bismuth Oxide Nanosheets for Electrochemical Carbon Dioxide Reduction to Formate

Author:

Palanimuthu Naveenkumar1,Subramaniam Mohan Raj1,P. Muthu Austeria2,Sharma Preetam Kumar34,Ramalingam Vinoth5,Peramaiah Karthik6,Ramakrishnan Shanmugam17,Gu Geun Ho2,Yu Eileen Hao4,Yoo Dong Jin18ORCID

Affiliation:

1. Graduate School Department of Energy Storage/Conversion Engineering (BK21 FOUR) Hydrogen and Fuel Cell Research Center Jeonbuk National University Jeonju Jeollabuk‐do 54896 Republic of Korea

2. Department of Energy Engineering Korea Institute of Energy Technology (KENTECH) Naju 58330 Republic of Korea

3. Institute for Materials Discovery University College London Malet Place London WC1E 7JE United Kingdom

4. Department of Chemical Engineering Loughborough University Loughborough LE11 3TU United Kingdom

5. School of Engineering Robert Gordon University Garthdee Road Aberdeen AB10 7GJ United Kingdom

6. Agency for Science, Technology, and Research, Institute of Sustainability for Chemicals Energy and Environment 1Pesek Road, Jurong Island Singapore 627833 Singapore

7. School of Engineering Newcastle University Merz Court Newcastle upon Tyne NE17RU United Kingdom

8. Department of Life Science Jeonbuk National University Jeonju Jeollabuk‐do 54896 Republic of Korea

Abstract

AbstractElectrochemical 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.

Funder

Ministry of Education

National Research Foundation of Korea

Ministry of Science, ICT and Future Planning

UK Research and Innovation

Publisher

Wiley

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