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Abstract
Electrochemical CO2 reduction reaction (CO2RR) provides a renewable approach to transform CO2 to produce chemicals and fuels. Unfortunately, it faces the challenges of sluggish CO2 activation and slow water dissociation. This study reports the modification of Bi-based electrocatalyst by S, which leads to a remarkable enhancement in activity and selectivity during electrochemical CO2 reduction to formate. Based on comprehensive in situ examinations and kinetic evaluations, it is observed that the presence of S species over Bi catalyst can significantly enhance its interaction with K+(H2O)n, facilitating fast dissociation of water molecules to generate protons. Further in situ attenuated total reflectance surface-enhanced infrared absorption spectroscopy (ATR-SEIRAS) and in situ Raman spectroscopy measurements reveal that S modification is able to decrease the oxidation state of Bi active site, which can effectively enhance CO2 activation and facilitate HCOO* intermediate formation while suppressing competing hydrogen evolution reaction. Consequently, the S-modified Bi catalyst achieves impressive electrochemical CO2RR performance, reaching a formate Faradaic efficiency (FEformate) of 91.2% at a formate partial current density of ≈135 mA cm−2 and a potential of −0.8 V versus RHE in an alkaline electrolyte. © 2024 Wiley-VCH GmbH.
Original language | English |
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Article number | 2403547 |
Number of pages | 8 |
Journal | Advanced Functional Materials |
DOIs | |
Publication status | Accepted/In press/Filed - 16 May 2024 |
Funding
Y.L. and Z.W. contributed equally to this work. This work was supported by the National Natural Science Foundation of China (No. 22075195), City University of Kong Hong startup fund (9020003), ITF–RTH – Global STEM Professorship (9446006), and 2022 Jiangsu Graduate Research and Practice Innovation Plan (KYCX22_3255).
Research Keywords
- electrochemical CO2RR
- formate
- in situ characterization
- water dissociation
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Dive into the research topics of 'Promoting Electrochemical CO2 Reduction to Formate via Sulfur-Assisted Electrolysis'. Together they form a unique fingerprint.Projects
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ITF-RTH: GSP212 - Research Talent Hub
LIU, B. (Principal Investigator / Project Coordinator)
2/03/23 → …
Project: Research
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RMGS: On-site Green Hydrogen Production and Storage for Distributed Carbon Neutral Applications
LIU, B. (Principal Investigator / Project Coordinator)
1/03/23 → …
Project: Research