Abstract
Formic acid (or formate) is suggested to be one of the most economically viable products from electrochemical carbon dioxide reduction. However, its commercial viability hinges on the development of highly active and selective electrocatalysts. Here we report that structural defects have a profound positive impact on the electrocatalytic performance of bismuth. Bismuth oxide double-walled nanotubes with fragmented surface are prepared as a template, and are cathodically converted to defective bismuth nanotubes. This converted electrocatalyst enables carbon dioxide reduction to formate with excellent activity, selectivity and stability. Most significantly, its current density reaches ~288 mA cm−2 at −0.61 V versus reversible hydrogen electrode within a flow cell reactor under ambient conditions. Using density functional theory calculations, the excellent activity and selectivity are rationalized as the outcome of abundant defective bismuth sites that stabilize the *OCHO intermediate. Furthermore, this electrocatalyst is coupled with silicon photocathodes and achieves high-performance photoelectrochemical carbon dioxide reduction.
Highlights
Formic acid is suggested to be one of the most economically viable products from electrochemical carbon dioxide reduction
In order to resolve the detailed atomic-scale structure of the product, we carried out simultaneous bright field (BF) and high-angle annular dark field (HAADF) imaging on an aberration-corrected scanning transmission electron microscope (STEM)
In this study, we demonstrated that the CO2 reduction reaction (CO2RR) activity and selectivity of Bi were dramatically boosted by introducing surface defects
Summary
Formic acid (or formate) is suggested to be one of the most economically viable products from electrochemical carbon dioxide reduction. Bismuth oxide double-walled nanotubes with fragmented surface are prepared as a template, and are cathodically converted to defective bismuth nanotubes This converted electrocatalyst enables carbon dioxide reduction to formate with excellent activity, selectivity and stability. Using density functional theory calculations, the excellent activity and selectivity are rationalized as the outcome of abundant defective bismuth sites that stabilize the *OCHO intermediate This electrocatalyst is coupled with silicon photocathodes and achieves highperformance photoelectrochemical carbon dioxide reduction. Direct conversion of CO2 to formic acid via the mild and energy-efficient electrochemical approach is highly desired[16] It is predicted in the “Global Roadmap for Implementing CO2 Utilization” by the Global CO2 Initiative that the global market size of formic acid from CO2 reduction can be up to 475,000 ton year−1 by 2030 if suitable electrocatalyst materials are developed[16]. This sets the performance target if we want to bring any electrocatalyst material from benchtop scale science to industrial scale implementation
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