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Electrifying HCOOH synthesis from CO 2 building blocks over Cu-Bi nanorod arrays.
- Source :
-
Proceedings of the National Academy of Sciences of the United States of America [Proc Natl Acad Sci U S A] 2024 Jul 16; Vol. 121 (29), pp. e2400898121. Date of Electronic Publication: 2024 Jul 09. - Publication Year :
- 2024
-
Abstract
- Precise electrochemical synthesis of commodity chemicals and fuels from CO <subscript>2</subscript> building blocks provides a promising route to close the anthropogenic carbon cycle, in which renewable but intermittent electricity could be stored within the greenhouse gas molecules. Here, we report state-of-the-art CO <subscript>2</subscript> -to-HCOOH valorization performance over a multiscale optimized Cu-Bi cathodic architecture, delivering a formate Faradaic efficiency exceeding 95% within an aqueous electrolyzer, a C-basis HCOOH purity above 99.8% within a solid-state electrolyzer operated at 100 mA cm <superscript>-2</superscript> for 200 h and an energy efficiency of 39.2%, as well as a tunable aqueous HCOOH concentration ranging from 2.7 to 92.1 wt%. Via a combined two-dimensional reaction phase diagram and finite element analysis, we highlight the role of local geometries of Cu and Bi in branching the adsorption strength for key intermediates like *COOH and *OCHO for CO <subscript>2</subscript> reduction, while the crystal orbital Hamiltonian population analysis rationalizes the vital contribution from moderate binding strength of η <superscript>2</superscript> (O,O)-OCHO on Cu-doped Bi surface in promoting HCOOH electrosynthesis. The findings of this study not only shed light on the tuning knobs for precise CO <subscript>2</subscript> valorization, but also provide a different research paradigm for advancing the activity and selectivity optimization in a broad range of electrosynthetic systems.<br />Competing Interests: Competing interests statement:The authors declare no competing interest.
Details
- Language :
- English
- ISSN :
- 1091-6490
- Volume :
- 121
- Issue :
- 29
- Database :
- MEDLINE
- Journal :
- Proceedings of the National Academy of Sciences of the United States of America
- Publication Type :
- Academic Journal
- Accession number :
- 38980900
- Full Text :
- https://doi.org/10.1073/pnas.2400898121