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Molecularly Designed Cathode for Copper-Benzimidazole-Induced CO2 Reduction to MeOH
Stockholm University, Faculty of Science, Department of Organic Chemistry.
Stockholm University, Faculty of Science, Department of Organic Chemistry.
Stockholm University, Faculty of Science, Department of Materials and Environmental Chemistry (MMK).ORCID iD: 0000-0001-7947-3860
Stockholm University, Faculty of Science, Department of Materials and Environmental Chemistry (MMK).ORCID iD: 0000-0002-3261-8134
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Number of Authors: 82025 (English)In: Angewandte Chemie International Edition, ISSN 1433-7851, E-ISSN 1521-3773Article in journal (Refereed) Epub ahead of print
Abstract [en]

Conversion of carbon dioxide (CO₂) into value-added products is aimed to develop scalable technologies to promote a circular economy. While the electrochemical reduction of CO₂ to carbon monoxide (CO) and formic acid has advanced significantly, a major challenge remains achieving further reduced and more energy-dense products, such as methanol (MeOH), through sustainable pathways. Herein, we report a molecular electrode capable of direct six-electron reduction of CO₂ to MeOH using water as a proton source with a global Faradaic efficiency (FEG) of 22% and product selectivity of 61% for MeOH. The design consists of an active copper-hydride center surrounded by two closely spaced benzimidazole–hydride units, facilitating the catalytic transfer of three hydrides to produce MeOH. The concurrent formation of formic acid and the absence of formaldehyde suggest that MeOH is generated via a formato pathway. DFT investigations revealed the complete mechanistic pathway, which supports the experimental observations. The morphology and stability of the electrode were evaluated before and after prolonged electrolysis (12 h) experiments using electron microscopic techniques.

Place, publisher, year, edition, pages
2025.
Keywords [en]
Benzimidazole, Copper, Hydride, Methanol, Molecular electrode
National Category
Materials Chemistry
Identifiers
URN: urn:nbn:se:su:diva-243098DOI: 10.1002/anie.202504783ISI: 001458917500001Scopus ID: 2-s2.0-105002142601OAI: oai:DiVA.org:su-243098DiVA, id: diva2:1957026
Available from: 2025-05-08 Created: 2025-05-08 Last updated: 2025-05-08

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Bengtsson, PamelaEriksson, LarsJansson, KjellTai, Cheuk-WaiMartín‐Matute, BelénDas, Biswanath

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Bengtsson, PamelaEriksson, LarsJansson, KjellTai, Cheuk-WaiMartín‐Matute, BelénDas, Biswanath
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Department of Organic ChemistryDepartment of Materials and Environmental Chemistry (MMK)
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Angewandte Chemie International Edition
Materials Chemistry

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