Cited by 1,194CO2 Reduction Techniques and CatalystsCarbon dioxide utilization in catalysisCatalysts for Methane Reforming

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Domino electroreduction of CO2 to methanol on a molecular catalyst

Wu, Yueshen, Jiang, Zhan, Lu, Xu, Liang, Yongye, Wang, Hailiang·2019·Nature

DOI 10.1038/s41586-019-1760-8

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Abstract

Electrochemical carbon dioxide (CO 2) reduction can in principle convert carbon emissions to fuels and value-added chemicals, such as hydrocarbons and alcohols, using renewable energy, but the efficiency of the process is limited by its sluggish kinetics 1,2. Molecular catalysts have well defined active sites and accurately tailorable structures that allow mechanism-based performance optimization, and transition-metal complexes have been extensively explored in this regard. However, these catalysts generally lack the ability to promote CO 2 reduction beyond the two-electron process to generate more valuable products 1,3. Here we show that when immobilized on carbon nanotubes, cobalt phthalocyanine-used previously to reduce CO 2 to primarily CO-catalyses the six-electron reduction of CO 2 to methanol with appreciable activity and selectivity. We find that the conversion, which proceeds via a distinct domino process with CO as an intermediate, generates methanol with a Faradaic efficiency higher than 40 per cent and a partial current density greater than 10 milliamperes per square centimetre at -0.94 volts with respect to the reversible hydrogen electrode in a near-neutral electrolyte. The catalytic activity decreases over time owing to the detrimental reduction of the phthalocyanine ligand, which can be suppressed by appending electron-donating amino substituents to the phthalocyanine ring. The improved molecule-based electrocatalyst converts CO 2 to methanol with considerable activity and selectivity and with stable performance over at least 12 hours.

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Authors: Wu, Y., Jiang, Z., Lu, X., Liang, Y., & Wang, H.
Affiliations: Yale University (US)
Southern University of Science and Technology (CN)
Corresponding author: Liang, Yongye
Wang, Hailiang
ORCID: Wu, Yueshen
Jiang, Zhan
Liang, Yongye
Wang, Hailiang
Venue: Nature
Publisher: Springer Science and Business Media LLC
Published: 2019-11-27
Volume: 575
Issue: 7784
Pages: 639-642
ISSN: 0028-0836 (ISSN-L)
1476-4687
DOI: 10.1038/s41586-019-1760-8
OpenAlex: W2990950642
Cited by: 1,194
References: 29
Citations by year: 2026: 123 · 2025: 208 · 2024: 229 · 2023: 191 · 2022: 162 · 2021: 177 · 2020: 102 · 2019: 1
FWCI: 23.57
Type: journal article
Language: en
Open access: closed
Licence: www.springernature.com/gp/researchers/text-and-data-mining (tdm)
www.springernature.com/gp/researchers/text-and-data-mining (vor)
Locations: Nature (publishedVersion)
PubMed (publishedVersion)
RePEc: Research Papers in Economics (submittedVersion)
Topics: Physical Sciences › Energy › Renewable Energy, Sustainability and the Environment › CO2 Reduction Techniques and Catalysts
Physical Sciences › Chemical Engineering › Process Chemistry and Technology › Carbon dioxide utilization in catalysis
Physical Sciences › Chemical Engineering › Catalysis › Catalysts for Methane Reforming
Keywords: electrochemical CO2 reduction, CO2 to methanol, cobalt phthalocyanine, molecular electrocatalysts, CO intermediate, Faradaic efficiency, ligand reduction, catalyst stability
MeSH terms: Methanol, Carbon Dioxide, Catalysis, Electrochemistry, Indoles, Organometallic Compounds, Nanotubes, Carbon

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Domino electroreduction of CO2 to methanol on a molecular catalyst

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