Domino electroreduction of CO2 to methanol on a molecular catalyst

Wu, Yueshen; Jiang, Zhan; Lu, Xu; Liang, Yongye; Wang, Hailiang

doi:10.1038/s41586-019-1760-8

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

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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Since pioneering works by Hori et al., massive efforts have been devoted to boost catalytic performance of electrochemical CO2RR, especially within the past decade.
“Since the pioneering works by Hori et al.,313,314 massive efforts have been devoted to boost the catalytic performance of electrochemical CO2RR, especially within the past decade.315, 316, 317, 318, 319, 320, 321”
From Technologies and perspectives for achieving carbon neutrality (2021) · cites this paper as [319]

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“X is categorized into three different groups according to the CO adsorption energies with reference to Cu: (1) weak, Au; (2) intermediate, Pd, Pt and Ni; (3) strong, Fe and Ru.”
Background
Amination strategy to boost the CO 2 electroreduction current density of M–N/C single-atom catalysts to the industrial application level
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“This selectivity is similar to the one obtained with the Co SMA previously mentioned.(85)”
Result
Heterogeneous Molecular Catalysts of Metal Phthalocyanines for Electrochemical CO 2 Reduction Reactions
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Playing Domino with Carbon: Electrochemical CO2 Reduction to Methanol with Cobalt PhthalocyaninePreprint
Raglione, V., Palmeri, F., Khodadadi, A., Zanotti, G., Zendehdel, M., Flammini, R., & Contini, G. (2026) · ChemRxiv · doi:10.26434/chemrxiv.15009603/v1
Molecular Electrochemical Reduction of COx-to-Methanol with Cobalt Phthalocyanines Combined Electrochemical and Spectroscopic Studies
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Aqueous Electrochemical Reduction of Carbon Dioxide and Carbon Monoxide into Methanol with Cobalt Phthalocyanine
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CO2 electrochemical catalytic reduction with a highly active cobalt phthalocyanine
Wang, M., Torbensen, K., Salvatore, D. A., Ren, S., Joulié, D., Dumoulin, F., Mendoza, D., Lassalle‐Kaiser, B., İşçi, Ü., Berlinguette, C. P., et al. (2019) · Nature Communications · doi:10.1038/s41467-019-11542-w · Cited by 507 · see citing works
Catalytic electroreduction of CO2 to methanol on cobalt phthalocyanines and the effect of macrocycle functionalization
Tabaries, C., Capitolis, J., Khodadadi, A., G., Z., Flammini, R., Contini, G., Piccolo, L., & Prévot, M. S. (2025) · HAL

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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