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Domino electroreduction of CO2 to methanol on a molecular catalyst
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 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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Metadata
- 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
- Venue
- Nature
- Published
- 2019-11-27
- Volume
- 575
- Issue
- 7784
- Pages
- 639-642
- ISSN
- 0028-0836 (ISSN-L)
- 1476-4687
- 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
- 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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