Cited by 1,865CO2 Reduction Techniques and CatalystsCatalysts for Methane ReformingElectrocatalysts for Energy Conversion

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Partially oxidized atomic cobalt layers for carbon dioxide electroreduction to liquid fuel

Gao, Shan, Lin, Yue, Jiao, Xingchen, Sun, Yongfu, Luo, Qiquan, Zhang, Wenhua, Li, Dianqi, Yang, Jinlong, Xie, Yi·2016·Nature

DOI 10.1038/nature16455

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Abstract

Electroreduction of CO2 into useful fuels, especially if driven by renewable energy, represents a potentially 'clean' strategy for replacing fossil feedstocks and dealing with increasing CO2 emissions and their adverse effects on climate. The critical bottleneck lies in activating CO2 into the CO2(•-) radical anion or other intermediates that can be converted further, as the activation usually requires impractically high overpotentials. Recently, electrocatalysts based on oxide-derived metal nanostructures have been shown to enable CO2 reduction at low overpotentials. However, it remains unclear how the electrocatalytic activity of these metals is influenced by their native oxides, mainly because microstructural features such as interfaces and defects influence CO2 reduction activity yet are difficult to control. To evaluate the role of the two different catalytic sites, here we fabricate two kinds of four-atom-thick layers: pure cobalt metal, and co-existing domains of cobalt metal and cobalt oxide. Cobalt mainly produces formate (HCOO(-)) during CO2 electroreduction; we find that surface cobalt atoms of the atomically thin layers have higher intrinsic activity and selectivity towards formate production, at lower overpotentials, than do surface cobalt atoms on bulk samples. Partial oxidation of the atomic layers further increases their intrinsic activity, allowing us to realize stable current densities of about 10 milliamperes per square centimetre over 40 hours, with approximately 90 per cent formate selectivity at an overpotential of only 0.24 volts, which outperforms previously reported metal or metal oxide electrodes evaluated under comparable conditions. The correct morphology and oxidation state can thus transform a material from one considered nearly non-catalytic for the CO2 electroreduction reaction into an active catalyst. These findings point to new opportunities for manipulating and improving the CO2 electroreduction properties of metal systems, especially once the influence of both the atomic-scale structure and the presence of oxide are mechanistically better understood.

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Self-citation

Authors: Gao, S., Lin, Y., Jiao, X., Sun, Y., Luo, Q., Zhang, W., Li, D., Yang, J., & Xie, Y.
Affiliations: University of Science and Technology of China (CN)
Corresponding author: Sun, Yongfu
Xie, Yi
ORCID: Gao, Shan
Lin, Yue
Jiao, Xingchen
Sun, Yongfu
Luo, Qiquan
Zhang, Wenhua
Yang, Jinlong
Xie, Yi
Venue: Nature
Publisher: Springer Science and Business Media LLC
Published: 2016-01
Volume: 529
Issue: 7584
Pages: 68-71
ISSN: 0028-0836 (ISSN-L)
1476-4687
DOI: 10.1038/nature16455
OpenAlex: W2227974961
Cited by: 1,865
References: 26
Citations by year: 2026: 62 · 2025: 108 · 2024: 153 · 2023: 154 · 2022: 195 · 2021: 222 · 2020: 264 · 2019: 226 · 2018: 233 · 2017: 171 · 2016: 77
FWCI: 63.89
Type: journal article
Language: en
Open access: closed
Licence: www.springer.com/tdm (tdm)
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 › Catalysis › Catalysts for Methane Reforming
Physical Sciences › Energy › Renewable Energy, Sustainability and the Environment › Electrocatalysts for Energy Conversion
Keywords: carbon dioxide electroreduction, cobalt electrocatalyst, atomic layers, cobalt oxide, partial oxidation, formate production, CO2 radical anion, liquid fuels, CO2 emission reduction, catalyst stability, CO2 selectivity

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Partially oxidized atomic cobalt layers for carbon dioxide electroreduction to liquid fuel

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