Cited by 2,000CO2 Reduction Techniques and CatalystsElectrocatalysts for Energy ConversionCatalysts for Methane Reforming

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Enhanced electrocatalytic CO2 reduction via field-induced reagent concentration

Liu, Min, Pang, Yuanjie, Zhang, Bo, De Luna, Phil, Voznyy, Oleksandr, Xu, Jixian, Zheng, Xueli, Dinh, Cao Thang, Fan, Fengjia, Cao, Changhong, de Arquer, F. Pelayo García, Safaei, Tina Saberi, Mepham, Adam, Klinkova, Anna, Kumacheva, Eugenia, Filleter, Tobin, Sinton, David, Kelley, Shana O., Sargent, Edward H.·2016·Nature

DOI 10.1038/nature19060

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Abstract

Electrochemical reduction of carbon dioxide (CO 2) to carbon monoxide (CO) is the first step in the synthesis of more complex carbon-based fuels and feedstocks using renewable electricity. Unfortunately, the reaction suffers from slow kinetics owing to the low local concentration of CO 2 surrounding typical CO 2 reduction reaction catalysts. Alkali metal cations are known to overcome this limitation through non-covalent interactions with adsorbed reagent species, but the effect is restricted by the solubility of relevant salts. Large applied electrode potentials can also enhance CO 2 adsorption, but this comes at the cost of increased hydrogen (H 2) evolution. Here we report that nanostructured electrodes produce, at low applied overpotentials, local high electric fields that concentrate electrolyte cations, which in turn leads to a high local concentration of CO 2 close to the active CO 2 reduction reaction surface. Simulations reveal tenfold higher electric fields associated with metallic nanometre-sized tips compared to quasi-planar electrode regions, and measurements using gold nanoneedles confirm a field-induced reagent concentration that enables the CO 2 reduction reaction to proceed with a geometric current density for CO of 22 milliamperes per square centimetre at -0.35 volts (overpotential of 0.24 volts). This performance surpasses by an order of magnitude the performance of the best gold nanorods, nanoparticles and oxide-derived noble metal catalysts. Similarly designed palladium nanoneedle electrocatalysts produce formate with a Faradaic efficiency of more than 90 per cent and an unprecedented geometric current density for formate of 10 milliamperes per square centimetre at -0.2 volts, demonstrating the wider applicability of the field-induced reagent concentration concept.

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Authors: Liu, M., Pang, Y., Zhang, B., De Luna, P., Voznyy, O., Xu, J., Zheng, X., Dinh, C. T., Fan, F., Cao, C., de Arquer, F. P. G., Safaei, T. S., Mepham, A., Klinkova, A., Kumacheva, E., Filleter, T., Sinton, D., Kelley, S. O., & Sargent, E. H.
Affiliations: University of Toronto (CA)
East China University of Science and Technology (CN)
Tianjin University (CN)
Corresponding author: Sargent, Edward H.
ORCID: Liu, Min
Pang, Yuanjie
Zhang, Bo
Voznyy, Oleksandr
Xu, Jixian
Zheng, Xueli
Dinh, Cao Thang
Fan, Fengjia
Cao, Changhong
Klinkova, Anna
Kumacheva, Eugenia
Filleter, Tobin
Sinton, David
Kelley, Shana O.
Sargent, Edward H.
Venue: Nature
Publisher: Springer Science and Business Media LLC
Published: 2016-08-03
Volume: 537
Issue: 7620
Pages: 382-386
ISSN: 0028-0836 (ISSN-L)
1476-4687
DOI: 10.1038/nature19060
OpenAlex: W2496132953
Cited by: 2,000
References: 42
Citations by year: 2026: 150 · 2025: 195 · 2024: 265 · 2023: 238 · 2022: 218 · 2021: 233 · 2020: 226 · 2019: 201 · 2018: 164 · 2017: 104 · 2016: 6
FWCI: 43.01
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)
King Abdullah University of Science and Technology Repository (King Abdullah University of Science and Technology) (submittedVersion)
Topics: Physical Sciences › Energy › Renewable Energy, Sustainability and the Environment › CO2 Reduction Techniques and Catalysts
Physical Sciences › Energy › Renewable Energy, Sustainability and the Environment › Electrocatalysts for Energy Conversion
Physical Sciences › Chemical Engineering › Catalysis › Catalysts for Methane Reforming
Keywords: electrochemical CO2 reduction, local electric field, CO2 adsorption, carbon monoxide production, formate production, nanostructured electrodes, alkali metal cations, CO2 reduction kinetics, hydrogen evolution suppression, electrocatalyst design, CO2 selectivity

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Enhanced electrocatalytic CO2 reduction via field-induced reagent concentration

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