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Enhanced electrocatalytic CO2 reduction via field-induced reagent concentration
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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“Tafel analysis showed faster kinetics of the first electron transfer for the Au nanoneedles as compared to Au nanorods and Au nanoparticles.”
From Electrochemical CO 2 Reduction into Chemical Feedstocks: From Mechanistic Electrocatalysis Models to System Design (2019) · cites this paper as [76]
In the citing paper
“For example, Liu et al. designed a catalyst that significantly boosted local electric fields, enhancing the local concentration of electrolyte cations (Figure.4A) and CO2, through ultrasharp nanoneedle structuring of Au (Figure .4B) .[76]”
From Electrochemical CO 2 Reduction into Chemical Feedstocks: From Mechanistic Electrocatalysis Models to System Design (2019) · cites this paper as [76]
In the citing paper
“As a result, the authors attained high FE (>95%) and current density (22 mA/cm 2 ) for CO generation with very low overpotential (0.24 V) using Au nanoneedles (Figure.4C).”
From Electrochemical CO 2 Reduction into Chemical Feedstocks: From Mechanistic Electrocatalysis Models to System Design (2019) · cites this paper as [76]
In the citing paper
“However, the current understanding of the key underlying mechanism is inconclusive and requires further study.[76]”
From Electrochemical CO 2 Reduction into Chemical Feedstocks: From Mechanistic Electrocatalysis Models to System Design (2019) · cites this paper as [76]
In the citing paper
“Analogous effects pertaining to adsorbed chloride and cyanide anions has been observed on Au electrodes.[75,76]”
From Electrochemical CO 2 Reduction into Chemical Feedstocks: From Mechanistic Electrocatalysis Models to System Design (2019) · cites this paper as [76]
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Metadata
- 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
- Venue
- Nature
- Published
- 2016-08-03
- Volume
- 537
- Issue
- 7620
- Pages
- 382-386
- ISSN
- 0028-0836 (ISSN-L)
- 1476-4687
- 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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