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Efficient electrocatalytic CO 2 reduction on a three-phase interface

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TLDR
Cui et al. as discussed by the authors designed a catalytic system that mimics the alveolus structure in mammalian lungs with high gas permeability but very low water diffusibility, enabling an array of three-phase catalytic interfaces.
Abstract
Electrochemical CO2 reduction is a critical approach to reducing the globally accelerating CO2 emission and generating value-added products. Despite great efforts to optimize catalyst activity and selectivity, facilitating the catalyst accessibility to high CO2 concentrations while maintaining electrode durability remains a significant challenge. Here, we designed a catalytic system that mimics the alveolus structure in mammalian lungs with high gas permeability but very low water diffusibility, enabling an array of three-phase catalytic interfaces. Flexible, hydrophobic, nanoporous polyethylene membranes with high gas permeability were used to enable efficient CO2 access and a high local alkalinity on the catalyst surface at different CO2 flow rates. Such an alveolus-mimicking structure generates a high CO production Faradaic efficiency of 92% and excellent geometric current densities of CO production (25.5 mA cm−2) at −0.6 V versus the reversible hydrogen electrode, with a very thin catalyst thickness of 20−80 nm. The efficient design of electrochemical CO2 reduction catalysts requires high CO2 concentrations on the catalyst surface. Here, Cui and co-workers make use of flexible, hydrophobic, nanoporous polyethylene membranes with good gas permeability to design a catalytic set-up that mimics the alveolus structure in mammalian lungs, achieving high activity and selectivity to CO.

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Citations
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Strategies in catalysts and electrolyzer design for electrochemical CO2 reduction toward C2+ products

TL;DR: A detailed review of the state-of-the-art C─C coupling strategies to be provided to the community for further development and inspiration in both fundamental understanding and technological applications is provided.
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Structural defects on converted bismuth oxide nanotubes enable highly active electrocatalysis of carbon dioxide reduction.

TL;DR: Nanotube-derived bismuth is reported for electrocatalytic reduction of carbon dioxide to formate, with performance that is enhanced by defects, and coupled with silicon photocathodes and achieves high-performance photoelectrochemical carbon dioxide reduction.
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Defect and Interface Engineering for Aqueous Electrocatalytic CO2 Reduction

TL;DR: In this article, the surface defects and interface can be rationally designed and functioned in electrocatalytic CO2 reduction (ECR) catalysts, and how these atomic-level controlling approaches help to promote efficiency and selectivity.
References
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Journal ArticleDOI

New insights into the electrochemical reduction of carbon dioxide on metallic copper surfaces

TL;DR: In this paper, the authors report new insights into the electrochemical reduction of CO2 on a metallic copper surface, enabled by the development of an experimental methodology with unprecedented sensitivity for the identification and quantification of CO 2 electroreduction products.
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CO2 Reduction at Low Overpotential on Cu Electrodes Resulting from the Reduction of Thick Cu2O Films

TL;DR: Modified Cu electrodes were prepared by annealing Cu foil in air and electrochemically reducing the resulting Cu(2)O layers, which resulted in electrodes whose activities were indistinguishable from those of polycrystalline Cu and a higher level of activity than all previously reported metal electrodes evaluated under comparable conditions.
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Aqueous CO2 reduction at very low overpotential on oxide-derived Au nanoparticles.

TL;DR: Electrokinetic studies indicate that the improved catalysis is linked to dramatically increased stabilization of the CO(2)(•-) intermediate on the surfaces of the oxide-derived Au electrodes.
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Enhanced electrocatalytic CO2 reduction via field-induced reagent concentration

TL;DR: It is reported that nanostructured electrodes produce, at low applied overpotentials, local high electric fields that concentrate electrolyte cations, which leads to a high local concentration of CO2 close to the active CO2 reduction reaction surface, which surpasses by an order of magnitude the performance of the best gold nanorods, nanoparticles and oxide-derived noble metal catalysts.
Journal ArticleDOI

Ionic Liquid–Mediated Selective Conversion of CO2 to CO at Low Overpotentials

TL;DR: An electrocatalytic system that reduces CO2 to carbon monoxide (CO) at overpotentials below 0.2 volt is reported, and the system continued producing CO for at least 7 hours at Faradaic efficiencies greater than 96%.
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