CO
            <sub>2</sub>
            electrolysis to multicarbon products at activities greater than 1 A cm
            <sup>−2</sup>

Arquer, F. Pelayo Garcı́a de; Dinh, Cao-Thang; Ozden, Adnan; Wicks, Joshua; McCallum, Christopher; Kirmani, Ahmad R.; Nam, Dae‐Hyun; Gabardo, Christine M.; Seifitokaldani, Ali; Wang, Xue; Li, Yuguang C.; Li, Fengwang; Edwards, Jonathan P.; Richter, Lee J.; Thorpe, Steven J.; Sargent, Edward H.

doi:10.1126/science.aay4217

Cited by 1,103 publications

(939 citation statements)

References 69 publications

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“…Vapor-fed CO 2 R cells have several advantages for CO 2 R such as the ability to overcome mass transport limitations of CO 2 solubility in aqueous electrolytes 36 . Examples of vapor-fed CO 2 R cells have exhibited large current densities, increased selectivity, and high single pass conversion rates for CO 2 R on Cu-based electrodes [37][38][39][40][41][42] . To test the proof-of-concept design, a vapor-fed CO 2 R cell similar to other previously reported cells was employed 38 .…”

Section: Electrochemical Conversion Of Co 2 In a Vapor-fed Devicementioning

confidence: 99%

A direct coupled electrochemical system for capture and conversion of CO2 from oceanwater

et al. 2020

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Capture and conversion of CO 2 from oceanwater can lead to net-negative emissions and can provide carbon source for synthetic fuels and chemical feedstocks at the gigaton per year scale. Here, we report a direct coupled, proof-of-concept electrochemical system that uses a bipolar membrane electrodialysis (BPMED) cell and a vapor-fed CO 2 reduction (CO 2 R) cell to capture and convert CO 2 from oceanwater. The BPMED cell replaces the commonly used water-splitting reaction with one-electron, reversible redox couples at the electrodes and demonstrates the ability to capture CO 2 at an electrochemical energy consumption of 155.4 kJ mol −1 or 0.98 kWh kg −1 of CO 2 and a CO 2 capture efficiency of 71%. The direct coupled, vapor-fed CO 2 R cell yields a total Faradaic efficiency of up to 95% for electrochemical CO 2 reduction to CO. The proof-of-concept system provides a unique technological pathway for CO 2 capture and conversion from oceanwater with only electrochemical processes.

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Section: Electrochemical Conversion Of Co 2 In a Vapor-fed Devicementioning

confidence: 99%

A direct coupled electrochemical system for capture and conversion of CO2 from oceanwater

et al. 2020

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“…Additionally, the surface and architecture of the cathode catalyst significantly influences the CD and is critical in achieving high (>100 mA/cm 2 ) CD [98]. For example, hydrophobic gas diffusion layers (GDL) have been reported to increase the transfer of CO 2 molecules toward the catalyst surface [95][96][97]. Ideally, effective porous catalyst layers should have both hydrophobicity to avoid flooding and hydrophilicity to help absorption of CO 2 on catalysts [99][100][101].…”

Section: Introductionmentioning

confidence: 99%

Three-Dimensional Cathodes for Electrochemical Reduction of CO2: From Macro- to Nano-Engineering

et al. 2020

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Rising anthropogenic CO2 emissions and their climate warming effects have triggered a global response in research and development to reduce the emissions of this harmful greenhouse gas. The use of CO2 as a feedstock for the production of value-added fuels and chemicals is a promising pathway for development of renewable energy storage and reduction of carbon emissions. Electrochemical CO2 conversion offers a promising route for value-added products. Considerable challenges still remain, limiting this technology for industrial deployment. This work reviews the latest developments in experimental and modeling studies of three-dimensional cathodes towards high-performance electrochemical reduction of CO2. The fabrication–microstructure–performance relationships of electrodes are examined from the macro- to nanoscale. Furthermore, future challenges, perspectives and recommendations for high-performance cathodes are also presented.

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“…Secondary coordination sphere effects, routinely employed by enzymes, 7 have been translated to both molecular 8,9 and heterogeneous [10][11][12][13] CO2R electrocatalysts. In the context of heterogeneous systems, CO2R performance has been successfully modulated through the use of grafted surface ligands which interact with adsorbed species or promote their transfer to the catalyst surface, [14][15][16][17][18][19] design of enzyme-mimetic catalytic pockets in porous materials, 20,21 and tuning of the electrolyte. [22][23][24] Complementary to CO2R system design is the innovation of operando techniques which provide mechanistic information on the reaction and are performed simultaneously as the reaction proceeds.…”

Section: Introductionmentioning

confidence: 99%

Surface Chemistry Modulates CO2 Reduction Reaction Intermediates on Silver Nanoparticle Electrocatalysts

Harris¹,

Chartrand²,

Heidary³

et al. 2020

Preprint

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<div>Electrocatalytic reduction of carbon dioxide (CO2R) to fuels and chemicals is a pressing scientific</div><div>and engineering challenge that is, in part, hampered by a lack of understanding of the surface reaction</div><div>mechanism, even for relatively simple systems. While many efforts have been dedicated to promoting CO2R</div><div>on catalytic surfaces by tuning composition, morphology, and defects, the role of the reaction environment</div><div>around the active site, and how this can be leveraged to modulate CO2R, is less clear. To this end, we</div><div>focused on a model CO2R catalyst, Ag nanoparticles, and carried out a combined electrocatalytic and</div><div>operando Raman spectroscopic investigation of CO2R on their surfaces. Bare Ag and chemically modified</div><div>Ag nanoparticles were investigated to understand how the surface reaction environment dictates</div><div>intermediate binding and catalytic efficiency en route to CO generation. The results revealed that the</div><div>primary product on Ag is CO, which is formed through a doubly-bound CObridge configuration. In contrast,</div><div>electrografted imidazole and polyvinylpyrrolidone (PVP)-coated Ag feature CO in a singly-bound COatop</div><div>configuration on their surfaces, whereas porous zeolitic-imidazolate framework-coated Ag was observed</div><div>to bind both CObridge and COatop. Further, another function of the Ag surface modifications is to dictate the</div><div>type of Ag surface sites which form Ag-C bonds with CO2R intermediates. Through analysis of the of</div><div>electrochemical and spectroscopic data, we deduce which key aspects of CO2R on Ag surface render a</div><div>CO2R system efficient and show how surface chemistry dictates diverging CO2R surface reaction</div><div>mechanisms. The insights gained here are important as they provide the community with a greater</div><div>understanding of heterogeneous CO2R and can be further translated to a number of catalytic systems. </div>

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CO ₂ electrolysis to multicarbon products at activities greater than 1 A cm ⁻²

Cited by 1,103 publications

References 69 publications

A direct coupled electrochemical system for capture and conversion of CO2 from oceanwater

A direct coupled electrochemical system for capture and conversion of CO2 from oceanwater

Three-Dimensional Cathodes for Electrochemical Reduction of CO2: From Macro- to Nano-Engineering

Surface Chemistry Modulates CO2 Reduction Reaction Intermediates on Silver Nanoparticle Electrocatalysts

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CO 2 electrolysis to multicarbon products at activities greater than 1 A cm −2

Cited by 1,103 publications

References 69 publications

A direct coupled electrochemical system for capture and conversion of CO2 from oceanwater

A direct coupled electrochemical system for capture and conversion of CO2 from oceanwater

Three-Dimensional Cathodes for Electrochemical Reduction of CO2: From Macro- to Nano-Engineering

Surface Chemistry Modulates CO2 Reduction Reaction Intermediates on Silver Nanoparticle Electrocatalysts

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Product

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CO ₂ electrolysis to multicarbon products at activities greater than 1 A cm ⁻²