Insights into the Low Overpotential Electroreduction of CO<sub>2</sub> to CO on a Supported Gold Catalyst in an Alkaline Flow Electrolyzer

Verma, Sumit; Hamasaki, Yuki; Kim, Chaerin; Huang, Wenxin; Lu, Shawn; Jhong, Huei Ru Molly; Gewirth, Andrew A.; Fujigaya, Tsuyohiko; Nakashima, Naotoshi; Kenis, Paul J. A.

doi:10.1021/acsenergylett.7b01096

Cited by 444 publications

(504 citation statements)

References 53 publications

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“…Using Co phthalocyanine as catalysts, we have shown that this dogma can be overcome by applying the complex into a flow cell, generating CO with 94 % selectivity at 165 mA cm −2 current density at basic pH (14) . Such performances approach those obtained with Ag‐ and Au‐based catalytic materials . However, the Co complex, like the above mentioned solid nano‐catalysts, operates at quite large overpotential, in the range of 800 mV at comparably current densities.…”

Section: Methodsmentioning

confidence: 89%

Iron Porphyrin Allows Fast and Selective Electrocatalytic Conversion of CO₂ to CO in a Flow Cell

Torbensen

Han

Boudy

et al. 2020

Chemistry A European J

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Molecular catalysts have been shown to have high selectivity for CO2 electrochemical reduction to CO, but with current densities significantly below those obtained with solid‐state materials. By depositing a simple Fe porphyrin mixed with carbon black onto a carbon paper support, it was possible to obtain a catalytic material that could be used in a flow cell for fast and selective conversion of CO2 to CO. At neutral pH (7.3) a current density as high as 83.7 mA cm−2 was obtained with a CO selectivity close to 98 %. In basic solution (pH 14), a current density of 27 mA cm−2 was maintained for 24 h with 99.7 % selectivity for CO at only 50 mV overpotential, leading to a record energy efficiency of 71 %. In addition, a current density for CO production as high as 152 mA cm−2 (>98 % selectivity) was obtained at a low overpotential of 470 mV, outperforming state‐of‐the‐art noble metal based catalysts.

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Section: Methodsmentioning

confidence: 89%

Iron Porphyrin Allows Fast and Selective Electrocatalytic Conversion of CO₂ to CO in a Flow Cell

Torbensen

Han

Boudy

et al. 2020

Chemistry A European J

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“…Prior to application the mixture was sonicated for 20 min. All the anodes had a final loading of 2.01 mg cm −2 …”

Section: Methodsmentioning

confidence: 99%

Electrodeposited Cu₂O Films on Gas Diffusion Layers for Selective CO₂ Electroreduction to Ethylene in an Alkaline Flow Electrolyzer

et al. 2019

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Novel electrodes for the electroreduction of CO2 were prepared by the electrodeposition of copper (I) oxide (Cu2O) catalytic films on a gas diffusion layer. Different electrodes were prepared by varying the deposition time, corresponding to catalyst loadings of 0.37, 0.74, 2.22, 3.70 mg cm−2 and a total charge density of 0.5, 1, 3, and 5 C cm−2, respectively. The electrodes were characterized with SEM, XRD, and UPD. The effect of catalyst loading on the selectivity towards ethylene was investigated in an alkaline flow electrolyzer under ambient conditions. The electrodes were found to be highly selective (>60 %) towards ethylene. The 1 C cm−2 electrode reached Faradaic efficiency values as high as 67 % at industrially relevant current densities of 183 mA cm−2, −0.8 V cathode overpotential and 36 % cell energy efficiency. This performance was attributed to the interplaying role of applied potential, local pH, availability of active sites, and reduced CO2 mass transport limitations.

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“…These include the development of structurally complex gas-diffusion electrodes for use in flow cells, [26,27] polymer electrolytes, [28,29] and ionicl iquids [30] that leverage tailorede lectrode-contacting phases to favor high CO 2 availability.I ns ome cases, these approaches rely on interfacial phenomena [31] or involve preparation of membraneelectrode assemblies. These include the development of structurally complex gas-diffusion electrodes for use in flow cells, [26,27] polymer electrolytes, [28,29] and ionicl iquids [30] that leverage tailorede lectrode-contacting phases to favor high CO 2 availability.I ns ome cases, these approaches rely on interfacial phenomena [31] or involve preparation of membraneelectrode assemblies.…”

Section: Introductionmentioning

confidence: 99%

Intensified Electrocatalytic CO₂ Conversion in Pressure‐Tunable CO₂‐Expanded Electrolytes

et al. 2019

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Multimolar CO2 concentrations are achieved in acetonitrile solutions containing supporting electrolyte at relatively mild CO2 pressures (<5 MPa) and ambient temperature. Such CO2‐rich, electrolyte‐containing solutions are termed as CO2‐eXpanded Electrolytes (CXEs) because significant volumetric expansion of the liquid phase accompanies CO2 dissolution. Cathodic polarization of a model polycrystalline gold electrode‐catalyst in CXE media enhances CO2 to CO conversion rates by up to an order of magnitude compared with those attainable at near‐ambient pressures, without loss of selectivity. The observed catalytic process intensification stems primarily from markedly increased CO2 availability. However, a non‐monotonic correlation between the dissolved CO2 concentration and catalytic activity is observed, with an optimum occurring at approximately 5 m CO2 concentration. At the highest applied CO2 pressures, catalysis is significantly attenuated despite higher CO2 concentrations and improved mass‐transport characteristics, attributed in part to increased solution resistance. These results reveal that pressure‐tunable CXE media can significantly intensify CO2 reduction rates over known electrocatalysts by alleviating substrate starvation, with CO2 pressure as a crucial variable for optimizing the efficiency of electrocatalytic CO2 conversion.

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Insights into the Low Overpotential Electroreduction of CO₂ to CO on a Supported Gold Catalyst in an Alkaline Flow Electrolyzer

Cited by 444 publications

References 53 publications

Iron Porphyrin Allows Fast and Selective Electrocatalytic Conversion of CO₂ to CO in a Flow Cell

Iron Porphyrin Allows Fast and Selective Electrocatalytic Conversion of CO₂ to CO in a Flow Cell

Electrodeposited Cu₂O Films on Gas Diffusion Layers for Selective CO₂ Electroreduction to Ethylene in an Alkaline Flow Electrolyzer

Intensified Electrocatalytic CO₂ Conversion in Pressure‐Tunable CO₂‐Expanded Electrolytes

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Insights into the Low Overpotential Electroreduction of CO2 to CO on a Supported Gold Catalyst in an Alkaline Flow Electrolyzer

Cited by 444 publications

References 53 publications

Iron Porphyrin Allows Fast and Selective Electrocatalytic Conversion of CO2 to CO in a Flow Cell

Iron Porphyrin Allows Fast and Selective Electrocatalytic Conversion of CO2 to CO in a Flow Cell

Electrodeposited Cu2O Films on Gas Diffusion Layers for Selective CO2 Electroreduction to Ethylene in an Alkaline Flow Electrolyzer

Intensified Electrocatalytic CO2 Conversion in Pressure‐Tunable CO2‐Expanded Electrolytes

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Product

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Insights into the Low Overpotential Electroreduction of CO₂ to CO on a Supported Gold Catalyst in an Alkaline Flow Electrolyzer

Iron Porphyrin Allows Fast and Selective Electrocatalytic Conversion of CO₂ to CO in a Flow Cell

Iron Porphyrin Allows Fast and Selective Electrocatalytic Conversion of CO₂ to CO in a Flow Cell

Electrodeposited Cu₂O Films on Gas Diffusion Layers for Selective CO₂ Electroreduction to Ethylene in an Alkaline Flow Electrolyzer

Intensified Electrocatalytic CO₂ Conversion in Pressure‐Tunable CO₂‐Expanded Electrolytes