Heterogeneously catalyzed two-step cascade electrochemical reduction of CO2 to ethanol

Theaker, Nolan; Strain, Jacob M.; Kumar, Bijandra; Brian, J. Patrick; Kumari, Sudesh; Spurgeon, Joshua M.

doi:10.1016/j.electacta.2018.04.072

Cited by 58 publications

(39 citation statements)

References 49 publications

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“…Thus, a promising approach to mitigate the limitations of the CO 2 RR scaling relations is the further direct electrochemical reduction of CO in a second electrocatalytic system. Cascade electrolysis systems have been demonstrated by first reducing CO 2 to CO with Au or Ag, then subsequently flowing the CO to a second electrolyzer or catalyst for a more selective secondary reduction . With OD‐Cu, for instance, the grain boundary active sites promote adjacent CO binding and subsequent C−C bond formation, leading to higher FE for C 2 products such as ethanol and acetate compared to conventional Cu for the electrochemical CO reduction reaction (CORR) .…”

Section: Introductionmentioning

confidence: 99%

Pulsed Electrochemical Carbon Monoxide Reduction on Oxide‐Derived Copper Catalyst

et al. 2020

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Efficient electroreduction of carbon dioxide has been a widely pursued goal as a sustainable method to produce value‐added chemicals while mitigating greenhouse gas emissions. Processes have been demonstrated for the electroreduction of CO2 to CO at nearly 100 % faradaic efficiency, and as a consequence, there has been growing interest in the further electroreduction of carbon monoxide. Oxide‐derived copper catalysts have promising performance for the reduction of CO to hydrocarbons but have still been unable to achieve high selectivity to individual products. A pulsed‐bias technique is one strategy for tuning electrochemical selectivity without changing the catalyst. Herein a pulsed‐bias electroreduction of CO was investigated on oxide‐derived copper catalyst. Increased selectivity for single‐carbon products (i.e., formate and methane) was achieved for higher pulse frequencies (<1 s pulse times), as well as an increase in the fraction of charge directed to CO reduction rather than hydrogen evolution.

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Section: Introductionmentioning

confidence: 99%

Pulsed Electrochemical Carbon Monoxide Reduction on Oxide‐Derived Copper Catalyst

et al. 2020

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“…37 Recently, Spurgeon and co-workers have reported on a related, compartmentalized, approach for CO 2 R, using Ag and Cu in separate chambers to, respectively, produce CO and to convert CO to ethanol. 38 However, well less than 10% of the intermediate CO was converted in the upstream chamber due to mixing during the transport between the chambers. In contrast, we will show that closer positioning of the electrodes reduces diffusion losses of the intermediate such that much higher conversion rates can be attained.…”

Section: Introductionmentioning

confidence: 99%

Sequential Cascade Electrocatalytic Conversion of Carbon Dioxide to C–C Coupled Products

Gurudayal¹,

Perone

Malani³

et al. 2019

ACS Appl. Energy Mater.

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Cascade catalytic processes perform multi-step chemical transformations without isolating the intermediates. Here, we demonstrate a sequential cascade pathway to convert CO 2 to C 2+ hydrocarbons and oxygenates in a two-step electrocatalytic process using CO as the intermediate. CO 2 to CO conversion is performed by using Ag and further conversion of CO to CC coupled products is performed with Cu. Temporal separation between the two reaction steps is accomplished by situating the Ag electrode upstream of the Cu electrode in a continuous flow reactor. Convection-diffusion simulations and experimental evaluation of the electrodes individually were performed to identify optimal conditions. With the upstream Ag electrode poised at-1 V vs RHE in a flow of CO 2-saturated water in aqueous carbonate buffer, over 80% of the CO can be converted on the downstream Cu electrode. When the Ag electrode is on, a supersaturation of CO is achieved near the Cu electrode, which leads to a relative increase in the formation rate of C 2 and C 3 oxygenates as compared to ethylene.

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“…[106] Therefore, as long as this ratio is different between two competing pathways, the pH will serve to regulate the reaction selectivity. Going further, this may possibly even lead to a multi-step chemical conversion system, either as cascade catalysis, [107][108][109] or as several chemical reactors connected in series. This variability could allow specific reactions to proceed and concentrate in a certain niche environment.…”

Section: Usage Of Sequential Proton-electron Transfer (Spet) To Regulmentioning

confidence: 99%

“…This variability could allow specific reactions to proceed and concentrate in a certain niche environment. Going further, this may possibly even lead to a multi-step chemical conversion system, either as cascade catalysis, [107][108][109] or as several chemical reactors connected in series. This is a critical difference from previous origin of life theories such as the soup model and pond model, where no pH or potential gradients were available to guide the selectivity of prebiotic reactions.…”

Section: Usage Of Sequential Proton-electron Transfer (Spet) To Regulmentioning

confidence: 99%

Electrochemistry at Deep‐Sea Hydrothermal Vents: Utilization of the Thermodynamic Driving Force towards the Autotrophic Origin of Life

2019

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Temperature gradients are an under-utilized source of energy with which to drive chemical reactions. Here, we review our past efforts to understand how deep-sea hydrothermal vents may harness thermal energy to promote difficult chemical reactions such as CO 2 reduction. Strategies to amplify the driving force using temperature will be covered first, followed by a discussion on how spatially separated thermodynamic gradients can be used to regulate reaction selectivity. Although desirable material properties of hydrothermal vent walls have been inferred previously from the bioenergetic membranes of modern cells, strategies based on fundamental laws of physical chemistry allow naturally occurring chimney minerals to circumvent the lack of structural and catalytic optimization. The principles that underlie both the establishment and the utilization of the thermodynamic driving force at hydrothermal vents can be employed in abiotic systems such as the modern chemical industry, yielding insight into carbon fixation reactions important today and possibly at the autotrophic origin of life.

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Heterogeneously catalyzed two-step cascade electrochemical reduction of CO2 to ethanol

Cited by 58 publications

References 49 publications

Pulsed Electrochemical Carbon Monoxide Reduction on Oxide‐Derived Copper Catalyst

Pulsed Electrochemical Carbon Monoxide Reduction on Oxide‐Derived Copper Catalyst

Sequential Cascade Electrocatalytic Conversion of Carbon Dioxide to C–C Coupled Products

Electrochemistry at Deep‐Sea Hydrothermal Vents: Utilization of the Thermodynamic Driving Force towards the Autotrophic Origin of Life

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