Continuous Carbon Dioxide Electroreduction to Concentrated Multi-carbon Products Using a Membrane Electrode Assembly

Gabardo, Christine M.; O’Brien, Colin P.; Edwards, Jonathan P.; McCallum, Christopher; Xu, Yi; Dinh, Cao-Thang; Li, Jun; Sargent, Edward H.

doi:10.1016/j.joule.2019.07.021

Cited by 377 publications

(478 citation statements)

References 45 publications

(61 reference statements)

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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%

“…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 . The outlet CO 2 stream from the BPMED cell was directly fed through tandem vapor-fed cells, the first for oxygen reduction reaction (ORR) and second for CO 2 R. The first ORR pre-electrolysis cell was used to eliminate any residue O 2 from flowing into the vaporfed CO 2 R cell ( Supplementary Fig.…”

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

confidence: 99%

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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%

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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“…This requires the use of flow cells (Figure B) or zero‐gap cells (Figure C) . Both systems are inherently more efficient, as the reaction occurs at the triple phase boundary between CO 2,gas , the solid/liquid electrolyte, and the M‐N‐C catalytic layer, and thus the need for CO 2 dissolution is avoided.…”

Section: Toward Syngas Generation On An Industrial Scalementioning

confidence: 99%

“…[88] However, to avoid operating under such extreme alkaline conditions and to eliminate the losses induced by CO 2 dissolution/diffusion, providing the CO 2 in ah umidified gaseous phase appearsmandatory. [89] This requires the use of flow cells [90] (Figure4B) or zero-gap cells ( Figure 4C). [46,83,91,92] Both systems are inherently more efficient, as the reactiono ccurs at the triple phase boundary between CO 2,gas ,t he solid/liquid electrolyte, and the M-N-C catalytic layer,a nd thus the need for CO 2 dissolution is avoided.…”

Section: Toward Syngas Generation On An Industrial Scalementioning

confidence: 99%

Metal–Nitrogen–Carbon Electrocatalysts for CO₂ Reduction towards Syngas Generation

2020

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Shifting syngas (an H2/CO mixture) production away from fossil‐fuel‐dependent processes (e.g., steam methane reforming and coal gasification) is mandatory, as syngas is of interest as both a fuel and as a value‐added chemical precursor. With appropriate electrocatalysts, such as silver‐based and metal–nitrogen–carbon (M‐N‐C) materials, the electrochemical CO2 reduction reaction (CO2RR) allows for the production of CO alongside H2 (from the hydrogen evolution reaction), and thus leads to syngas generation. In this Minireview, the application of M‐N‐C electrocatalysts for syngas generation is discussed. The mechanisms leading to different faradaic selectivities for CO are reviewed as a function of the nature of the metal, by using both computational and experimental approaches. The role played by the metal‐free moieties in the M‐N‐C electrocatalysts is underlined. Since M‐N‐C electrocatalysts only recently entered the CO2RR field (as opposed to Cu‐, Ag‐, or Au‐based nanostructures), they have been mainly characterized in static liquid environments, in which the reaction rate is significantly hampered by CO2‐dissolution/diffusion limitations. Therefore, the design of CO2RR electrolyzers for M‐N‐C electrocatalysts is addressed, and designs such as zero‐gap electrolyzers with anionic membranes and humidified CO2 gas feed at the cathode are highlighted.

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“…Accordingly, publications focused on scale-up have begun to highlight electrolyzers which operate with high current densities, 18 large total currents, 19 and, to a lesser extent, enriched product streams. [20][21][22] As CO2R cell prototypes begin to traverse these new operating regimes, challenges can be anticipated due to shifts in chemical compatibility requirements for reactor components (catalysts, electrodes, periphery), significant deviations from low-concentration kinetic behavior, and greater process safety concerns arising from concentrated toxic products. Here, we elect to focus on irregularities expected to arise for gas diffusion electrodes (GDEs) while operating gas-fed CO2R devices at high liquid product generation rates as the other topics are more widely studied at present.…”

Section: Industrial Co 2 To Liquids Electrolyzers Will Move Beyond DImentioning

confidence: 99%

Flooded by Success: On the Role of Electrode Wettability in CO2 Electrolyzers That Generate Liquid Products

Leonard¹,

Orella²,

Aiello³

et al. 2020

Preprint

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The economic operation of carbon dioxide (CO2) electrolyzers generating liquid products will likely require high reactant conversions and high product concentrations, conditions anticipated to challenge existing gas diffusion electrodes (GDEs). Notably, electrode wettability will increase as lower surface tension products (e.g., formic acid, methanol, ethanol, and 1-propanol) are introduced into flowing electrolyte streams potentially leading to flooding. To better understand the hydraulically stable electrolyzer operating envelopes in mixed aqueous-organic liquid domains, we connect intrinsic porous electrode wettability descriptors to system operating parameters such as electrolyte flow rate and applied current. Specifically, we first measure contact angles of various water-organic dilutions on polytetrafluoroethylene (PTFE) and graphite surfaces as ex situ planar analogues for the major GDE components. We then use material balances around the reactive gas-liquid interface, to calculate product mass fractions as a function of liquid water sweep rate (water source and diluent) and the total current. Product composition maps enable visualization of the extent to which changes in cell performance can lead to changes in capillary pressure, a crucial determinant of GDE saturation. These analyses reveal that formic acid product mixtures pose little risk for GDE flooding across a wide range of flow rate and current combinations, but that effluents enriched with less than 30% alcohols content by mass may cause flooding. This study provides initial guidance into estimating flooding conditions for PTFE-based GDEs in contact with organic-enriched streams and indicates opportunities for oleophobic surface treatments that repel aqueous and organic liquids, expanding regions of stable operation<br>

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Continuous Carbon Dioxide Electroreduction to Concentrated Multi-carbon Products Using a Membrane Electrode Assembly

Cited by 377 publications

References 45 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

Metal–Nitrogen–Carbon Electrocatalysts for CO₂ Reduction towards Syngas Generation

Flooded by Success: On the Role of Electrode Wettability in CO2 Electrolyzers That Generate Liquid Products

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Continuous Carbon Dioxide Electroreduction to Concentrated Multi-carbon Products Using a Membrane Electrode Assembly

Cited by 377 publications

References 45 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

Metal–Nitrogen–Carbon Electrocatalysts for CO2 Reduction towards Syngas Generation

Flooded by Success: On the Role of Electrode Wettability in CO2 Electrolyzers That Generate Liquid Products

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Metal–Nitrogen–Carbon Electrocatalysts for CO₂ Reduction towards Syngas Generation