Enhancing C<sub>≥2</sub> product selectivity in electrochemical CO<sub>2</sub> reduction by controlling the microstructure of gas diffusion electrodes

Bernasconi, Francesco; Senocrate, Alessandro; Kraus, Peter; Battaglia, Corsin

doi:10.1039/d3ey00140g

Cited by 10 publications

(6 citation statements)

References 37 publications

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“…The base case was derived from the lab-scale report of CO 2 coelectrolysis using gas diffusion electrodes (GDEs) and a cation exchange membrane to separate the two liquid chambers on the cathode and anode side, avoiding product crossover. The lab-scale results reported by F. Bernasconi et al (details in Section S4.2 in the Supporting Information) were extrapolated to a larger scale of 100 m 2 electrode active area, corresponding to C 2 H 4 production of approximately 0.2 tonnes/day. These quantities should be sufficient to achieve economies of scale for downstream separation processes in C 2 H 4 production .…”

Section: Methods and Process Descriptionmentioning

confidence: 99%

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From CO₂ to Sustainable Aviation Fuel: Navigating the Technology Landscape

Hirunsit,

Senocrate,

Gómez-Camacho

et al. 2024

ACS Sustainable Chem. Eng.

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Sustainable jet fuel plays a crucial role in reducing aviation's carbon footprint, offering a promising approach toward net-zero emissions in the aviation sector. This work investigates pathways for producing jet fuels directly from CO 2 . Given the early stage of many direct CO 2 utilization technologies, identifying promising pathways is essential. Our investigation focuses on the three most important routes for jet fuel production, each of which employs a distinct intermediate compound. These routes are the reverse water−gas shift and Fischer−Tropsch (RWGS-FT) route, the methanol route, and the CO 2 electrolysis route, which employ syngas, methanol, and ethylene as key intermediates, respectively. By performing comprehensive process simulations and analyzing the resulting energy intensity and thermal and CO 2 efficiency of each route, these findings provide quantitative early-stage evaluations and allow us to identify key technical development requirements. Our results indicate that the methanol route exhibits the lowest energy intensity, followed by the RWGS-FT and CO 2 electrolysis routes. H 2 production accounts for a significant share of the energy demand for the RWGS-FT and methanol routes. The RWGS-FT route shows the lowest CO 2 efficiency, while the methanol route achieves 92% CO 2 efficiency including recycle streams, highlighting its potential for jet fuel production. Furthermore, the CO 2 electrolysis route holds the potential to achieve close to 100% CO 2 efficiency and requires significantly less H 2 feedstock. However, it faces challenges of a high energy demand. In addition, our study investigates key effects of potential technology optimization, providing a guideline for research and technology optimization.

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Section: Methods and Process Descriptionmentioning

confidence: 99%

“…Furthermore, the direct electrochemical reduction of CO 2 to C 2 H 4 has shown promising results at the laboratory scale − and is considered a subprocess in the third route. This technology is still in an early stage of development, with low TRL.…”

Section: Introductionmentioning

confidence: 99%

From CO₂ to Sustainable Aviation Fuel: Navigating the Technology Landscape

Hirunsit,

Senocrate,

Gómez-Camacho

et al. 2024

ACS Sustainable Chem. Eng.

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“…In this study, we solve this discrepancy by using operando synchrotron wide-angle X-ray scattering (WAXS) to provide unambiguous experimental proof of (bi)carbonate precipitation during CO 2 RR even in strongly acidic electrolytes (pH 1) in polymer-based Ag and Cu GDEs. , This finding, along with the observation of catalyst’s secondary phases that are unstable in acidic electrolytes (e.g., AgCO 3 , CuCO 3 , Cu 2 (OH) 2 CO 3 ), provides strong evidence that the local pH close to the catalyst is basic even in acidic electrolytes. Linear scan voltammetry experiments coupled with product analysis confirm that when lowering electrolyte pH (from 4.5 to 0.7), a progressively higher current density is required to achieve the activation of the CO 2 RR, with H 2 being the only product detected at current densities below the threshold values, consistent with a local pH increase in the vicinity of the catalyst.…”

Section: Introductionmentioning

confidence: 99%

“…In this study, we solve this discrepancy by using operando synchrotron wide-angle X-ray scattering (WAXS) to provide unambiguous experimental proof of (bi)carbonate precipitation during CO 2 RR even in strongly acidic electrolytes (pH 1) in polymer-based Ag and Cu GDEs. 25,26 This finding, along with the observation of catalyst's secondary phases that are unstable in acidic electrolytes (e.g., AgCO 3 , CuCO confirm that when lowering electrolyte pH (from 4.5 to 0.7), a progressively higher current density is required to achieve the activation of the CO 2 RR, with H 2 being the only product detected at current densities below the threshold values, consistent with a local pH increase in the vicinity of the catalyst. A comparison between electrolytes with neutral and acidic pH (4.5 and 1) shows a similar correlation between (bi)carbonate precipitation and loss of selectivity over time.…”

Section: ■ Introductionmentioning

confidence: 99%

“…■ METHODS GDE substrates were prepared by electrospinning solutions of 15 wt % poly(vinyliden-fluoride-co-hexafluorpropylene) (PVDF-HFP) in a 1 wt % solution of tetraethylammonium bromide (TEABr) in dimethylformamide (DMF) at 30 kV as previously reported. 26 These substrates were used to prepare GDEs by single-sided deposition of a Ag or Cu catalyst layer with a nominal thickness of 500 nm, employing physical vapor deposition (magnetron sputtering). Ag and Cu GDE product selectivity and activity during CO 2 RR were assessed in a three-compartment electrochemical cell.…”

Section: ■ Introductionmentioning

confidence: 99%

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Operando Observation of (Bi)carbonate Precipitation during Electrochemical CO₂ Reduction in Strongly Acidic Electrolytes

Bernasconi,

Plainpan,

Mirolo

et al. 2024

ACS Catal.

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Precipitation of (bi)carbonate salts during the electrochemical CO2 reduction (CO2RR) has been identified as a major cause of degradation and one of the main challenges to be overcome before implementing this technology on the industrial scale. Recently, the use of acidic electrolytes has been suggested as a promising strategy to avoid this undesirable precipitation of carbonates and maximize the conversion of CO2 into valuable products. However, direct experimental evidence supporting this claim, as well as an understanding of degradation mechanisms in acidic electrolytes, is currently missing. In this study, we use operando synchrotron wide-angle X-ray scattering to provide unambiguous experimental proof that substantial (bi)carbonate precipitation takes place in Ag and Cu gas diffusion electrodes (GDEs) during CO2RR even in strongly acidic electrolytes (pH 1). The (bi)carbonate signal intensity increases over time, correlating with a loss of selectivity for carbon products and an increased level of H2 production. Electrochemical measurements coupled with products analysis also show that a minimum current is required to activate the CO2RR and suppress hydrogen evolution and that this current is higher for more acidic electrolytes. These findings provide experimental evidence for high local pH close to the catalyst even in acidic electrolytes. Our results confirm that the CO2RR performed in an acidic electrolyte can yield high selectivity to carbon products, provided sufficiently large current densities are applied to provoke local proton depletion in the vicinity of the catalyst, but that detrimental (bi)carbonate precipitation and selectivity losses occur even under these conditions.

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State‐of‐the‐Art CO₂ Reduction in Electrochemical Microfluidic Systems: A Short Review and New Perspectives

Abdul Ali,

Rodrigues Zanata,

Alves Martins

2024

ChemNanoMat

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The need to mitigate carbon dioxide has motivated an influx of interest in innovative technologies, and microfluidic systems have emerged as a promising forefront in this endeavor. This short review analyzes CO2 reduction within microfluidic platforms, thoroughly investigating existing methodologies, challenges, and novel perspectives. This work commences with a detailed exposition of the fundamental principles governing microfluidic electrolyzers, elucidating the interaction of microchannels and electrodes. We show the electrochemical reactions supporting CO2 reduction, detailing the processes at the cathode. The use of microfluidic systems encompasses precise control over reaction conditions, efficient mass transport, reduced energy consumption, high throughput screening capabilities, integration with analytical tools, and portability. Catalyst selection for optimal CO2 reduction products, technical complexities, integration of renewable energy sources, and cost‐effectiveness are notable challenges on the horizon. A perspective on potential pathways to resolution is delineated, with each impediment succinctly but insightfully addressed. Moreover, this review extends beyond a looking‐back analysis, propounding innovative perspectives. It posits the concept of microfluidic fuel cells directly fueled by CO2. This work seeks to inspire new researchers and innovation in the field by comparing the present state‐of‐the‐art with prospective avenues of exploration

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Enhancing C_≥2 product selectivity in electrochemical CO₂ reduction by controlling the microstructure of gas diffusion electrodes

Abstract: Cu gas diffusion electrodes based on hydrophobic polymer substrates show an enhanced selectivity towards C2H4 and C≥2 products during the electrochemical reduction of CO2 upon decreasing substrate pore size.

Cited by 10 publications

References 37 publications

From CO₂ to Sustainable Aviation Fuel: Navigating the Technology Landscape

From CO₂ to Sustainable Aviation Fuel: Navigating the Technology Landscape

Operando Observation of (Bi)carbonate Precipitation during Electrochemical CO₂ Reduction in Strongly Acidic Electrolytes

State‐of‐the‐Art CO₂ Reduction in Electrochemical Microfluidic Systems: A Short Review and New Perspectives

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Enhancing C≥2 product selectivity in electrochemical CO2 reduction by controlling the microstructure of gas diffusion electrodes

Abstract: Cu gas diffusion electrodes based on hydrophobic polymer substrates show an enhanced selectivity towards C2H4 and C≥2 products during the electrochemical reduction of CO2 upon decreasing substrate pore size.

Cited by 10 publications

References 37 publications

From CO2 to Sustainable Aviation Fuel: Navigating the Technology Landscape

From CO2 to Sustainable Aviation Fuel: Navigating the Technology Landscape

Operando Observation of (Bi)carbonate Precipitation during Electrochemical CO2 Reduction in Strongly Acidic Electrolytes

State‐of‐the‐Art CO2 Reduction in Electrochemical Microfluidic Systems: A Short Review and New Perspectives

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Product

Resources

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Enhancing C_≥2 product selectivity in electrochemical CO₂ reduction by controlling the microstructure of gas diffusion electrodes

From CO₂ to Sustainable Aviation Fuel: Navigating the Technology Landscape

From CO₂ to Sustainable Aviation Fuel: Navigating the Technology Landscape

Operando Observation of (Bi)carbonate Precipitation during Electrochemical CO₂ Reduction in Strongly Acidic Electrolytes

State‐of‐the‐Art CO₂ Reduction in Electrochemical Microfluidic Systems: A Short Review and New Perspectives