Continuous electroconversion of CO2 into formate using 2 nm tin oxide nanoparticles

Merino-Garcia, Iván; Tinat, Lionel; Albo, Jonathan; Alvarez‐Guerra, Manuel; Irabien, Ángel; Durupthy, Olivier; Vivier, Vincent; Sánchez‐Sánchez, Carlos M.

doi:10.1016/j.apcatb.2021.120447

Cited by 38 publications

(30 citation statements)

References 71 publications

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“…Table 2 shows the overpotential, faradaic efficiencies obtained for both products, and energy efficiency for CO 2 conversion to formate as a function of the electrolyte composition, H 2 O content and either applied potential or current during electrolysis in acetonitrile solution (see Figure S5). As formate can partially migrate from the catholyte to the anolyte, [7] a systematic analysis of both catholyte and anolyte solutions was performed in all electrolysis reported here, proving that between 15 and 20 % of the total formate generated during the electrolysis was detected within the anolyte solution. Thus, analyzing the presence of reaction products in both compartments allowed closing quite efficiently the mass balance of the electrolysis reaching in most cases a total FE (FE

{{_{{\rm HCOO}{^{- }}}}}

+FE

{{_{{\rm H}{_{2}}}}}

) between 78 and 100 %.…”

Section: Resultssupporting

confidence: 54%

Electrocatalytic Conversion of CO₂ to Formate at Low Overpotential by Electrolyte Engineering in Model Molecular Catalysis

et al. 2022

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An electrolyte engineering strategy was developed for CO2 reduction into formate with a model molecular catalyst, [Rh(bpy)(Cp*)Cl]Cl, by modifying the solvent (organic or aqueous), the proton source (H2O or acetic acid), and the electrode/solution interface with imidazolium‐ and pyrrolidinium‐based ionic liquids (ILs). Experimental and theoretical density functional theory investigations suggested that π+‐π interactions between the imidazolium‐based IL cation and the reduced bipyridine ligand of the catalyst improved the efficiency of the CO2 reduction reaction (CO2RR) by lowering the overpotential, while granting partial suppression of the hydrogen evolution reaction. This allowed tuning the selectivity towards formate, reaching for this catalyst an unprecedented faradaic efficiency (FEHCOO−) ≥90 % and energy efficiency of 66 % in acetonitrile solution. For the first time, relevant CO2 conversion to formic acid/formate was reached at low overpotential (0.28 V) using a homogeneous catalyst in acidic aqueous solution (pH=3.8). These results open up a new strategy based on electrolyte engineering for enhancing carbon balance in CO2RR.

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{{_{{\rm HCOO}{^{- }}}}}

+FE

{{_{{\rm H}{_{2}}}}}

) between 78 and 100 %.…”

Section: Resultssupporting

confidence: 54%

Electrocatalytic Conversion of CO₂ to Formate at Low Overpotential by Electrolyte Engineering in Model Molecular Catalysis

et al. 2022

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“…Economically competitive application of the CO 2 RR technology needs to convert CO 2 at a high current density, whereas the reaction rate in a H-type cell is significantly limited by the low solubility of CO 2 in the electrolyte. − Therefore, the catalytic properties of these catalysts were further evaluated in a flow cell configuration. The LSV curves (Figures f and S18) reveal that the reaction rates in the flow cell are greatly accelerated both in KOH and KHCO 3 electrolytes.…”

Section: Resultsmentioning

confidence: 99%

Heterogeneous Structure of Sn/SnO₂ Constructed via Phase Engineering for Efficient and Stable CO₂ Reduction

Liu

Mao

et al. 2023

ACS Appl. Mater. Interfaces

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The electrochemical carbon dioxide reduction reaction (CO 2 RR) catalyzed by Sn-based materials shows great potential for CO 2 -to-formate conversion. The presence of tin species with different oxidation states can promote the catalytic performance, most likely due to the interfaces of metallic and oxide phases that induce a synergistic effect. Therefore, it is desirable yet challenging to synthesize a hybrid catalyst with abundant active heterogeneous interfaces. Herein, we synthesize a hybrid catalyst constructed by decorating nanosized SnS 2 in the SnO 2 matrix. The uniformly distributed SnS 2 nanoparticles are first reduced to metallic tin, which assists in the generation of abundant Sn/SnO 2 heterogeneous interfaces under the in situ reduction process. Because of the electronic modulation at the heterogeneous interfaces, the resulting catalyst delivers a high current density of 200 mA• cm −2 at −0.86 V vs RHE, and the performance is stable for over 20 h. This work suggests a potentially powerful interface engineering strategy for the development of high-performance electrocatalysts for the CO 2 RR.

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“…Tin-based catalysts are already well established among the preferred catalyst for the eCO 2 R toward the formate. Recently, it has been shown that the oxidized (IV) tin performed even better. − To analyze if this behavior remains in a bicarbonate electrolyzer, we have performed experiments with porous carbon on which either Sn or SnO 2 nanoparticles were deposited. The results displayed in Figure (left) show that at low current densities (10 mA cm –2 ), the FE Formate is slightly better on Sn (38%) versus SnO 2 (33%).…”

Section: Results and Discussionmentioning

confidence: 99%

Engineering Aspects for the Design of a Bicarbonate Zero-Gap Flow Electrolyzer for the Conversion of CO₂ to Formate

Gutiérrez-Sánchez

Mot

Bulut

et al. 2022

ACS Appl. Mater. Interfaces

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CO2 electrolyzers require gaseous CO2 or saturated CO2 solutions to achieve high energy efficiency (EE) in flow reactors. However, CO2 capture and delivery to electrolyzers are in most cases responsible for the inefficiency of the technology. Recently, bicarbonate zero-gap flow electrolyzers have proven to convert CO2 directly from bicarbonate solutions, thus mimicking a CO2 capture medium, obtaining high Faradaic efficiency (FE) and partial current density (CD) toward carbon products. However, since bicarbonate electrolyzers use a bipolar membrane (BPM) as a separator, the cell voltage (VCell) is high, and the system becomes less efficient compared to analogous CO2 electrolyzers. Due to the role of the bicarbonate both as a carbon donor and proton donor (in contrast to gas-fed CO2 electrolyzers), optimization by using know-how from conventional gas-fed CO2 electrolyzers is not valid. In this study, we have investigated how different engineering aspects, widely studied for upscaling gas-fed CO2 electrolyzers, influence the performance of bicarbonate zero-gap flow electrolyzers when converting CO2 to formate. The temperature, flow rate, and concentration of the electrolyte are evaluated in terms of FE, productivity, V Cell, and EE in a broad range of current densities (10–400 mA cm–2). A CD of 50 mA cm–2, room temperature, high flow rate (5 mL cm–2) of the electrolyte, and high carbon load (KHCO3 3 M) are proposed as potentially optimal parameters to benchmark a design to achieve the highest EE (27% is obtained this way), one of the most important criteria when upscaling and evaluating carbon capture and conversion technologies. On the other hand, at high CD (>300 mA cm–2), low flow rate (0.5 mL cm–2) has the highest interest for downstream processing (>40 g L–1 formate is obtained this way) at the cost of a low EE (<10%).

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Continuous electroconversion of CO2 into formate using 2 nm tin oxide nanoparticles

Cited by 38 publications

References 71 publications

Electrocatalytic Conversion of CO₂ to Formate at Low Overpotential by Electrolyte Engineering in Model Molecular Catalysis

Electrocatalytic Conversion of CO₂ to Formate at Low Overpotential by Electrolyte Engineering in Model Molecular Catalysis

Heterogeneous Structure of Sn/SnO₂ Constructed via Phase Engineering for Efficient and Stable CO₂ Reduction

Engineering Aspects for the Design of a Bicarbonate Zero-Gap Flow Electrolyzer for the Conversion of CO₂ to Formate

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Continuous electroconversion of CO2 into formate using 2 nm tin oxide nanoparticles

Cited by 38 publications

References 71 publications

Electrocatalytic Conversion of CO2 to Formate at Low Overpotential by Electrolyte Engineering in Model Molecular Catalysis

Electrocatalytic Conversion of CO2 to Formate at Low Overpotential by Electrolyte Engineering in Model Molecular Catalysis

Heterogeneous Structure of Sn/SnO2 Constructed via Phase Engineering for Efficient and Stable CO2 Reduction

Engineering Aspects for the Design of a Bicarbonate Zero-Gap Flow Electrolyzer for the Conversion of CO2 to Formate

Contact Info

Product

Resources

About

Electrocatalytic Conversion of CO₂ to Formate at Low Overpotential by Electrolyte Engineering in Model Molecular Catalysis

Electrocatalytic Conversion of CO₂ to Formate at Low Overpotential by Electrolyte Engineering in Model Molecular Catalysis

Heterogeneous Structure of Sn/SnO₂ Constructed via Phase Engineering for Efficient and Stable CO₂ Reduction

Engineering Aspects for the Design of a Bicarbonate Zero-Gap Flow Electrolyzer for the Conversion of CO₂ to Formate