Achieving high current density for electrocatalytic reduction of CO2 to formate on bismuth-based catalysts

Fan, Tingting; Ma, Wenchao; Xie, Mingcan; Liu, Huan; Zhang, Ji‐Guang; Yang, S. L.; Huang, Pingping; Dong, Yuanyuan; Chen, Zhou; Yi, Xiaodong

doi:10.1016/j.xcrp.2021.100353

Cited by 51 publications

(56 citation statements)

References 48 publications

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“…In gas-fed electrolyzers the rate of CO 2 RR is not limited by slow CO 2 mass transport, and as a consequence, much higher applied overpotentials (or current densities) can be achieved, while still maintaining high formate selectivity. [54][55]58 In the present study, we demonstrate that an accelerated mass transport of gaseous CO 2 not only boosts the formate production to values beyond PCD formate = -1 A cm -2 but can also lead to a substantial stabilization of subcarbonate phases beyond the stability regime observed in classical CO 2 RR test environments. 38 Our experimental results strongly suggest that observations previously made using H-type cell configurations cannot simply be transferred to experimental conditions realized in practical gas-fed electrolyzers.…”

Section: Introductionsupporting

confidence: 52%

CO2 Conversion at High Current Densities: Stabilization of Bi(III) Containing Electrocatalysts under CO2 Gas Flow Conditions

Montiel

Dutta

Kiran

et al. 2022

Preprint

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Herein, we demonstrate the superior performance of novel bismuth subcarbonate ((BiO)2CO3) film catalysts for formate production using a fluidic CO2-fed electrolyzer device. The subcarbonate catalyst readily forms in situ from a CO2-absorbing Bi2O3 precursor material during the CO2 reduction reaction (CO2RR). In 1 mol dm–3 KOH electrolyte solution, a maximum Faradaic efficiency of FEformate = 97.4% (corresponding partial current density of formate formation: PCDformate = –111.6 mA cm–2) was achieved at a comparably low applied electrolysis potential of –0.8 V versus the reversible hydrogen electrode (RHE). Even higher values of PCDformate = –441.2 mA cm–2 (FEformate = 62%) were observed at more cathodic potential, –2.5 V vs. RHE. As the alkalinity of the liquid electrolyte is further increased (e.g., by using 5 mol dm–3 KOH solution), the performance of formate production is boosted beyond PCDformate values of –1 A cm–2. Combined X-ray diffraction and Raman spectroscopic investigations demonstrate an extraordinarily high stability of Bi(III) cations in the catalytically active subcarbonate catalyst phase down to cathode potentials of –1.5 V vs. RHE. This stabilization effect can clearly be attributed to the high abundance of gaseous CO2 under the operating conditions of the gas-fed electrolyzer. In the absence of any CO2 supply, however, the reductive Bi(III)-to-Bi(0) transition already occurs at much milder conditions of –0.3 V vs. RHE, as evidenced by in situ Raman spectroscopy in CO2-free 1 mol dm–3 KOH electrolyte solution. Advanced X-ray diffraction computed tomography (XRD-CT) technique was applied to gain deeper insights into the spatial distribution of the metallic and subcarbonate phases comprising the active composite catalyst layer (CL) during the CO2RR.

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Section: Introductionsupporting

confidence: 52%

CO2 Conversion at High Current Densities: Stabilization of Bi(III) Containing Electrocatalysts under CO2 Gas Flow Conditions

Montiel

Dutta

Kiran

et al. 2022

Preprint

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“…Considering that the current density cannot reach 200 mA cm -2 in a traditional H-type cell, we designed a flow cell with a gas diffusion electrode (GDE) as depicted in Figure 6a and Figure S34, Supporting Information. [29] The GDE can reduce the mass transfer resistance by accelerating the CO 2 diffusion rate on the cathode surface, thereby increasing the current density of the CO 2 RR process. [30] LSV and chronopotentiometry measurements were conducted to evaluate the catalytic performance of the three catalysts in 1 m KOH electrolyte, and the solution resistance (Rs) and iR compensation of flow cell were given in Table S6, Supporting Information.…”

Section: Flow Cell Performancementioning

confidence: 99%

Electro‐Reconstruction‐Induced Strain Regulation and Synergism of Ag‐In‐S toward Highly Efficient CO₂ Electrolysis to Formate

Zhang

Fan

Huang

et al. 2022

Adv Funct Materials

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Formate production from direct CO2 electrolysis is economically appealing yet challenging in activity, selectivity, and stability. Herein, sulfur and silver dual‐decorated indium quasi‐core–shell structures with compressive or tensile strain are rationally designed for efficiently electrocatalyzing CO2 to formate. The introduction of Ag and S increases the current density, Faradaic efficiency, and operational stability of formate both in H‐cell and flow cell systems. As a result, the optimized Ag‐In‐S bimetallic catalysts exhibit the FEHCOO− of ≈94.0% with a JHCOO− of more than −560.0 mA cm−2 at ≈−0.951 VRHE in the flow cell system, which far surpasses the undecorated In catalyst. The experimental and theoretical calculations provide a deeper understanding of the role of the interfacial strain between In or In4Ag9 shell and AgIn2 core in boosting the electrocatalytic CO2 reduction efficiency, in which the formation energy of *OCHO intermediate decreases and the charge transfer rate is accelerated by interface strain.

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“…Weekes et al 222 and Endrődi et al 223 discussed the role of cell architecture in the electroreduction of CO2, while more detailed aspects are out of the scope as well as the analysis of the recent development in electrocatalytic CO2 reduction, which for formate production from CO2 reached recently extremely high current densities (~930 mA•cm -2 ) with high Faradaic efficiency (FEHCOO-= 93%) on defective Bi2O2CO3 nanosheets. 227 While thus high J and FE are possible in the electrocatalytic approach (with an external source of potential and electrical current), the direct integration of a photoactive element in the device (photoanode, PV cell) allows largely lower J values, although with other advantages as earlier discussed.…”

Section: The Case Of Co2mentioning

confidence: 97%

Current density in solar fuel technologies

Romano

D’Angelo

Perathoner

2021

Energy Environ. Sci.

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Achieving high current density for electrocatalytic reduction of CO2 to formate on bismuth-based catalysts

Cited by 51 publications

References 48 publications

CO2 Conversion at High Current Densities: Stabilization of Bi(III) Containing Electrocatalysts under CO2 Gas Flow Conditions

CO2 Conversion at High Current Densities: Stabilization of Bi(III) Containing Electrocatalysts under CO2 Gas Flow Conditions

Electro‐Reconstruction‐Induced Strain Regulation and Synergism of Ag‐In‐S toward Highly Efficient CO₂ Electrolysis to Formate

Current density in solar fuel technologies

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Achieving high current density for electrocatalytic reduction of CO2 to formate on bismuth-based catalysts

Cited by 51 publications

References 48 publications

CO2 Conversion at High Current Densities: Stabilization of Bi(III) Containing Electrocatalysts under CO2 Gas Flow Conditions

CO2 Conversion at High Current Densities: Stabilization of Bi(III) Containing Electrocatalysts under CO2 Gas Flow Conditions

Electro‐Reconstruction‐Induced Strain Regulation and Synergism of Ag‐In‐S toward Highly Efficient CO2 Electrolysis to Formate

Current density in solar fuel technologies

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Electro‐Reconstruction‐Induced Strain Regulation and Synergism of Ag‐In‐S toward Highly Efficient CO₂ Electrolysis to Formate