In Situ ATR–SEIRAS of Carbon Dioxide Reduction at a Plasmonic Silver Cathode

Corson, Elizabeth R.; Kaş, Recep; Kostecki, Robert; Urban, Jeffrey J.; Smith, Wilson A.; McCloskey, Bryan D.; Kortlever, Ruud

doi:10.1021/jacs.0c01953

Cited by 76 publications

(79 citation statements)

References 68 publications

(278 reference statements)

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“…[ 7–11 ] Metal electrode is considered as an ideal candidate for electrocatalytic CO 2 reduction considering its good chemical stability, high catalytic activity, and eco‐friendly properties. [ 12–15 ] Gold (Au), silver (Ag), and palladium (Pd) have been commonly reported as catalyst electrodes for CO 2 reduction reaction due to their relatively weak CO (*CO) binding abilities on the surface compared with H 2 evolution catalyst such as Pt. [ 16–18 ] Compared with Au and Pd, the relatively lower cost and higher abundance of Ag makes it a more promising candidate for commercial applications.…”

Section: Introductionmentioning

confidence: 99%

In Situ Growth and Activation of Ag/Ag₂S Nanowire Clusters by H₂S Plasma Treatment for Promoted Electrocatalytic CO₂ Reduction

Yang

et al. 2021

Advanced Sustainable Systems

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Nonmetallic activation of metal electrodes is effective and universal to improve the catalytic activity for the CO2 reduction reaction. Here, selective electrocatalytic reduction of CO2 is performed on a plasma‐activated Ag/Ag2S catalyst for the first time. By a facile H2S plasma treatment on Ag foil and subsequent electrochemical prereduction, Ag/Ag2S nanowire clusters are obtained in situ with different sizes. High Faradaic efficiency for CO generation on Ag/Ag2S is shifted to a significantly lower overpotential compared with untreated Ag foil with high current density. Density functional theory studies reveal that the promoted catalytic activity can be ascribed to the enhanced CO2 activation and reduced reaction energy barrier of the limiting step.

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Section: Introductionmentioning

confidence: 99%

In Situ Growth and Activation of Ag/Ag₂S Nanowire Clusters by H₂S Plasma Treatment for Promoted Electrocatalytic CO₂ Reduction

Yang

et al. 2021

Advanced Sustainable Systems

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“…[26] The peak at 1970 cm −1 indicated the formation of CO from CO 2 RR. [27] Based on the results and previous researches, the proposed mechanism for the CO 2 RR to formate is shown in Figure 4d. [6c,7b,9,14,26,28] Appropriate copper chloride and PB precursor can form rich Cu/C heterogenous interfaces after annealing at high temperature.…”

Section: Resultsmentioning

confidence: 96%

Copper/Carbon Heterogenous Interfaces for Enhanced Selective Electrocatalytic Reduction of CO₂ to Formate

Xin

Dong

et al. 2021

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bismuth-, [5,7] and tin-based [8] electrodes, the low abundance and uneven distribution of the respective elements result in a high cost. Cu is an Earth abundant element and has a considerably lower price. [9] Recent studies revealed that formate could be generated over metallic Cu catalysts via CO 2 RR, while it is always accompanied by the production of other products. To improve the performance of Cu-based catalyst for formate production, an effective approach was to design Cu-based heterostructures. [10] Cu-Au bimetallic catalyst showed an outstanding formate Faradaic efficiency (FE) of 81% and a formate current density (j formate ) of 10.4 mA cm −2 for formate at −0.6 V versus reversible hydrogen electrode (RHE). [11] Wang et al. reported a CuS/Cu 2 O catalyst which exhibited FE of 67.6% for formate production with current density of 15.3 mA cm −2 at the given potential −0.9 V versus RHE. [9] On cobaltdecorated Cu thin films, formate could be formed with FE of 80% and the current density of 1.1 mA cm −2 at −0.65 V versus RHE. [12] Carbon-supported copper catalysts also were used to produce formate via CO 2 RR, [3,13] and it has been well known that electrocatalytic performance not only depends on the morphologic and structural characteristics of metal particles, but also the properties of the carbon substrates. Metal-organic frameworks (MOFs) are one of the attractive carbon precursors which have been widely used to fabricate the hybrid catalysts containing metal (oxides) nanoparticles and porous carbon materials. MOF-derived Cu 2 O/Cu nanospheres anchored in nitrogen-doped hollow porous carbon hybrid composites (Cu 2 O/ Cu@NC) exhibited FE of 70.5% for formate production with current density of below 10 mA cm −2 at −0.68 V versus RHE. [14] Yang et al. presented a catalyst of Cu nanoparticles embedded in carbon substrate for CO 2 RR to formate with FE of 78% and current density of 6 mA cm −2 at −1.2 V versus RHE. [15] In spite of these impressive efforts, the current density of CO 2 to formate over Cu-based catalysts is always very low. A current density of 65.8 mA cm −2 at −1.8 V versus Ag/Ag + was observed with an FE to formic acid of 90.5% over MOFs-decorated Cu cathode in the electrolytes containing ionic liquid, organic solvent, and H 2 O. [16] However, the utilization of organic solvent and ionic liquid increases the preparation cost, and the volatilization of acetonitrile may lead to the loss of electrolyte. Therefore, developing a Cu-based electrocatalyst with high formate selectivity and activity under the aqueous media remains a great challenge.Herein, we developed a hybrid composite electrocatalyst including Cu 2 O, Cu, and nitrogen-doped carbon (HCS/Cu), Electrochemical reduction of CO 2 (CO 2 RR) to formate is a promising route to prepare value-added chemical. Developing low-cost and efficient electrocatalysts with high product selectivity is still a grand challenge. Herein, a novel Cu anchored on hollow carbon spheres catalysts (HCS/Cu-x, x represents the mass of CuCl 2 added in the system) ...

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“…This is consistent with the conclusion from the ATR-SEIRAS report that light enhanced the CO desorption from the Ag surface rather than influencing the reaction pathway. [35] However, this data alone cannot conclusively identify the reaction pathway nor discount that the reaction mechanism in the light may be a different first-order pathway than that in the dark.…”

Section: Reaction Ordermentioning

confidence: 86%

“…However, an attenuated total reflectance surface-enhanced infrared absorption spectroscopy (ATR-SEIRAS) study showed no shift in the peak position of adsorbed CO 2 upon illumination (365 nm LED, 125 mW cm −2 ) of a plasmonically active Ag cathode during CO 2 reduction in 0.1 M KHCO 2 at -0.6 or -0.7 V RHE . [35] The CO 2 peak position additionally did not shift in the dark with potential from -0.7 to -0.9…”

Section: Reaction Order Trends With Applied Potentialmentioning

confidence: 89%

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Effect of pressure and temperature on carbon dioxide reduction at a plasmonically active silver cathode

Corson

Creel

Kostecki

et al. 2021

Electrochimica Acta

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Carbon dioxide reduction at a plasmonically active silver cathode was investigated by varying the pressure and temperature at multiple applied potentials under both dark and illuminated conditions to understand the mechanism of selectivity changes driven by plasmon-enhanced electrochemical conversion. Carbon dioxide partial pressures (P CO2 ) from 0.2 to 1 atm were studied during linear sweep voltammetry and chronoamperometry at -0.7, -0.9, and -1.1 V RHE . At a given applied overpotential the total current density increased with increasing P CO2 in both the dark and the light, but there were significant differences in the Tafel behavior between dark and illuminated conditions. The reduction of CO 2 to carbon monoxide (CO) was found to have first-order behavior with respect to P CO2 at all applied potentials in both the dark and the light, likely indicating no change in the rate-determining step upon illumination. Activity for the hydrogen (H 2 ) evolution reaction decreased with increasing P CO2 at slightly different rates in the dark and the light at each applied potential, making it unclear if light is influencing CO or H 2 intermediate adsorbate coverage. Both formate and methanol production showed no dependence on P CO2 under any conditions, but the true reaction orders may be masked by the much higher activity for CO and H 2 at the silver cathode. The investigation of product distribution with temperature at 14, 22, and 32°C at -0.7, -0.9, and -1.1 V RHE in both the dark and the light demonstrated that the selectivity changes observed upon illumination are not caused by local heating of the cathode surface.

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In Situ ATR–SEIRAS of Carbon Dioxide Reduction at a Plasmonic Silver Cathode

Cited by 76 publications

References 68 publications

In Situ Growth and Activation of Ag/Ag₂S Nanowire Clusters by H₂S Plasma Treatment for Promoted Electrocatalytic CO₂ Reduction

In Situ Growth and Activation of Ag/Ag₂S Nanowire Clusters by H₂S Plasma Treatment for Promoted Electrocatalytic CO₂ Reduction

Copper/Carbon Heterogenous Interfaces for Enhanced Selective Electrocatalytic Reduction of CO₂ to Formate

Effect of pressure and temperature on carbon dioxide reduction at a plasmonically active silver cathode

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In Situ ATR–SEIRAS of Carbon Dioxide Reduction at a Plasmonic Silver Cathode

Cited by 76 publications

References 68 publications

In Situ Growth and Activation of Ag/Ag2S Nanowire Clusters by H2S Plasma Treatment for Promoted Electrocatalytic CO2 Reduction

In Situ Growth and Activation of Ag/Ag2S Nanowire Clusters by H2S Plasma Treatment for Promoted Electrocatalytic CO2 Reduction

Copper/Carbon Heterogenous Interfaces for Enhanced Selective Electrocatalytic Reduction of CO2 to Formate

Effect of pressure and temperature on carbon dioxide reduction at a plasmonically active silver cathode

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In Situ Growth and Activation of Ag/Ag₂S Nanowire Clusters by H₂S Plasma Treatment for Promoted Electrocatalytic CO₂ Reduction

In Situ Growth and Activation of Ag/Ag₂S Nanowire Clusters by H₂S Plasma Treatment for Promoted Electrocatalytic CO₂ Reduction

Copper/Carbon Heterogenous Interfaces for Enhanced Selective Electrocatalytic Reduction of CO₂ to Formate