Tin Oxide Dependence of the CO<sub>2</sub> Reduction Efficiency on Tin Electrodes and Enhanced Activity for Tin/Tin Oxide Thin-Film Catalysts

Chen, Yihong; Kanan, Matthew W.

doi:10.1021/ja2108799

Cited by 908 publications

(891 citation statements)

References 29 publications

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“…36). However, for np-Ag, the Tafel slope of 58 mV dec À 1 indicates a fast initial electron transfer step before a later non-electron transfer rate-determining step 15,36,37 , which proves that the np-Ag surfaces are able to stabilize the CO 2 À intermediate much better than a flat surface. Therefore, the dramatic decrease in Tafel slope for np-Ag indicates that, in addition to 150 times larger electrochemical surface area, np-Ag is also intrinsically better than polycrystalline Ag for CO 2 reduction at moderate overpotentials.…”

Section: Discussionmentioning

confidence: 94%

A selective and efficient electrocatalyst for carbon dioxide reduction

et al. 2014

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Converting carbon dioxide to useful chemicals in a selective and efficient manner remains a major challenge in renewable and sustainable energy research. Silver is an interesting electrocatalyst owing to its capability of converting carbon dioxide to carbon monoxide selectively at room temperature; however, the traditional polycrystalline silver electrocatalyst requires a large overpotential. Here we report a nanoporous silver electrocatalyst that is able to electrochemically reduce carbon dioxide to carbon monoxide with approximately 92% selectivity at a rate (that is, current) over 3,000 times higher than its polycrystalline counterpart under moderate overpotentials of o0.50 V. The high activity is a result of a large electrochemical surface area (approximately 150 times larger) and intrinsically high activity (approximately 20 times higher) compared with polycrystalline silver. The intrinsically higher activity may be due to the greater stabilization of CO 2 À intermediates on the highly curved surface, resulting in smaller overpotentials needed to overcome the thermodynamic barrier.

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Section: Discussionmentioning

confidence: 94%

A selective and efficient electrocatalyst for carbon dioxide reduction

et al. 2014

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“…57 There has also been substantial interest in high surface area Cu-based catalysts for CO 2 reduction, and in particular those derived from the reduction of oxidized Cu. 4,7,[58][59][60][61][62][63][64] It has been reported that pre-oxidized Cu catalysts exhibit an exceptionally high activity for producing multi-carbon products, such as C 2 H 4 and C 2 H 5 OH. These studies have stimulated efforts aimed at understanding the origin of the seemingly superior catalytic activity of these oxide-derived catalysts compared to polycrystalline Cu foils.…”

Section: ‫ܣܥܵܧ‬ = ‫ܥ‬ ‫ܥ‬ ோாிmentioning

confidence: 99%

Standards and Protocols for Data Acquisition and Reporting for Studies of the Electrochemical Reduction of Carbon Dioxide

et al. 2018

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Objective evaluation of the performance of electrocatalysts for CO 2 reduction has been complicated by a lack of standardized methods for measuring and reporting activity data. In this perspective, we advocate that standardizing these practices can aid in advancing research efforts toward the development of efficient and selective CO 2 reduction electrocatalysts. Using information taken from experimental studies, we identify variables that influence the measured performance of CO 2 reduction electrocatalysts and propose procedures to improve the accuracy and reproducibility of reported data. We recommend that catalysts be measured under conditions which do not introduce artifacts from impurities, either from the electrolyte or counter electrode, and advocate the acquisition of data measured in the absence of mass transport effects.Furthermore, measured rates of electrochemical reactions should be normalized to both the geometric electrode area as well as the electrochemically active surface area to facilitate the comparison of reported catalysts with those previously known. We demonstrate that when these factors are accounted for, the CO 2 reduction activity of Ag and Cu measured in different laboratories exhibit little difference. Adoption of the recommendations presented in this perspective would greatly facilitate the identification of superior catalysts for CO 2 reduction arising solely from changes in their composition and pretreatment.

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“…18 Rosenthal and co-workers have reported a generalized strategy for the electrodeposition of inexpensive electrocatalytic films from triflate salts of Bi 3+ , Sb 3+ , Sn 2+ , and Pb 2+ in organic media. [19][20][21] When the Bi-based electrodes are used for electrochemical CO 2 reduction in acetonitrile with a low overpotential of 250 mV, the 4 electrocatalysts are highly selective towards CO only when an appropriate ionic liquid is present in the system (1-ethyl-3-methylimidazolium hexafluorophosphate [EMIM]PF 6 , or 1-butyl-3-methylimidazolium hexafluorophosphate [BMIM]PF 6 , with an average 81% CO FE with [25][26][27][28][29][30] mA cm −2 ). [19][20][21] These seminal studies have thus clearly indicated that non-noble catalysts have the capability to compete with noble metals for CO 2 reduction.…”

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confidence: 99%

“…25 In contrast, oxidized Sn dendrites exhibited ~30 to 50% FE towards formate at −0.66 V vs. RHE, together with 20% FE to CO. 28 Electrodeposited SnO x thin films on an Sn sheet substrate produced formate with a 40% FE yet with an increased selectivity towards CO (60% FE at −0.7 5 V vs. RHE). 29 This increased selectivity, compared with pristine Sn, was ascribed to the surface oxide species, which may stabilize the CO 2 − intermediate. 28,29 Consistently, H 2 was favored when more positive potentials than −0.7 V vs. RHE were applied to the Sn surface but with lower current densities due to the high overpotential to catalyze the hydrogen evolution reaction on metallic Sn.…”

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confidence: 99%

Cu–Sn Bimetallic Catalyst for Selective Aqueous Electroreduction of CO₂ to CO

et al. 2016

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ABSTRACT. We report a selective and stable electrocatalyst utilizing non-noble metals consisting of Cu and Sn for the efficient and selective reduction of CO 2 to CO over a wide potential range. The bimetallic electrode was prepared through the electrodeposition of Sn species on the surface of oxide-derived copper (OD-Cu). The Cu surface, when decorated with an optimal amount of Sn, resulted in a Faradaic efficiency (FE) for CO greater than 90% and a current density of −1.0 mA cm −2 at −0.6 V vs. RHE, compared to the CO FE of 63% and −2.1 mA cm −2 for OD-Cu. Excess Sn on the surface caused H 2 evolution with a decreased current density. X-ray diffraction (XRD) suggests the formation of Cu-Sn alloy. Auger electron spectroscopy of the sample surface exhibits zero-valent Cu and Sn after the electrodeposition step. Density functional theory (DFT) calculations show that replacing a single Cu atom with a Sn atom leaves the d-band orbitals mostly unperturbed, signifying no dramatic shifts in the bulk electronic structure. However, the Sn atom discomposes the multi-fold sites on pure Cu, Page 1 of 37 1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 19 20 21 22 23 24 25 26 27 28 29 30 31 32 33 34 35 36 37 38 39 40 41 42 43 44 45 46 47 48 49 50 51 52 53 54 55 56 57 58 59 60 2 disfavoring the adsorption of H and leaving the adsorption of CO relatively unperturbed. Our catalytic results along with DFT calculations indicate that the presence of Sn on reduced OD-Cu diminishes the hydrogenation capability-i.e., the selectivity towards H 2 and HCOOH-while hardly affecting the CO productivity. While the pristine monometallic surfaces (both Cu and Sn) fail to selectively reduce CO 2 , the Cu-Sn bimetallic electrocatalyst generates a surface that inhibits adsorbed H*, resulting in improved CO FE. This study presents a strategy to provide a low-cost non-noble metals that can be utilized as a highly selective electrocatalyst for the efficient aqueous reduction of CO 2 . ACS Paragon Plus Environment ACS Catalysis

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Tin Oxide Dependence of the CO₂ Reduction Efficiency on Tin Electrodes and Enhanced Activity for Tin/Tin Oxide Thin-Film Catalysts

Cited by 908 publications

References 29 publications

A selective and efficient electrocatalyst for carbon dioxide reduction

A selective and efficient electrocatalyst for carbon dioxide reduction

Standards and Protocols for Data Acquisition and Reporting for Studies of the Electrochemical Reduction of Carbon Dioxide

Cu–Sn Bimetallic Catalyst for Selective Aqueous Electroreduction of CO₂ to CO

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Tin Oxide Dependence of the CO2 Reduction Efficiency on Tin Electrodes and Enhanced Activity for Tin/Tin Oxide Thin-Film Catalysts

Cited by 908 publications

References 29 publications

A selective and efficient electrocatalyst for carbon dioxide reduction

A selective and efficient electrocatalyst for carbon dioxide reduction

Standards and Protocols for Data Acquisition and Reporting for Studies of the Electrochemical Reduction of Carbon Dioxide

Cu–Sn Bimetallic Catalyst for Selective Aqueous Electroreduction of CO2 to CO

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Tin Oxide Dependence of the CO₂ Reduction Efficiency on Tin Electrodes and Enhanced Activity for Tin/Tin Oxide Thin-Film Catalysts

Cu–Sn Bimetallic Catalyst for Selective Aqueous Electroreduction of CO₂ to CO