A selective and efficient electrocatalyst for carbon dioxide reduction

Lü, Qi; Rosen, Jonathan; Yang, Zhou; Hutchings, Gregory S.; Kimmel, Yannick C.; Chen, Jingguang G.; Jiao, Feng

doi:10.1038/ncomms4242

Cited by 1,222 publications

(1,211 citation statements)

References 38 publications

(55 reference statements)

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“…This improvement was likely correlated with the nanostructured surface populated with highly active sites for stabilizing COOH intermediate as well as a high local pH arising from porosity‐induced transport limitation. A nanoporous silver was synthesized by Jiao and co‐workers from two‐step dealloying of an Ag‐Al precursor 74. Electrochemical measurements demonstrated that it was capable of reducing CO 2 to CO with ≈92% selectivity at a rate >3000 times higher than bulk Ag under moderate overpotentials (<0.5 V).…”

Section: Electrocatalytic Materials For Co2 Reductionmentioning

confidence: 99%

CO₂ Reduction: From the Electrochemical to Photochemical Approach

et al. 2017

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Increasing CO2 concentration in the atmosphere is believed to have a profound impact on the global climate. To reverse the impact would necessitate not only curbing the reliance on fossil fuels but also developing effective strategies capture and utilize CO2 from the atmosphere. Among several available strategies, CO2 reduction via the electrochemical or photochemical approach is particularly attractive since the required energy input can be potentially supplied from renewable sources such as solar energy. In this Review, an overview on these two different but inherently connected approaches is provided and recent progress on the development, engineering, and understanding of CO2 reduction electrocatalysts and photocatalysts is summarized. First, the basic principles that govern electrocatalytic or photocatalytic CO2 reduction and their important performance metrics are discussed. Then, a detailed discussion on different CO2 reduction electrocatalysts and photocatalysts as well as their generally designing strategies is provided. At the end of this Review, perspectives on the opportunities and possible directions for future development of this field are presented.

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Section: Electrocatalytic Materials For Co2 Reductionmentioning

confidence: 99%

CO₂ Reduction: From the Electrochemical to Photochemical Approach

et al. 2017

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“…A single-step electrochemical process that can directly convert CO 2 to methane under conditions of ambient pressure and temperature may represent an attractive alternative. Of the metals explored as catalysts for electrochemical CO 2 reduction,(8) the most active and selective identified to date are gold, silver, and bismuth, (9)(10)(11)(12)(13)(14) which produce CO as their terminal product. Copper is attractive in comparison, as it produces more reduced hydrocarbon products.…”

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confidence: 99%

Enhanced Electrochemical Methanation of Carbon Dioxide with a Dispersible Nanoscale Copper Catalyst

2014

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Although the vast majority of hydrocarbon fuels and products are presently derived from petroleum, there is much interest in the development of routes for synthesizing these same products by hydrogenating CO 2 . The simplest hydrocarbon target is methane, which can utilize existing infrastructure for natural gas storage, distribution, and consumption. Electrochemical methods for methanizing CO 2 currently suffer from a combination of low activities and poor selectivities. We demonstrate that copper nanoparticles supported on glassy carbon (n-Cu/C) achieve up to 4 times greater methanation current densities compared to high-purity copper foil electrodes. The n-Cu/ C electrocatalyst also exhibits an average Faradaic efficiency for methanation of 80% during extended electrolysis, the highest Faradaic efficiency for room-temperature methanation reported to date. We find that the level of copper catalyst loading on the glassy carbon support has an enormous impact on the morphology of the copper under catalytic conditions and the resulting Faradaic efficiency for methane. The improved activity and Faradaic efficiency for methanation involves a mechanism that is distinct from what is generally thought to occur on copper foils. Electrochemical data indicate that the early steps of methanation on n-Cu/C involve a pre-equilibrium one-electron transfer to CO 2 to form an adsorbed radical, followed by a rate-limiting nonelectrochemical step in which the adsorbed CO 2 radical reacts with a second CO 2 molecule from solution. These nanoscale copper electrocatalysts represent a first step toward the preparation of practical methanation catalysts that can be incorporated into membrane-electrode assemblies in electrolyzers.

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“…10 However, their implementation at an industrial scale is unsustainable and has limitations owing to the scarcity of noble metals. [7][8][9][10] Previous studies by Hori and coworkers have demonstrated that Cu is unique compared with other metals in its ability to produce hydrocarbons at potentials more negative than −1 V vs RHE. 11 Nevertheless, the large overpotential renders the process inefficient.…”

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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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A selective and efficient electrocatalyst for carbon dioxide reduction

Cited by 1,222 publications

References 38 publications

CO₂ Reduction: From the Electrochemical to Photochemical Approach

CO₂ Reduction: From the Electrochemical to Photochemical Approach

Enhanced Electrochemical Methanation of Carbon Dioxide with a Dispersible Nanoscale Copper Catalyst

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

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A selective and efficient electrocatalyst for carbon dioxide reduction

Cited by 1,222 publications

References 38 publications

CO2 Reduction: From the Electrochemical to Photochemical Approach

CO2 Reduction: From the Electrochemical to Photochemical Approach

Enhanced Electrochemical Methanation of Carbon Dioxide with a Dispersible Nanoscale Copper Catalyst

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

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Product

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CO₂ Reduction: From the Electrochemical to Photochemical Approach

CO₂ Reduction: From the Electrochemical to Photochemical Approach

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