Morphology-controlled CuO nanoparticles for electroreduction of CO<sub>2</sub> to ethanol

Chi, Dinghui; Yang, Hengpan; Du, Yunchen; Lv, Ting; Sui, Guo-Jiao; Wang, Huan; Lu, Jia‐Xing

doi:10.1039/c4ra05415f

Cited by 74 publications

(72 citation statements)

References 16 publications

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“…Analysis of the electrolyte showed no further liquid products. The HER could not be totally suppressed probably due to the poor solubility of ethyne (19) in water. However, up to 61% of the charge passed went into the reduction of ethyne (19) to ethene (12) as opposed to 2% ethane (18) yield for ethene (12) feed.…”

Section: Reactivity Of Alkynesmentioning

confidence: 99%

“…The HER could not be totally suppressed probably due to the poor solubility of ethyne (19) in water. However, up to 61% of the charge passed went into the reduction of ethyne (19) to ethene (12) as opposed to 2% ethane (18) yield for ethene (12) feed. Palladium, a noble metal well known for its hydrogenation activity, was also recently reported to selectively electro-hydrogenate ethyne (19) to ethene (12) by Song et al [68].…”

Section: Reactivity Of Alkynesmentioning

confidence: 99%

“…As the dimerization of carbynes to alkynes is even known to proceed on single metal centers [67], they could also be proposed as intermediates. As models for triple-bond ethyne (19), propargyl alcohol (33) and 2-butyn-1-ol (34) were used. The latter served as model for an internal triple bond.…”

Section: Reactivity Of Alkynesmentioning

confidence: 99%

“…Copper-catalyzed CO 2 reduction to hydrocarbons was first reported by Hori in 1985 [10]. In the following decades, publications using copper electrodes [11][12][13][14][15][16][17], copper oxide electrodes [18][19][20][21], copper-containing perovskites [22], oxide-supported copper catalysts [23], halide-derived copper catalysts [24][25][26][27], copper-based alloys [28], copper-based metal-organic frameworks [29], molecular copper complexes [30], as well as alternative systems [5,[31][32][33][34][35][36] vastly increased. Also pyridine-based co-catalysis known from Pd electrodes [37] could recently be transferred to copper-based systems [38].…”

Section: Introductionmentioning

confidence: 99%

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Reactivity of Copper Electrodes towards Functional Groups and Small Molecules in the Context of CO2 Electro-Reductions

et al. 2017

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Abstract:The direct electro-reduction of CO 2 to functional molecules like ethene is a highly desirable variant of CO 2 utilization. The formation of, for example, ethene from CO 2 is a multistep electrochemical process going through various intermediates. As these intermediates are organic species, the CO 2 reducing electro-catalyst has to be competent for a variety of organic functional group transformations to yield the final product. In this work, the activity of an in situ-grown nano-structured copper catalyst towards a variety of organic functional group conversions was studied. The model reagents were selected from the product spectrum of actual CO 2 reduction reaction (CO 2 RR) experiments and from proposals in the literature. The CO 2 bulk electrolysis benchmark was conducted at 170 mAcm −2 current density with up to 43% Faradaic Efficiency (FE) for ethene and 23% FE for ethanol simultaneously. To assure relevance for application-oriented conditions, the reactivity screening was conducted at elevated current densities and, thus, overpotentials. The found reactivity pattern was then also transferred to the CO reduction reaction (CORR) under benchmark conditions yielding additional insights. The results suggest that at high current density/high overpotential conditions, also other ethene formation pathways apart from acetaldehyde reduction such as CH 2 dimerization are present. A new suggestion for a high current density mechanism will be presented, which is in agreement with the experimental observations and the found activity pattern of copper cathodes toward organic functional group conversion.

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Section: Reactivity Of Alkynesmentioning

confidence: 99%

Section: Reactivity Of Alkynesmentioning

confidence: 99%

Section: Reactivity Of Alkynesmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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Reactivity of Copper Electrodes towards Functional Groups and Small Molecules in the Context of CO2 Electro-Reductions

et al. 2017

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“…6,7 However, the explanation becomes more complicated when dealing with nanostructured copper materials derived from oxidized precursors, which show both higher activity and greatly enhanced selectivity towards multicarbon products. [8][9][10][11][12][13][14][15][16] It has been hypothesized that this could be related for instance to an increase of local pH, [17][18][19] grain boundaries, 20 undercoordinated sites, 21 or residual oxides. [22][23][24] Several groups have shown the existence of sites with higher CO binding energy in oxidederived copper.…”

mentioning

confidence: 99%

Subsurface Oxygen in Oxide-Derived Copper Electrocatalysts for Carbon Dioxide Reduction

Eilert

Cavalca

Roberts

et al. 2016

J. Phys. Chem. Lett.

388

396

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Copper electrocatalysts derived from an oxide have shown extraordinary electrochemical properties for the carbon dioxide reduction reaction (CO 2 RR). Using in situ Ambient Pressure Xray Photoelectron Spectroscopy (APXPS) and quasi in situ Electron Energy Loss Spectroscopy (EELS) in a Transmission Electron Microscope (TEM), we show that there is a substantial amount of residual oxygen in nanostructured, oxide-derived copper electrocatalysts, but no residual copper oxide. Based on these findings in combination with Density Functional Theory (DFT) simulations, we propose that residual subsurface oxygen changes the electronic structure of the catalyst and creates sites with higher carbon monoxide binding energy. If such sites are stable under the strongly reducing conditions found in CO 2 RR, these findings would explain the high efficiencies of oxide-derived copper in reducing carbon dioxide to multi-carbon compounds such as ethylene.

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Recent Progresses in Electrochemical Carbon Dioxide Reduction on Copper‐Based Catalysts toward Multicarbon Products

Wang

et al. 2021

Adv Funct Materials

159

116

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Electrochemical carbon dioxide reduction reaction (CO2RR) offers a promising way of effectively converting CO2 to value‐added chemicals and fuels by utilizing renewable electricity. To date, the electrochemical reduction of CO2 to single‐carbon products, especially carbon monoxide and formate, has been well achieved. However, the efficient conversion of CO2 to more valuable multicarbon products (e.g., ethylene, ethanol, n‐propanol, and n‐butanol) is difficult and still under intense investigation. Here, recent progresses in the electrochemical CO2 reduction to multicarbon products using copper‐based catalysts are reviewed. First, the mechanism of CO2RR is briefly described. Then, representative approaches of catalyst engineering are introduced toward the formation of multicarbon products in CO2RR, such as composition, morphology, crystal phase, facet, defect, strain, and surface and interface. Subsequently, key aspects of cell engineering for CO2RR, including electrode, electrolyte, and cell design, are also discussed. Finally, recent advances are summarized and some personal perspectives in this research direction are provided.

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Morphology-controlled CuO nanoparticles for electroreduction of CO₂ to ethanol

Abstract: Morphology-controlled CuO nanoparticles for electroreduction of CO2 with an excellent selectivity for ethanol.

Cited by 74 publications

References 16 publications

Reactivity of Copper Electrodes towards Functional Groups and Small Molecules in the Context of CO2 Electro-Reductions

Reactivity of Copper Electrodes towards Functional Groups and Small Molecules in the Context of CO2 Electro-Reductions

Subsurface Oxygen in Oxide-Derived Copper Electrocatalysts for Carbon Dioxide Reduction

Recent Progresses in Electrochemical Carbon Dioxide Reduction on Copper‐Based Catalysts toward Multicarbon Products

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Morphology-controlled CuO nanoparticles for electroreduction of CO2 to ethanol

Abstract: Morphology-controlled CuO nanoparticles for electroreduction of CO2 with an excellent selectivity for ethanol.

Cited by 74 publications

References 16 publications

Reactivity of Copper Electrodes towards Functional Groups and Small Molecules in the Context of CO2 Electro-Reductions

Reactivity of Copper Electrodes towards Functional Groups and Small Molecules in the Context of CO2 Electro-Reductions

Subsurface Oxygen in Oxide-Derived Copper Electrocatalysts for Carbon Dioxide Reduction

Recent Progresses in Electrochemical Carbon Dioxide Reduction on Copper‐Based Catalysts toward Multicarbon Products

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Morphology-controlled CuO nanoparticles for electroreduction of CO₂ to ethanol