Facile synthesis of cubic cuprous oxide for electrochemical reduction of carbon dioxide

Zeng, Juqin; Castellino, Micaela; Sacco, Adriano; Martino, Gaia Di; Farkhondehfal, M. Amin; Chiodoni, Angelica; Hernández, Simelys; Pirri, Candido Fabrizio

doi:10.1007/s10853-020-05278-y

Cited by 23 publications

(18 citation statements)

References 50 publications

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“…The reason for the decreased Ag content might be that it is flushed away by electrolytes. XPS results of Cu 2 O-Ag after CO 2 RR in Figure S9 show the characteristic metallic Ag peaks and mixed Cu 0 + Cu + peaks, confirming the existence of Ag and reduction of Cu 2 O to Cu, and the XPS spectrum of Cu 2 O after CO 2 RR also shows the mixed Cu 0 + Cu + peaks ( Figure S10 ) [ 56 , 57 , 58 ].…”

Section: Resultsmentioning

confidence: 88%

Cu2O-Ag Tandem Catalysts for Selective Electrochemical Reduction of CO2 to C2 Products

et al. 2021

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The electrochemical carbon dioxide reduction reaction (CO2RR) to C2 chemicals has received great attention. Here, we report the cuprous oxide (Cu2O) nanocubes cooperated with silver (Ag) nanoparticles via the replacement reaction for a synergetic CO2RR. The Cu2O-Ag tandem catalyst exhibits an impressive Faradaic efficiency (FE) of 72.85% for C2 products with a partial current density of 243.32 mA·cm−2. The electrochemical experiments and density functional theory (DFT) calculations reveal that the introduction of Ag improves the intermediate CO concentration on the catalyst surface and meanwhile reduces the C-C coupling reaction barrier energy, which is favorable for the synthesis of C2 products.

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Section: Resultsmentioning

confidence: 88%

Cu2O-Ag Tandem Catalysts for Selective Electrochemical Reduction of CO2 to C2 Products

et al. 2021

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“…It is worth to notice that the diffusion of charges cannot be appreciated due to low frequency (0.1 Hz) limitations [ 12 ]. The experimental data were fitted employing the equivalent electric circuit shown in the inset of Figure S7a , in order to obtain the parameters related to the different processes, namely the high frequency ( R t and C t ) and low frequency ( R ct and C dl ) ones, including the series resistance R s [ 43 ]. Since all the parameters except from the charge transfer resistance R ct exhibit negligible dependence on the applied potential [ 44 ], the values related to the measurement acquired at −0.59 V are reported as examples in Table S5 .…”

Section: Resultsmentioning

confidence: 99%

Zn- and Ti-Doped SnO2 for Enhanced Electroreduction of Carbon Dioxide

et al. 2021

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The electrocatalytic reduction of CO2 into useful fuels, exploiting rationally designed, inexpensive, active, and selective catalysts, produced through easy, quick, and scalable routes, represents a promising approach to face today’s climate challenges and energy crisis. This work presents a facile strategy for the preparation of doped SnO2 as an efficient electrocatalyst for the CO2 reduction reaction to formic acid and carbon monoxide. Zn or Ti doping was introduced into a mesoporous SnO2 matrix via wet impregnation and atomic layer deposition. It was found that doping of SnO2 generates an increased amount of oxygen vacancies, which are believed to contribute to the CO2 conversion efficiency, and among others, Zn wet impregnation resulted the most efficient process, as confirmed by X-ray photoelectron spectroscopy analysis. Electrochemical characterization and active surface area evaluation show an increase of availability of surface active sites. In particular, the introduction of Zn elemental doping results in enhanced performance for formic acid formation, in comparison to un-doped SnO2 and other doped SnO2 catalysts. At −0.99 V versus reversible hydrogen electrode, the total faradaic efficiency for CO2 conversion reaches 80%, while the partial current density is 10.3 mA cm−2. These represent a 10% and a threefold increases for faradaic efficiency and current density, respectively, with respect to the reference un-doped sample. The enhancement of these characteristics relates to the improved charge transfer and conductivity with respect to bare SnO2.

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“…% after electrolysis at -0.7 V and -0.9 V. This Sn content is in good agreement with surface composition reported in previous studies on low surface area CO-selective Cu-Sn catalysts 21,22,28 and Sn functionalized Cu foams. 23 Similarly, in the formate-selective catalyst, CuNW-SnHIGH, originally the catalyst surface is composed of SnO2 exclusively (~20 nm), which remains largely unaffected after CP prereduction (98 at. % Sn).…”

Section: Quasi In Situ Xpsmentioning

confidence: 99%

“…Furthermore, improved activity and selectivity are reported in catalysts with high surface area. Highly CO-selective catalysts have been achieved by the functionalization of high surface area Cu nanostructures with low amounts of Sn by electrodeposition, 23,24 electroless deposition 25 or atomic layer deposition (ALD) of SnO2. 16 Interestingly, high surface area Cu nanostructures functionalized with Sn overlayers have also been reported as highly selective catalysts towards formate.…”

Section: Introductionmentioning

confidence: 99%

Tracking Structure and Composition Changes in Oxide Derived Cu-Sn Catalysts During CO2 Electroreduction Using X-Ray Spectroscopy

L¹,

Arndt²,

Stojkovikj³

et al. 2021

Preprint

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<div> In the field of electrochemical CO2 conversion, the development of earth-abundant catalysts which are selective for a single product is a central challenge. Cu-Sn bimetallic catalysts have been reported to yield selective CO2 reduction towards either carbon monoxide or formate. To advance the understanding of possible synergetic effects between Cu and Sn which direct product selectivity, a thorough investigation of the catalyst structure and composition in its active state is desired. We present an X-ray spectroscopy investigation of oxide-derived Cu-Sn catalysts prepared by functionalization of Cu(OH)2 nanowire arrays with ultrathin SnO2 overlayers. This method allows precisely tunable Sn composition, which enables synthesis of composite catalysts with high selectivity toward either CO or formate. Under CO2 reduction conditions, the materials undergo significant transformations before reaching their catalytically active forms. Complementary information on the electrocatalysts’ dynamic bulk and surface structure was revealed via correlating observations from multiple X-ray spectroscopy methods. In situ investigations of Cu K-edge revealed that in the bulk Cu is fully reduced from Cu2+ to Cu° after a pre reduction step. Quasi in situ XPS demonstrated that, at the catalyst surface, Cu is also present exclusively as Cu°, whereas significant differences in Sn quantification and speciation were observed between the CO- and formate-selective catalysts. After CO<a>2</a> electrolysis, CO-selective catalysts exhibited a surface Sn content of 13 at. % predominantly present as Sn oxide, while the formate-selective catalysts had a Sn content of ~70 at. % consisting of both metallic Sn° and Sn oxide species. Our study reveals the complex dependence of catalyst structure, composition, and speciation with applied electrochemical bias in Sn-functionalized nanostructured Cu catalysts.</div>

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Facile synthesis of cubic cuprous oxide for electrochemical reduction of carbon dioxide

Cited by 23 publications

References 50 publications

Cu2O-Ag Tandem Catalysts for Selective Electrochemical Reduction of CO2 to C2 Products

Cu2O-Ag Tandem Catalysts for Selective Electrochemical Reduction of CO2 to C2 Products

Zn- and Ti-Doped SnO2 for Enhanced Electroreduction of Carbon Dioxide

Tracking Structure and Composition Changes in Oxide Derived Cu-Sn Catalysts During CO2 Electroreduction Using X-Ray Spectroscopy

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