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Journal ArticleDOI: 10.1021/ACSCATAL.0C04887

Acceleration of Electrochemical CO2 Reduction to Formate at the Sn/Reduced Graphene Oxide Interface

02 Mar 2021-ACS Catalysis (American Chemical Society (ACS))-Vol. 11, Iss: 6, pp 3310-3318
Abstract: Electrochemical CO2 reduction is a key technology to recycle CO2 as a renewable resource, but adsorbing CO2 on the catalyst surface is challenging. We explored the effects of reduced graphene oxide...

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Topics: Graphene (56%), Oxide (54%), Formate (50%)
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14 results found


Journal ArticleDOI: 10.1016/J.CEJ.2021.130003
Baohua Zhang1, Song Chen1, Bari Wulan1, Jintao Zhang1Institutions (1)
Abstract: For CO2 electrocatalytic reduction, it is highly challenging to activate CO2 at a low overpotential. Herein, we demonstrated to modify the surface properties of tin dioxide nanosheets loaded on carbon fibers via the partial coating of nitrogen-doped carbon (NC). The NC layers with Lewis base sites on SnO2 nanosheets would facilitate the surface adsorption and subsequent conversion of CO2 into formate. Therefore, the optimal electrocatalyst exhibits very high Faradic efficiency (>80%) in a broad potential range of −0.6 – −1.0 V (vs. RHE) with the maximum value up to 93% and good long-term stability for 24 h. Both experimental results and theoretical calculations firstly revealed that the improved performance would be attributed to the improved local CO2 concentration due to the surface modification of SnO2 nanosheets with NC. Therefore, the surface regulation of SnO2 plays a significant role in promoting the catalytic performance in CO2 electroreduction reaction.

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Topics: Electrocatalyst (55%), Surface modification (55%), Overpotential (53%)

3 Citations


Open accessDOI: 10.1016/J.APMATE.2021.10.003
Yufei Jia1, Fei Li1, Ke Fan1, Licheng Sun2  +2 moreInstitutions (3)
15 Nov 2021-
Abstract: The extensive consumption of fossil fuels has caused the rapid increase in the CO2 level in the atmosphere, forcing people to find a clean and efficient technology of CO2 conversion to alleviate CO2 emissions and develop value-added products. Among various CO2 conversion systems, electroreduction of CO2 to value-added chemicals is a feasible way for practical applications. Copper, the only metal that can catalyze CO2 reduction to multi-carbon products, has attracted the most attention among various catalysts. However, slow reaction kinetics, low product selectivity, as well as poor stability are the main drawbacks of single metallic Cu-based catalysts. Such issues can be addressed by introducing second metal in Cu-based catalysts. Here, we summarize the recent progress relating to the Cu-based bimetallic electrocatalysts for CO2 reduction, and discuss the composition and structure effects on the activity and selectivity of electrochemical CO2 reduction. Last, we outline the challenges and perspectives on electrocatalysts for this field. We expect that this review can provide new insights into the further development of Cu-based bimetallic electrocatalysts for CO2 reduction.

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3 Citations


Journal ArticleDOI: 10.1016/J.APCATB.2021.120581
Jiayu Li1, Jinxia Li1, Xianglin Liu1, Jiacheng Chen1  +4 moreInstitutions (1)
Abstract: Electrodeposited Bi, Sn and In catalysts are employed as model catalysts to investigate the nature of active sites and the influence of surface hydroxyls on the formation of formate during CO2 electroreduction (CO2RR). With SEM, XPS, in situ XRD, electrochemical measurements and DFT calculations, the active sites are Bi0, SnO and In2O3, with their affinities to hydroxyls following the trend of Bi0

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Topics: Formate (52%)

3 Citations




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67 results found



Open accessJournal ArticleDOI: 10.1038/NGEO689
01 Dec 2009-Nature Geoscience
Abstract: Efforts to control climate change require the stabilization of atmospheric CO2 concentrations. This can only be achieved through a drastic reduction of global CO2 emissions. Yet fossil fuel emissions increased by 29% between 2000 and 2008, in conjunction with increased contributions from emerging economies, from the production and international trade of goods and services, and from the use of coal as a fuel source. In contrast, emissions from land-use changes were nearly constant. Between 1959 and 2008, 43% of each year's CO2 emissions remained in the atmosphere on average; the rest was absorbed by carbon sinks on land and in the oceans. In the past 50 years, the fraction of CO2 emissions that remains in the atmosphere each year has likely increased, from about 40% to 45%, and models suggest that this trend was caused by a decrease in the uptake of CO2 by the carbon sinks in response to climate change and variability. Changes in the CO2 sinks are highly uncertain, but they could have a significant influence on future atmospheric CO2 levels. It is therefore crucial to reduce the uncertainties.

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Topics: Carbon sink (55%), Climate change (51%)

1,775 Citations


Journal ArticleDOI: 10.1039/C2EE21234J
Abstract: We report new insights into the electrochemical reduction of CO2 on a metallic copper surface, enabled by the development of an experimental methodology with unprecedented sensitivity for the identification and quantification of CO2 electroreduction products. This involves a custom electrochemical cell designed to maximize product concentrations coupled to gas chromatography and nuclear magnetic resonance for the identification and quantification of gas and liquid products, respectively. We studied copper across a range of potentials and observed a total of 16 different CO2 reduction products, five of which are reported here for the first time, thus providing the most complete view of the reaction chemistry reported to date. Taking into account the chemical identities of the wide range of C1–C3 products generated and the potential-dependence of their turnover frequencies, mechanistic information is deduced. We discuss a scheme for the formation of multicarbon products involving enol-like surface intermediates as a possible pathway, accounting for the observed selectivity for eleven distinct C2+ oxygenated products including aldehydes, ketones, alcohols, and carboxylic acids.

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1,647 Citations


Journal ArticleDOI: 10.1002/ADFM.200900166
Cecilia Mattevi1, Goki Eda1, Stefano Agnoli2, Steve Miller1  +6 moreInstitutions (3)
Abstract: A detailed description of the electronic properties, chemical state, and structure of uniform single and few-layered graphene oxide (GO) thin films at different stages of reduction is reported. The residual oxygen content and structure of GO are monitored and these chemical and structural characteristics are correlated to electronic properties of the thin films at various stages of reduction. It is found that the electrical characteristics of reduced GO do not approach those of intrinsic graphene obtained by mechanical cleaving because the material remains significantly oxidized. The residual oxygen forms sp3 bonds with carbon atoms in the basal plane such that the carbon sp2 bonding fraction in fully reduced GO is ∼0.80. The minority sp3 bonds disrupt the transport of carriers delocalized in the sp2 network, limiting the mobility, and conductivity of reduced GO thin films. Extrapolation of electrical conductivity data as a function of oxygen content reveals that complete removal of oxygen should lead to properties that are comparable to graphene.

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Topics: Graphene oxide paper (60%), Graphene (58%), Oxide (53%) ... show more

1,521 Citations


Journal ArticleDOI: 10.1021/JA3010978
Christina W. Li1, Matthew W. Kanan1Institutions (1)
Abstract: Modified Cu electrodes were prepared by annealing Cu foil in air and electrochemically reducing the resulting Cu2O layers. The CO2 reduction activities of these electrodes exhibited a strong dependence on the initial thickness of the Cu2O layer. Thin Cu2O layers formed by annealing at 130 °C resulted in electrodes whose activities were indistinguishable from those of polycrystalline Cu. In contrast, Cu2O layers formed at 500 °C that were ≥ ∼3 μm thick resulted in electrodes that exhibited large roughness factors and required 0.5 V less overpotential than polycrystalline Cu to reduce CO2 at a higher rate than H2O. The combination of these features resulted in CO2 reduction geometric current densities >1 mA/cm2 at overpotentials <0.4 V, a higher level of activity than all previously reported metal electrodes evaluated under comparable conditions. Moreover, the activity of the modified electrodes was stable over the course of several hours, whereas a polycrystalline Cu electrode exhibited deactivation within...

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Topics: Overpotential (55%), Electrode (50%)

1,363 Citations


Performance
Metrics
No. of citations received by the Paper in previous years
YearCitations
20222
202112