Browse
Submit Data
Databases
API
Help

Dataset Information

41 Views

0 Connections

0 Citations

0 Reanalyses

0 Downloads

Omics score: 0

Selective electrochemical reduction of carbon dioxide to ethanol via a relay catalytic platform.

ABSTRACT: Efficient electroreduction of carbon dioxide (CO₂) to ethanol is of great importance, but remains a challenge because it involves the transfer of multiple proton-electron pairs and carbon-carbon coupling. Herein, we report a CoO-anchored N-doped carbon material composed of mesoporous carbon (MC) and carbon nanotubes (CNT) as a catalyst for CO₂ electroreduction. The faradaic efficiencies of ethanol and current density reached 60.1% and 5.1 mA cm^-2, respectively. Moreover, the selectivity for ethanol products was extremely high among the products produced from CO₂. A proposed mechanism is discussed in which the MC-CNT/Co catalyst provides a relay catalytic platform, where CoO catalyzes the formation of CO* intermediates which spill over to MC-CNT for carbon-carbon coupling to form ethanol. The high selectivity for ethanol is attributed mainly to the highly selective carbon-carbon coupling active sites on MC-CNT.

SUBMITTER: Du J

PROVIDER: S-EPMC8159220 | biostudies-literature | 2020 Apr

REPOSITORIES: biostudies-literature

ACCESS DATA

Json Xml

Publications

Selective electrochemical reduction of carbon dioxide to ethanol via a relay catalytic platform.

Du Juan J Li Shaopeng S Liu Shulin S Xin Yu Y Chen Bingfeng B Liu Huizhen H Han Buxing B

Chemical science 20200424 19

Efficient electroreduction of carbon dioxide (CO2) to ethanol is of great importance, but remains a challenge because it involves the transfer of multiple proton-electron pairs and carbon-carbon coupling. Herein, we report a CoO-anchored N-doped carbon material composed of mesoporous carbon (MC) and carbon nanotubes (CNT) as a catalyst for CO2 electroreduction. The faradaic efficiencies of ethanol and current density reached 60.1% and 5.1 mA cm-2, respectively. M ...[more]

PMID: 34122967

Similar Datasets

Ultrastable atomic copper nanosheets for selective electrochemical reduction of carbon dioxide.

Project description:The electrochemical conversion of CO2 and H2O into syngas using renewably generated electricity is an attractive approach to simultaneously achieve chemical fixation of CO2 and storage of renewable energy. Developing cost-effective catalysts for selective electroreduction of CO2 into CO is essential to the practical applications of the approach. We report a simple synthetic strategy for the preparation of ultrathin Cu/Ni(OH)2 nanosheets as an excellent cost-effective catalyst for the electrochemical conversion of CO2 and H2O into tunable syngas under low overpotentials. These hybrid nanosheets with Cu(0)-enriched surface behave like noble metal nanocatalysts in both air stability and catalysis. Uniquely, Cu(0) within the nanosheets is stable against air oxidation for months because of the presence of formate on their surface. With the presence of atomically thick ultrastable Cu nanosheets, the hybrid Cu/Ni(OH)2 nanosheets display both excellent activity and selectivity in the electroreduction of CO2 to CO. At a low overpotential of 0.39 V, the nanosheets provide a current density of 4.3 mA/cm2 with a CO faradaic efficiency of 92%. No decay in the current is observed for more than 22 hours. The catalysts developed in this work are promising for building low-cost CO2 electrolyzers to produce CO.

| S-EPMC5587021 | biostudies-literature

Active sites of copper-complex catalytic materials for electrochemical carbon dioxide reduction.

Project description:Restructuring-induced catalytic activity is an intriguing phenomenon of fundamental importance to rational design of high-performance catalyst materials. We study three copper-complex materials for electrocatalytic carbon dioxide reduction. Among them, the copper(II) phthalocyanine exhibits by far the highest activity for yielding methane with a Faradaic efficiency of 66% and a partial current density of 13 mA cm-2 at the potential of - 1.06 V versus the reversible hydrogen electrode. Utilizing in-situ and operando X-ray absorption spectroscopy, we find that under the working conditions copper(II) phthalocyanine undergoes reversible structural and oxidation state changes to form ~ 2 nm metallic copper clusters, which catalyzes the carbon dioxide-to-methane conversion. Density functional calculations rationalize the restructuring behavior and attribute the reversibility to the strong divalent metal ion-ligand coordination in the copper(II) phthalocyanine molecular structure and the small size of the generated copper clusters under the reaction conditions.

| S-EPMC5788987 | biostudies-literature

Kinetic Understanding of Catalytic Selectivity and Product Distribution of Electrochemical Carbon Dioxide Reduction Reaction.

Project description:CO2 can be electrochemically reduced to different products depending on the nature of catalysts. In this work, we report comprehensive kinetic studies on catalytic selectivity and product distribution of the CO2 reduction reaction on various metal surfaces. The influences on reaction kinetics can be clearly analyzed from the variation of reaction driving force (binding energy difference) and reaction resistance (reorganization energy). Moreover, the CO2RR product distributions are further affected by external factors such as electrode potential and solution pH. A potential-mediated mechanism is found to determine the competing two-electron reduction products of CO2 that shifts from thermodynamics-controlled product formic acid at less negative electrode potentials to kinetic-controlled product CO at more negative electrode potentials. Based on detailed kinetic simulations, a three-parameter descriptor is applied to identify the catalytic selectivity of CO, formate, hydrocarbons/alcohols, as well as side product H2. The present kinetic study not only well explains the catalytic selectivity and product distribution of experimental results but also provides a fast way for catalyst screening.

| S-EPMC10052237 | biostudies-literature

Understanding trends in electrochemical carbon dioxide reduction rates.

Project description:Electrochemical carbon dioxide reduction to fuels presents one of the great challenges in chemistry. Herein we present an understanding of trends in electrocatalytic activity for carbon dioxide reduction over different metal catalysts that rationalize a number of experimental observations including the selectivity with respect to the competing hydrogen evolution reaction. We also identify two design criteria for more active catalysts. The understanding is based on density functional theory calculations of activation energies for electrochemical carbon monoxide reduction as a basis for an electrochemical kinetic model of the process. We develop scaling relations relating transition state energies to the carbon monoxide adsorption energy and determine the optimal value of this descriptor to be very close to that of copper.

| S-EPMC5458145 | biostudies-literature

Effects of Annealing Conditions on the Catalytic Performance of Anodized Tin Oxide for Electrochemical Carbon Dioxide Reduction.

Project description:The electrochemical reduction of CO2 (CO2RR) to value-added products has garnered significant interest as a sustainable solution to mitigate CO2 emissions and harness renewable energy sources. Among CO2RR products, formic acid/formate (HCOOH/HCOO-) is particularly attractive due to its industrial relevance, high energy density, and potential candidate as a liquid hydrogen carrier. This study investigates the influence of the initial oxidation state of tin on CO2RR performance using nanostructured SnOx catalysts. A simple, quick, scalable, and cost-effective synthesis strategy was employed to fabricate SnOx catalysts with controlled oxidation states while maintaining consistent morphology and particle size. The catalysts were characterized using SEM, TEM, XRD, Raman, and XPS to correlate structure and surface properties with catalytic performance. Electrochemical measurements revealed that SnOx catalysts annealed in air at 525 °C exhibited the highest formate selectivity and current density, attributed to the optimized oxidation state and the presence of oxygen vacancies. Flow cell tests further demonstrated enhanced performance under practical conditions, achieving stable formate production with high faradaic efficiency over prolonged operation. These findings highlight the critical role of tin oxidation states and surface defects in tuning CO2RR performance, offering valuable insights for the design of efficient catalysts for CO2 electroreduction to formate.

| S-EPMC11767452 | biostudies-literature

Boosting Electrochemical Carbon Dioxide Reduction on Atomically Dispersed Nickel Catalyst.

Project description:Single-atom catalysts (SACs) with metal-nitrogen (M-N) sites are one of the most promising electrocatalysts for electrochemical carbon dioxide reduction (ECO2R). However, challenges in simultaneously enhancing the activity and selectivity greatly limit the efficiency of ECO2R due to the improper interaction of reactants/intermediates on these catalytic sites. Herein, we report a carbon-based nickel (Ni) cluster catalyst containing both single-atom and cluster sites (NiNx-T, T = 500-800) through a ligand-mediated method and realize a highly active and selective electrocatalytic CO2R process. The catalytic performance can be regulated by the dispersion of Ni-N species via controlling the pyrolysis condition. Benefitting from the synergistic effect of pyrrolic-nitrogen coordinated Ni single-atom and cluster sites, NiNx-600 exhibits a satisfying catalytic performance, including a high partial current density of 61.85 mA cm-2 and a high turnover frequency (TOF) of 7,291 h-1 at -1.2 V vs. RHE, and almost 100% selectivity toward carbon monoxide (CO) production, as well as good stability under 10 h of continuous electrolysis. This work discloses the significant role of regulating the coordination environment of the transition metal sites and the synergistic effect between the isolated single-site and cluster site in enhancing the ECO2R performance.

| S-EPMC8811444 | biostudies-literature

The impact of nitrogen oxides on electrochemical carbon dioxide reduction.

Project description:The electroreduction of carbon dioxide offers a promising avenue to produce valuable fuels and chemicals using greenhouse gas carbon dioxide as the carbon feedstock. Because industrial carbon dioxide point sources often contain numerous contaminants, such as nitrogen oxides, understanding the potential impact of contaminants on carbon dioxide electrolysis is crucial for practical applications. Herein, we investigate the impact of various nitrogen oxides, including nitric oxide, nitrogen dioxide, and nitrous oxide, on carbon dioxide electroreduction on three model electrocatalysts (i.e., copper, silver, and tin). We demonstrate that the presence of nitrogen oxides (up to 0.83%) in the carbon dioxide feed leads to a considerable Faradaic efficiency loss in carbon dioxide electroreduction, which is caused by the preferential electroreduction of nitrogen oxides over carbon dioxide. The primary products of nitrogen oxides electroreduction include nitrous oxide, nitrogen, hydroxylamine, and ammonia. Despite the loss in Faradaic efficiency, the electrocatalysts exhibit similar carbon dioxide reduction performances once a pure carbon dioxide feed is restored, indicating a negligible long-term impact of nitrogen oxides on the catalytic properties of the model catalysts.

| S-EPMC7672067 | biostudies-literature

Spatiotemporal Mapping of Local Heterogeneities during Electrochemical Carbon Dioxide Reduction.

Project description:The activity and selectivity of a copper electrocatalyst during the electrochemical CO2 reduction reaction (eCO2RR) are largely dominated by the interplay between local reaction environment, the catalyst surface, and the adsorbed intermediates. In situ characterization studies have revealed many aspects of this intimate relationship between surface reactivity and adsorbed species, but these investigations are often limited by the spatial and temporal resolution of the analytical technique of choice. Here, Raman spectroscopy with both space and time resolution was used to reveal the distribution of adsorbed species and potential reaction intermediates on a copper electrode during eCO2RR. Principal component analysis (PCA) of the in situ Raman spectra revealed that a working electrocatalyst exhibits spatial heterogeneities in adsorbed species, and that the electrode surface can be divided into CO-dominant (mainly located at dendrite structures) and C-C dominant regions (mainly located at the roughened electrode surface). Our spectral evaluation further showed that in the CO-dominant regions, linear CO was observed (as characterized by a band at ∼2090 cm-1), accompanied by the more classical Cu-CO bending and stretching vibrations located at ∼280 and ∼360 cm-1, respectively. In contrast, in the C-C directing region, these three Raman bands are suppressed, while at the same time a band at ∼495 cm-1 and a broad Cu-CO band at ∼2050 cm-1 dominate the Raman spectra. Furthermore, PCA revealed that anodization creates more C-C dominant regions, and labeling experiments confirmed that the 495 cm-1 band originates from the presence of a Cu-C intermediate. These results indicate that a copper electrode at work is very dynamic, thereby clearly displaying spatiotemporal heterogeneities, and that in situ micro-spectroscopic techniques are crucial for understanding the eCO2RR mechanism of working electrocatalyst materials.

| S-EPMC10369669 | biostudies-literature

Double layer charging driven carbon dioxide adsorption limits the rate of electrochemical carbon dioxide reduction on Gold.

Project description:Electrochemical CO[Formula: see text] reduction is a potential route to the sustainable production of valuable fuels and chemicals. Here, we perform CO[Formula: see text] reduction experiments on Gold at neutral to acidic pH values to elucidate the long-standing controversy surrounding the rate-limiting step. We find the CO production rate to be invariant with pH on a Standard Hydrogen Electrode scale and conclude that it is limited by the CO[Formula: see text] adsorption step. We present a new multi-scale modeling scheme that integrates ab initio reaction kinetics with mass transport simulations, explicitly considering the charged electric double layer. The model reproduces the experimental CO polarization curve and reveals the rate-limiting step to be *COOH to *CO at low overpotentials, CO[Formula: see text] adsorption at intermediate ones, and CO[Formula: see text] mass transport at high overpotentials. Finally, we show the Tafel slope to arise from the electrostatic interaction between the dipole of *CO[Formula: see text] and the interfacial field. This work highlights the importance of surface charging for electrochemical kinetics and mass transport.

| S-EPMC6946669 | biostudies-literature

Copper⁻Silver Bimetallic Nanowire Arrays for Electrochemical Reduction of Carbon Dioxide.

Project description:The electrochemical conversion of carbon dioxide (CO₂) into gaseous or liquid fuels has the potential to store renewable energies and reduce carbon emissions. Here, we report a three-step synthesis using Cu⁻Ag bimetallic nanowire arrays as catalysts for electrochemical reduction of CO₂. CuO/Cu₂O nanowires were first grown by thermal oxidation of copper mesh in ambient air and then reduced by annealing in the presence of hydrogen to form Cu nanowires. Cu⁻Ag bimetallic nanowires were then produced via galvanic replacement between Cu nanowires and the Ag⁺ precursor. The Cu⁻Ag nanowires showed enhanced catalytic performance over Cu nanowires for electrochemical reduction of CO₂, which could be ascribed to the incorporation of Ag into Cu nanowires leading to suppression of hydrogen evolution. Our work provides a method for tuning the selectivity of copper nanocatalysts for CO₂ reduction by controlling their composition.

| S-EPMC6410069 | biostudies-literature