CO₂ reduction on gas-diffusion electrodes and why catalytic performance must be assessed at commercially-relevant conditions

Energy & Environmental Science, Journal Year: 2019, Volume and Issue: 12(5), P. 1442 - 1453

Published: Jan. 1, 2019

The substantial implications of high current densities on the local reaction environment and design catalysts for electrochemical CO₂ reduction are addressed. presented perspectives also reflect practices within field offer new opportunities both future catalyst system-focused research efforts.

Language: Английский

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Coordinatively unsaturated nickel–nitrogen sites towards selective and high-rate CO₂electroreduction

Energy & Environmental Science, Journal Year: 2018, Volume and Issue: 11(5), P. 1204 - 1210

Published: Jan. 1, 2018

Coordinatively unsaturated Ni–N active sites facilitate CO₂electroreduction and inhibit the competitive hydrogen evolution reaction, demonstrating selective high-rate CO₂electroreduction.

Language: Английский

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Co-electrolysis of CO2 and glycerol as a pathway to carbon chemicals with improved technoeconomics due to low electricity consumption

Nature Energy, Journal Year: 2019, Volume and Issue: 4(6), P. 466 - 474

Published: April 22, 2019

Language: Английский

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Progress toward Commercial Application of Electrochemical Carbon Dioxide Reduction

Chem, Journal Year: 2018, Volume and Issue: 4(11), P. 2571 - 2586

Published: Sept. 13, 2018

Language: Английский

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Controlling the Oxidation State of the Cu Electrode and Reaction Intermediates for Electrochemical CO₂ Reduction to Ethylene

Journal of the American Chemical Society, Journal Year: 2020, Volume and Issue: 142(6), P. 2857 - 2867

Published: Jan. 20, 2020

Understanding the role of oxidation state Cu surface and surface-adsorbed intermediate species in electrochemical CO2 reduction is crucial for development selective CO2-to-fuel electrocatalysts. In this study, mechanism over catalysts with various states was studied by using situ surface-enhanced infrared absorption spectroscopy (SEIRAS), soft X-ray (Cu L-edge), online gas chromatography measurements. The atop-adsorbed CO (COatop) obtained on electrodeposited which primarily has Cu(I). COatop further reduced, followed formation C1 product such as CH4. residual bridge-adsorbed (CObridge) formed as-prepared Cu(0) inhibits hydrocarbon formation. contrast, CV-treated electrode prepared oxidizing contains different amounts Cu(I) states. major theme work that SEIRAS results show coexistence CObridge reaction intermediates during selectivity CO2-to-ethylene conversion enhanced electrode. modulated method exhibit well electrocatalytic properties.

Language: Английский

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Intrinsic Carbon‐Defect‐Driven Electrocatalytic Reduction of Carbon Dioxide

Advanced Materials, Journal Year: 2019, Volume and Issue: 31(19)

Published: March 28, 2019

Heteroatom-doped carbon catalysts are currently attracting enormous attention due to their excellent performance for the electrocatalytic dioxide reduction reaction (ECRR). However, origin of high catalytic activities doped-carbon materials remains obscure with role intrinsic defects in promoting ECRR receiving little despite abundance all carbon-based materials. Herein, a positive correlation is reported between and content contained within these catalysts. Further, it demonstrated that defective porous containing no active heteroatom dopants also show ECRR. C K-edge near edge X-ray absorption fine structure measurements density functional theory calculations reveal sp2 (octagonal pentagonal) rather than key activity This work thus makes an important contribution understanding catalysts, doping perhaps being less previously envisaged achieving performance.

Language: Английский

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High-Entropy Alloys as Catalysts for the CO₂ and CO Reduction Reactions

ACS Catalysis, Journal Year: 2020, Volume and Issue: 10(3), P. 2169 - 2176

Published: Jan. 13, 2020

We present an approach for a probabilistic and unbiased discovery of selective active catalysts the carbon dioxide (CO2) monoxide (CO) reduction reactions on high-entropy alloys (HEAs). By combining density functional theory (DFT) with supervised machine learning, we predict CO hydrogen (H) adsorption energies all surface sites (111) surfaces disordered CoCuGaNiZn AgAuCuPdPt HEAs. This allows optimization HEA compositions increased likelihood weak to suppress formation molecular strong favor CO. As opposed construction specific arrangements atoms, our makes desired more frequent through increase in their probability. leads several catalyst candidates which selectivity toward highly reduced compounds is expected some have been verified literature.

Language: Английский

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Potential Link between Cu Surface and Selective CO₂ Electroreduction: Perspective on Future Electrocatalyst Designs

Advanced Materials, Journal Year: 2020, Volume and Issue: 32(17)

Published: March 5, 2020

Abstract Electrochemical reduction of carbon dioxide (CO 2 RR) product distribution has been identified to be dependent on various surface factors, including the Cu facet, morphology, chemical states, doping, etc., which can alter binding strength key intermediates such as *CO and *OCCO during reduction. Therefore, in‐depth knowledge catalyst identification active species under reaction conditions aid in designing efficient Cu‐based electrocatalysts. This progress report categorizes electrocatalysts into four main groups, namely metallic Cu, alloys, compounds (Cu + non‐metal), supported catalysts by carbon, metal oxides, or polymers). The detailed mechanisms for selective CO RR are presented, followed recent relevant developments synthetic procedures preparing nanoparticles. Herein, potential link between performance is highlighted, especially terms but other significant factors defective sites roughened morphology equally considered discussion current studies with fully understand origin enhancement toward C formation. concludes providing suggestions future designs highly stable RR.

Language: Английский

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Covalently Grafting Cobalt Porphyrin onto Carbon Nanotubes for Efficient CO₂ Electroreduction

Angewandte Chemie International Edition, Journal Year: 2019, Volume and Issue: 58(20), P. 6595 - 6599

Published: Jan. 28, 2019

Molecular complexes with inexpensive transition-metal centers have drawn extensive attention, as they show a high selectivity in the electrochemical conversion of CO2 to CO. In this work, we propose new strategy covalently graft cobalt porphyrin onto surface carbon nanotube by substitution reaction at metal center. Material characterization and studies reveal that molecules are well dispersed loading 10 wt. %. As result, turnover frequency for CO formation is improved factor three compared traditional physically-mixed catalysts same content. This leads an outstanding overall current density 25.1 mA cm-2 Faradaic efficiency 98.3 % 490 mV overpotential excellent long-term stability. work provides effective pathway improvement performance electrocatalysts could inspire rational design molecular future.

Language: Английский

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TiO₂-based heterojunction photocatalysts for photocatalytic reduction of CO₂into solar fuels

Journal of Materials Chemistry A, Journal Year: 2018, Volume and Issue: 6(45), P. 22411 - 22436

Published: Jan. 1, 2018

Recent advances in the photocatalytic reduction of CO₂into solar fuels using TiO₂-based heterojunction photocatalysts have been highlighted.

Language: Английский

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