Construction of C–N bonds from small-molecule precursors through heterogeneous electrocatalysis

Nature Reviews Chemistry, Journal Year: 2022, Volume and Issue: 6(5), P. 303 - 319

Published: April 25, 2022

Language: Английский

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Interfacial Electrolyte Effects on Electrocatalytic CO₂ Reduction

ACS Catalysis, Journal Year: 2021, Volume and Issue: 12(1), P. 331 - 362

Published: Dec. 16, 2021

Electrocatalytic CO2 reduction (CO2RR), powered by renewable energy, has great potential in decreasing the concentration of atmosphere, as well producing high value-added fuels or chemicals. The electrode and electrolyte together determine catalytic performance CO2RR. Despite substantial progress been made design preparation high-performance catalysts, role at electrode–electrolyte interface (EEI) which could largely affect local environment not understood thoroughly. To maximize balance (i.e., activity, selectivity, stability) CO2RR from a standpoint application, fundamental understanding interfacial effects should be emphasized with equal importance to intrinsic properties catalyst. In this Review, we will focus on discussion (effects) electrolytes for We summarize according their compositions chemical environment, include solvents, pH, cations, anions, impurities, additives, modifiers. addition, in-depth investigations detection intermediates during reactions using situ spectroscopy techniques are included. mechanisms, current challenges, future developments, perspectives discussed.

Language: Английский

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Design strategies for markedly enhancing energy efficiency in the electrocatalytic CO₂ reduction reaction

Energy & Environmental Science, Journal Year: 2022, Volume and Issue: 15(9), P. 3603 - 3629

Published: Jan. 1, 2022

The review summarizes the recent strategies to improve energy efficiency of CO 2 electroreduction, a guiding metric for industrial application and economic feasibility, with emphasis on designing remarkable catalyst advanced electrolysis system.

Language: Английский

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Carbon-efficient carbon dioxide electrolysers

Nature Sustainability, Journal Year: 2022, Volume and Issue: 5(7), P. 563 - 573

Published: May 12, 2022

Language: Английский

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Bifunctional ionomers for efficient co-electrolysis of CO2 and pure water towards ethylene production at industrial-scale current densities

Nature Energy, Journal Year: 2022, Volume and Issue: 7(9), P. 835 - 843

Published: Aug. 18, 2022

Language: Английский

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Coverage-driven selectivity switch from ethylene to acetate in high-rate CO2/CO electrolysis

Nature Nanotechnology, Journal Year: 2023, Volume and Issue: 18(3), P. 299 - 306

Published: Jan. 12, 2023

Language: Английский

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Engineering Catalyst–Electrolyte Microenvironments to Optimize the Activity and Selectivity for the Electrochemical Reduction of CO₂ on Cu and Ag

Accounts of Chemical Research, Journal Year: 2022, Volume and Issue: 55(4), P. 484 - 494

Published: Feb. 1, 2022

ConspectusThe electrochemical reduction of carbon dioxide (CO2R) driven by renewably generated electricity (e.g., solar and wind) offers a promising means for reusing the CO2 released during production cement, steel, aluminum as well ammonia methanol. If could be removed from atmosphere at acceptable costs (i.e., <$100/t CO2), then CO2R used to produce carbon-containing chemicals fuels in fully sustainable manner. Economic considerations dictate that current densities must range 0.1 1 A/cm2 selectivity toward targeted product high order minimize separation costs. Industrially relevant operating conditions can achieved using gas diffusion electrodes (GDEs) maximize transport species cathode combining such with solid-electrolyte membrane eliminating ohmic losses associated liquid electrolytes. Additionally, attained careful tuning microenvironment near catalyst surface pH, concentrations H2O, identities cations double layer adjacent surface).We begin this Account discussion our experimental theoretical work aimed optimizing microenvironments CO2R. We first examine effects morphology on multicarbon (C2+) products over Cu-based catalysts explore role mass transfer combined kinetics buffer reactions local concentration pH surface. This is followed dependence dynamics formation specific both Cu Ag catalysts. Next, we impact electrolyte cation identity rate distribution products. Subsequently, look utilizing pulsed electrolysis tune The last part demonstrates ionomer-coated combination enable attainment very (>90%) C2+ an aqueous electrolyte. extended consider difference catalyst–nanoparticle microenvironment, present electrode assembly (MEA), respect planar immersed

Language: Английский

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Multiscale CO₂ Electrocatalysis to C₂₊ Products: Reaction Mechanisms, Catalyst Design, and Device Fabrication

Chemical Reviews, Journal Year: 2023, Volume and Issue: 123(17), P. 10530 - 10583

Published: Aug. 17, 2023

Electrosynthesis of value-added chemicals, directly from CO2, could foster achievement carbon neutral through an alternative electrical approach to the energy-intensive thermochemical industry for utilization. Progress in this area, based on electrogeneration multicarbon products CO2 electroreduction, however, lags far behind that C1 products. Reaction routes are complicated and kinetics slow with scale up high levels required commercialization, posing significant problems. In review, we identify summarize state-of-art progress synthesis a multiscale perspective discuss current hurdles be resolved generation reduction including atomistic mechanisms, nanoscale electrocatalysts, microscale electrodes, macroscale electrolyzers guidelines future research. The review ends cross-scale links discrepancies between different approaches extensions performance stability issues arise industrial environment.

Language: Английский

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Engineering Water Molecules Activation Center on Multisite Electrocatalysts for Enhanced CO₂ Methanation

Journal of the American Chemical Society, Journal Year: 2022, Volume and Issue: 144(28), P. 12807 - 12815

Published: July 5, 2022

The renewable energy-powered electrolytic reduction of carbon dioxide (CO2) to methane (CH4) using water as a reaction medium is one the most promising paths store intermittent energy and address global sustainability problems. However, role in electrolyte often overlooked. In particular, slow dissociation kinetics limits proton-feeding rate, which severely damages selectivity activity methanation process involving multiple electrons protons transfer. Here, we present novel tandem catalyst comprising Ir single-atom (Ir1)-doped hybrid Cu3N/Cu2O multisite that operates efficiently converting CO2 CH4. Experimental theoretical calculation results reveal Ir1 facilitates into proton feeds sites for *CO protonation pathway toward *CHO. displays high Faradaic efficiency 75% CH4 with current density 320 mA cm-2 flow cell. This work provides strategy rational design high-efficiency catalytic systems.

Language: Английский

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Tunable CO2 electroreduction to ethanol and ethylene with controllable interfacial wettability

Nature Communications, Journal Year: 2023, Volume and Issue: 14(1)

Published: June 16, 2023

The mechanism of how interfacial wettability impacts the CO2 electroreduction pathways to ethylene and ethanol remains unclear. This paper describes design realization controllable equilibrium kinetic-controlled *CO *H via modifying alkanethiols with different alkyl chain lengths reveal its contribution pathways. Characterization simulation that mass transport H2O is related wettability, which may result in variation ratio, affects Through modulating hydrophilic interface superhydrophobic interface, reaction limitation shifts from insufficient supply *H. ratio can be continuously tailored a wide range 0.9 1.92, remarkable Faradaic efficiencies toward multi-carbon (C2+) products up 53.7% 86.1%, respectively. A C2+ efficiency 80.3% achieved high partial current density 321 mA cm-2, among highest selectivity at such densities.

Language: Английский

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