Electrochemical reduction of carbon dioxide to multicarbon (C₂₊) products: challenges and perspectives

Energy & Environmental Science, Год журнала: 2023, Номер 16(11), С. 4714 - 4758

Опубликована: Янв. 1, 2023

This review analyzes advanced catalysts and C 2+ synthesis mechanisms based on theoretical explorations in situ / operando characterizations. Triphasic interface optimization is discussed for the potential of industry-compatible stability.

Язык: Английский

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

Chemical Reviews, Год журнала: 2023, Номер 123(17), С. 10530 - 10583

Опубликована: Авг. 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.

Язык: Английский

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Hydrophobic, Ultrastable Cu^δ+ for Robust CO₂ Electroreduction to C₂ Products at Ampere-Current Levels

Journal of the American Chemical Society, Год журнала: 2023, Номер 145(20), С. 11323 - 11332

Опубликована: Май 11, 2023

Copper (Cu) is the only known material that can efficiently electrocatalyze CO2 to value-added multicarbon products. Owing instability of Cuδ+ state and microscopic structure in reactions, Cu catalysts are still facing big challenges with low selectivity poor durability, particularly at high current densities. Herein, we report a rational one-step surface coordination approach for synthesis dendrites an ultrastable hydrophobicity (Cu CF), even after exposure air over 6 months. As result, CF exhibited C2 FE 90.6% partial density 453.3 mA cm-2 flow cell. A 400 h stable electrolysis 800 ground-breaking operation large industrial 10 were achieved membrane electrode assembly (MEA) form. We further demonstrated continuous production C2H5OH solution 90% relative purity 600 50 solid-electrolyte reactor. Spectroscopy computation results suggested Cu(II) carboxylate species formed on CF, which ensured stability hydrophobicity. rich active sites three-phase interface catalyst achieved, along optimized *CO adsorption strength configuration. The mixed configurations made dimerization process easier, promoted conversion This work provides promising paradigm design development Cu-based ultrahigh under

Язык: Английский

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Electrochemical Carbon Dioxide Reduction to Ethylene: From Mechanistic Understanding to Catalyst Surface Engineering

Nano-Micro Letters, Год журнала: 2023, Номер 15(1)

Опубликована: Июль 11, 2023

Electrochemical carbon dioxide reduction reaction (CO2RR) provides a promising way to convert CO2 chemicals. The multicarbon (C2+) products, especially ethylene, are of great interest due their versatile industrial applications. However, selectively reducing ethylene is still challenging as the additional energy required for C-C coupling step results in large overpotential and many competing products. Nonetheless, mechanistic understanding key steps preferred pathways/conditions, well rational design novel catalysts production have been regarded approaches achieving highly efficient selective CO2RR. In this review, we first illustrate CO2RR (e.g., adsorption/activation, formation *CO intermediate, step), offering conversion ethylene. Then alternative pathways conditions competitive products (C1 other C2+ products) investigated, guiding further development generation. Engineering strategies Cu-based CO2RR-ethylene summarized, correlations mechanism/pathways, engineering selectivity elaborated. Finally, major challenges perspectives research area proposed future practical

Язык: Английский

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Engineering Cu(I)/Cu(0) interfaces for efficient ethanol production from CO2 electroreduction

Chem, Год журнала: 2023, Номер 10(1), С. 211 - 233

Опубликована: Сен. 21, 2023

Язык: Английский

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Zeolitic imidazolate framework-67 and its derivatives for photocatalytic applications

Coordination Chemistry Reviews, Год журнала: 2023, Номер 502, С. 215612 - 215612

Опубликована: Дек. 18, 2023

Язык: Английский

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Local CO2 reservoir layer promotes rapid and selective electrochemical CO2 reduction

Nature Communications, Год журнала: 2024, Номер 15(1)

Опубликована: Апрель 22, 2024

Abstract Electrochemical CO 2 reduction reaction in aqueous electrolytes is a promising route to produce added-value chemicals and decrease carbon emissions. However, even Gas-Diffusion Electrode devices, low solubility limits catalysis rate selectivity. Here, we demonstrate that when assembled over heterogeneous electrocatalyst, film of nitrile-modified Metal-Organic Framework (MOF) acts as remarkable -solvation layer increases its local concentration by ~27-fold compared bulk electrolyte, reaching 0.82 M. When mounted on Bi catalyst Gas Diffusion Electrode, the MOF drastically improves -to-HCOOH conversion, above 90% selectivity partial HCOOH currents 166 mA/cm (at −0.9 V vs RHE). The also facilitates through stabilization intermediates, identified operando infrared spectroscopy Density Functional Theory. Hence, presented strategy provides new molecular means enhance electrochemical reaction, leading it closer requirements for practical implementation.

Язык: Английский

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Recent Progress of Transition Metal Selenides for Electrochemical Oxygen Reduction to Hydrogen Peroxide: From Catalyst Design to Electrolyzers Application

Small, Год журнала: 2024, Номер 20(22)

Опубликована: Фев. 16, 2024

Abstract Hydrogen peroxide (H 2 O ) is a highly value‐added and environmental‐friendly chemical with various applications. The production of H by electrocatalytic 2e − oxygen reduction reaction (ORR) has emerged as promising alternative to the energy‐intensive anthraquinone process. High selectivity Catalysts combining superior activity are critical for efficient electrosynthesis . Earth‐abundant transition metal selenides (TMSs) being discovered classic stable, low‐cost, active selective catalysts electrochemical ORR. These features come from relatively large atomic radius selenium element, metal‐like properties abundant reserves. Moreover, compared advanced noble or single‐atom catalysts, kinetic current density TMSs generation higher in acidic solution, which enable them become suitable catalyst candidates. Herein, recent progress ORR systematically reviewed. effects electrocatalysts on activity, stability summarized. It intended provide an insight design corresponding mechanisms device setup, discuss relationship between structure activity.

Язык: Английский

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Identification of Cu0/Cu+/Cu0 interface as superior active sites for CO2 electroreduction to C2+ in neutral condition

Chem, Год журнала: 2024, Номер 10(7), С. 2089 - 2102

Опубликована: Март 15, 2024

Язык: Английский

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CO2 electrochemical reduction: A state-of-the-art review with economic and environmental analyses

Process Safety and Environmental Protection, Год журнала: 2024, Номер 208, С. 934 - 955

Опубликована: Июль 14, 2024

The electrochemical reduction of carbon dioxide is an emerging strategy to reduce emissions, allowing the storage renewable energy and electrification chemical industry according principle utilization. Valuable fuels commodities can be obtained by ensuring a closed loop main important products are monoxide, formic acid, methanol, methane, ethylene, ethanol, propanol. Inside this context, here, we explore state-of-the-art electrolysis technologies, showing that efforts have been put into development reactor cell architectures catalysts able provide high selectivity efficiency. New insights currently about study reaction mechanisms, optimization design, more performing electro-catalysts. Moreover, overview economic environmental studies based on conducted in work preliminary screening levelized production cost climate change impact several through proposed for large-scale plant. Today, monoxide acid primary product targets from point view. In future, costs expected decrease, other low-carbon could competitive with market prices. Renewable sources low footprint contribute environmentally friendly process.

Язык: Английский

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