Cu-Zn-based alloy/oxide interfaces for enhanced electroreduction of CO2 to C2+ products

Journal of Energy Chemistry, Год журнала: 2023, Номер 83, С. 90 - 97

Опубликована: Май 11, 2023

Язык: Английский

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A Stable and Conductive Covalent Organic Framework with Isolated Active Sites for Highly Selective Electroreduction of Carbon Dioxide to Acetate

Angewandte Chemie International Edition, Год журнала: 2022, Номер 61(36)

Опубликована: Июнь 13, 2022

Electroreduction of CO2 to acetate provides a promising strategy reduce emissions and store renewable energy, but is usually by-product. Here, we show stable conductive two-dimensional phthalocyanine-based covalent-organic framework (COF) as an electrocatalyst for reduction with single-product Faradaic efficiency (FE) 90.3(2)% at -0.8 V (vs. RHE) current density 12.5 mA cm-2 in 0.1 M KHCO3 solution. No obvious degradation was observed over 80 hours continuous operation. Combined the comparison properties other catalysts isolated metal active sites, theoretical calculations situ infrared spectroscopy revealed that copper-phthalocyanine site high electron conducive key step C-C coupling *CH3 produce acetate, can avoid *CO or *CHO ethylene ethanol.

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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Synthesis of porous poly(ionic liquid)s for chemical CO₂fixation with epoxides

Green Chemistry, Год журнала: 2022, Номер 24(9), С. 3433 - 3460

Опубликована: Янв. 1, 2022

Porous poly(ionic liquid)s, combining the features of porous polymers and ionic moieties resembling structures functions liquids, have exhibited promising potential in CO 2 fixation via cycloadditions with epoxides.

Язык: Английский

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Energy Applications of Ionic Liquids: Recent Developments and Future Prospects

Chemical Reviews, Год журнала: 2023, Номер 123(21), С. 12170 - 12253

Опубликована: Окт. 25, 2023

Ionic liquids (ILs) consisting entirely of ions exhibit many fascinating and tunable properties, making them promising functional materials for a large number energy-related applications. For example, ILs have been employed as electrolytes electrochemical energy storage conversion, heat transfer fluids phase-change thermal storage, solvents and/or catalysts CO2 capture, biomass treatment biofuel extraction, high-energy propellants aerospace This paper provides an extensive overview on the various applications offers some thinking viewpoints current challenges emerging opportunities in each area. The basic fundamentals (structures properties) are first introduced. Then, motivations successful field concisely outlined. Later, detailed review recent representative works area is provided. application, role their associated benefits elaborated. Research trends insights into selection to achieve improved performance analyzed well. Challenges future pointed out before concluded.

Язык: Английский

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Selective CO₂ Reduction to Ethylene Mediated by Adaptive Small‐molecule Engineering of Copper‐based Electrocatalysts

Angewandte Chemie International Edition, Год журнала: 2023, Номер 62(50)

Опубликована: Окт. 30, 2023

Electrochemical CO2 reduction reaction (CO2 RR) over Cu catalysts exhibits enormous potential for efficiently converting to ethylene (C2 H4 ). However, achieving high C2 selectivity remains a considerable challenge due the propensity of undergo structural reconstruction during RR. Herein, we report an in situ molecule modification strategy that involves tannic acid (TA) molecules adaptive regulating Cu-based material pathway facilitates products. An excellent Faraday efficiency (FE) 63.6 % on with current density 497.2 mA cm-2 flow cell was achieved, about 6.5 times higher than pristine catalyst which mainly produce CH4 . The X-ray absorption spectroscopy and Raman studies reveal hydroxyl group TA stabilizes Cuδ+ Furthermore, theoretical calculations demonstrate /Cu0 interfaces lower activation energy barrier *CO dimerization, species stabilize *COH intermediate via hydrogen bonding, thereby promoting production. Such engineering modulated electronic structure provides promising achieve highly selective value-added chemicals.

Язык: Английский

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SiO₂ assisted Cu⁰–Cu⁺–NH₂ composite interfaces for efficient CO₂ electroreduction to C₂₊ products

Journal of Materials Chemistry A, Год журнала: 2023, Номер 12(2), С. 1218 - 1232

Опубликована: Дек. 13, 2023

SiO 2 assisted abundant Cu 0 –Cu + –NH composite interfaces enhance the adsorption and activation of CO H O, strengthen intermediates, promote C–C coupling to produce C 2+ products.

Язык: Английский

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Challenges and strategies towards copper-based catalysts for enhanced electrochemical CO2 reduction to multi-carbon products

Fuel, Год журнала: 2022, Номер 332, С. 126114 - 126114

Опубликована: Окт. 2, 2022

Язык: Английский

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Superscalar Phase Boundaries Derived Multiple Active Sites in SnO₂/Cu₆Sn₅/CuO for Tandem Electroreduction of CO₂ to Formic Acid

Advanced Energy Materials, Год журнала: 2023, Номер 13(13)

Опубликована: Фев. 12, 2023

Abstract The electrocatalytic CO 2 reduction reaction (CO RR) to fuels driven by electrocatalysts is a viable strategy for efficient utilization of emitted . RR involves multiple‐steps, including adsorption, activation, hydrogenation, etc. At present, copper‐tin alloy catalysts have shown the capability reduce formic acid or formate. However, their poor adsorption and activation capacities molecules, as well sluggish kinetics in *H supply restrict proton‐coupled electron transfer processes produce acid. In order solve above problems, ultra‐small SnO /Cu 6 Sn 5 /CuO nanocatalysts with superscalar phase boundaries are fabricated laser sputtering. introduction enhances , while CuO promotes H O decomposition provides abundant intermediates, resulting tandem catalytic sites on composite thus leading excellent activity high selectivity Faradic efficiency (FE HCOOH ) at electrode reaches 90.13% along current density 25.2 mA cm −2 −0.95 V versus reversible hydrogen electrode. role multiphase constructed oxides confirmed situ infrared spectroscopy kinetic isotope effects experiments, which consistent design concept.

Язык: Английский

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Gas diffusion enhanced electrode with ultrathin superhydrophobic macropore structure for acidic CO2 electroreduction

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

Опубликована: Янв. 15, 2024

Abstract Carbon dioxide (CO 2 ) electroreduction reaction RR) offers a promising strategy for the conversion of CO into valuable chemicals and fuels. RR in acidic electrolytes would have various advantages due to suppression carbonate formation. However, its rate is severely limited by slow diffusion absence hydroxide that facilitates an environment. Here, we design optimal architecture gas electrode (GDE) employing copper-based ultrathin superhydrophobic macroporous layer, which highly enhanced. This GDE retains applicability even under mechanical deformation conditions. The exhibits Faradaic efficiency 87% with partial current density $$( {j}_{{{{\rm{C}}}}_{2+}})$$ ( j C 2 + ) −1.6 A cm −2 multicarbon products (C 2+ ), $$ {j}_{{{{{{\rm{C}}}}}}_{2+}}$$ −0.34 when applying dilute 25% . In environment, C formation occurs via second order controlled both catalyst hydroxide.

Язык: Английский

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