Operando characterization techniques for electrocatalysis

Energy & Environmental Science, Год журнала: 2020, Номер 13(11), С. 3748 - 3779

Опубликована: Янв. 1, 2020

Significant progress toward the understanding of electrochemical process has been achieved in past decades, owning to advancements operando characterization techniques.

Язык: Английский

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Recent Progresses in Electrochemical Carbon Dioxide Reduction on Copper‐Based Catalysts toward Multicarbon Products

Advanced Functional Materials, Год журнала: 2021, Номер 31(37)

Опубликована: Июнь 26, 2021

Abstract Electrochemical carbon dioxide reduction reaction (CO 2 RR) offers a promising way of effectively converting CO to value‐added chemicals and fuels by utilizing renewable electricity. To date, the electrochemical single‐carbon products, especially monoxide formate, has been well achieved. However, efficient conversion more valuable multicarbon products (e.g., ethylene, ethanol, n ‐propanol, ‐butanol) is difficult still under intense investigation. Here, recent progresses in using copper‐based catalysts are reviewed. First, mechanism RR briefly described. Then, representative approaches catalyst engineering introduced toward formation RR, such as composition, morphology, crystal phase, facet, defect, strain, surface interface. Subsequently, key aspects cell for including electrode, electrolyte, design, also discussed. Finally, advances summarized some personal perspectives this research direction provided.

Язык: Английский

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Noble-Metal-Free Multicomponent Nanointegration for Sustainable Energy Conversion

Chemical Reviews, Год журнала: 2021, Номер 121(17), С. 10271 - 10366

Опубликована: Июль 6, 2021

Global energy and environmental crises are among the most pressing challenges facing humankind. To overcome these challenges, recent years have seen an upsurge of interest in development production renewable chemical fuels as alternatives to nonrenewable high-polluting fossil fuels. Photocatalysis, photoelectrocatalysis, electrocatalysis provide promising avenues for sustainable conversion. Single- dual-component catalytic systems based on nanomaterials been intensively studied decades, but their intrinsic weaknesses hamper practical applications. Multicomponent nanomaterial-based systems, consisting three or more components with at least one component nanoscale, recently emerged. The multiple integrated together create synergistic effects hence limitation outperformance. Such higher-efficiency will potentially bring additional benefit balance-of-system costs if they exclude use noble metals, considering expense sustainability. It is therefore timely review research this field, providing guidance noble-metal-free multicomponent nanointegration In work, we first recall fundamentals catalysis by nanomaterials, nanointegration, reactor configuration water splitting, CO2 reduction, N2 reduction. We then systematically discuss advances multicomponent-based photocatalytic, photoelectrochemical, electrochemical nanomaterials. On basis further laterally evaluate different integration strategies highlight impacts activity, performance stability, product selectivity. Finally, conclusions future prospects nanointegration. This work offers comprehensive insights into cost-competitive energy-conversion technologies assists researchers working toward addressing global environment.

Язык: Английский

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High‐Entropy Alloys for Electrocatalysis: Design, Characterization, and Applications

Small, Год журнала: 2021, Номер 18(7)

Опубликована: Ноя. 5, 2021

Abstract High‐entropy alloys (HEAs) are expected to function well as electrocatalytic materials, owing their widely adjustable composition and unique physical chemical properties. Recently, HEA catalysts extensively studied in the field of electrocatalysis; this motivated authors investigate relationship between structure HEAs performance. In review, latest advances electrocatalysts systematically summarized, with special focus on nitrogen fixation, carbon cycle, water splitting, fuel cells; addition, by combining characterization analysis microstructures, rational design strategies for optimizing electrocatalysts, including controllable preparation, component regulation, strain engineering, defect theoretical prediction proposed. Moreover, existing issues future trends predicted, which will help further develop these high‐entropy materials.

Язык: Английский

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Electrochemical CO₂ Reduction to Ethanol with Copper-Based Catalysts

ACS Energy Letters, Год журнала: 2021, Номер 6(2), С. 694 - 706

Опубликована: Янв. 27, 2021

Electrochemical CO2 reduction presents a sustainable route to storage of intermittent renewable energy. Ethanol is an important target product, which used as fuel additive and chemical feedstock. However, electrochemical ethanol production challenging, it involves the transfer multiple electrons protons alongside C–C bond formation. To date, most commonly employed effective catalysts are copper-based materials. This Review categorizes efficient selective Cu-based electrocatalysts, divided into three main groups: oxide-derived copper, bimetallics, copper- nitrogen-doped carbon Only few other specific examples fall outside this classification. The catalytic performance these materials for in aqueous conditions discussed terms current density, overpotential, faradaic efficiency. A critical evaluation factors that contribute high provided aid design more

Язык: Английский

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Quasi-graphitic carbon shell-induced Cu confinement promotes electrocatalytic CO2 reduction toward C2+ products

Nature Communications, Год журнала: 2021, Номер 12(1)

Опубликована: Июнь 21, 2021

Abstract For steady electroconversion to value-added chemical products with high efficiency, electrocatalyst reconstruction during electrochemical reactions is a critical issue in catalyst design strategies. Here, we report reconstruction-immunized system which Cu nanoparticles are protected by quasi-graphitic C shell. This shell epitaxially grew on bonding via gas–solid reaction governed the CO (g) - 2 (s) equilibrium. The shell-coated was stable reduction and provided platform for rational material design. 2+ product selectivity could be additionally improved doping p -block elements. These elements modulated electronic structure of surface its binding properties, can affect intermediate dimerization barrier. B-modified attained 68.1% Faradaic efficiency H 4 at −0.55 V (vs RHE) cathodic power conversion 44.0%. In case N-modified Cu, an 82.3% partial current density 329.2 mA/cm acquired. Quasi-graphitic shells, enable stabilization inner element doping, realize -to-C over 180 h allow practical application electrocatalysts renewable energy conversion.

Язык: Английский

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Electrocatalytic Valorization of Poly(ethylene terephthalate) Plastic and CO₂ for Simultaneous Production of Formic Acid

ACS Catalysis, Год журнала: 2022, Номер 12(11), С. 6722 - 6728

Опубликована: Май 23, 2022

The electro-reforming of polymer plastic waste and CO2 has the merits for producing value-added chemicals alleviating environmental pollution. Herein, we report an electrocatalytic integrating strategy efficient valorization poly(ethylene terephthalate) (PET) to simultaneously produce formic acid at both anode cathode. NiCo2O4 electrocatalyst displays a high Faradaic efficiency 90% production, which indicates excellent selectivity PET hydrolysate oxidation. By coupling oxidation reaction with reduction reaction, assembled electrolyzer exhibits low cell voltage 1.55 V drive integrated two half-reactions. Furthermore, 155% can be achieved 1.90 V. This study suggests that could energy-efficient economically viable realize production chemicals.

Язык: Английский

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Defect Engineering on Carbon-Based Catalysts for Electrocatalytic CO2 Reduction

Nano-Micro Letters, Год журнала: 2020, Номер 13(1)

Опубликована: Окт. 27, 2020

Abstract Electrocatalytic carbon dioxide (CO 2 ) reduction (ECR) has become one of the main methods to close broken cycle and temporarily store renewable energy, but there are still some problems such as poor stability, low activity, selectivity. While most promising strategy improve ECR activity is develop electrocatalysts with cost, high long-term stability. Recently, defective carbon-based nanomaterials have attracted extensive attention due unbalanced electron distribution electronic structural distortion caused by defects on materials. Here, present review mainly summarizes latest research progress construction diverse types (intrinsic defects, heteroatom doping metal atomic sites, edges detects) for materials in ECR, unveil structure–activity relationship its catalytic mechanism. The current challenges opportunities faced high-performance discussed, well possible future solutions. It can be believed that this provide inspiration development catalysts.

Язык: Английский

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Electrochemical CO2 reduction in membrane-electrode assemblies

Chem, Год журнала: 2022, Номер 8(3), С. 663 - 692

Опубликована: Янв. 10, 2022

Язык: Английский

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CO2 electroreduction to multicarbon products in strongly acidic electrolyte via synergistically modulating the local microenvironment

Nature Communications, Год журнала: 2022, Номер 13(1)

Опубликована: Дек. 9, 2022

Electrochemical CO2 reduction to multicarbon products faces challenges of unsatisfactory selectivity, productivity, and long-term stability. Herein, we demonstrate electroreduction in strongly acidic electrolyte (pH ≤ 1) on electrochemically reduced porous Cu nanosheets by combining the confinement effect cation synergistically modulate local microenvironment. A Faradaic efficiency 83.7 ± 1.4% partial current density 0.56 0.02 cm-2, single-pass carbon 54.4%, stable electrolysis 30 h a flow cell are demonstrated for aqueous consisting sulfuric acid KCl with pH 1. Mechanistically, accumulated species (e.g., K+ OH-) Helmholtz plane account selectivity activity toward kinetically reducing proton coverage thermodynamically favoring conversion. We find that cations facilitate C-C coupling through interaction between key intermediate *OCCO.

Язык: Английский

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