Electrochemical Oxidation of Small Molecules for Energy‐Saving Hydrogen Production

Advanced Energy Materials, Год журнала: 2024, Номер 14(30)

Опубликована: Май 27, 2024

Abstract Electrochemical water splitting is a promising technique for the production of high‐purity hydrogen. Substituting slow anodic oxygen evolution reaction with an oxidation that thermodynamically more favorable enables energy‐efficient Moreover, this approach facilitates degradation environmental pollutants and synthesis value‐added chemicals through rational selection small molecules as substrates. Strategies small‐molecule electrocatalyst design are critical to electrocatalytic performance, focus on achieving high current density, selectivity, Faradaic efficiency, operational durability. This perspective discusses key factors required further advancement, including technoeconomic analysis, new reactor system design, meeting requirements industrial applications, bridging gap between fundamental research practical product detection separation. aims advance development hybrid electrolysis applications.

Язык: Английский

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High‐Surface Area Mesoporous Sc₂O₃ with Abundant Oxygen Vacancies as New and Advanced Electrocatalyst for Electrochemical Biomass Valorization

Advanced Materials, Год журнала: 2024, Номер 36(16)

Опубликована: Янв. 15, 2024

Abstract Scandium oxide (Sc 2 O 3 ) is considered as omnipotent “Industrial Ajinomoto” and holds promise in catalytic applications. However, rarely little attention paid to its electrochemistry. Here, the first nanocasting design of high‐surface area Sc with abundant oxygen vacancies (mesoporous V ‐Sc for efficient electrochemical biomass valorization reported. In case electro‐oxidation 5‐hydroxymethylfurfural (HMF) 2,5‐furandicarboxylic acid (FDCA), quantitative HMF conversion, high yield, faradic efficiency FDCA via hydroxymethylfurancarboxylic pathway are achieved by this advanced electrocatalyst. The beneficial effect on electrocatalytic performance mesoporous revealed enhanced adsorption reactants reduced energy barrier process. concerted design, situ ex experimental studies theoretical calculations shown work should shed light rational elaboration electrocatalysts, contribute establishment a circular carbon economy since bio‐plastic monomer green hydrogen efficiently synthesized.

Язык: Английский

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Iron Molybdenum Sulfide‐Supported Ultrafine Ru Nanoclusters for Robust Sulfion Degradation‐Assisted Hydrogen Production

Advanced Functional Materials, Год журнала: 2024, Номер 34(27)

Опубликована: Март 5, 2024

Abstract Electrocatalytic hydrogen evolution and (S 2− ) recycling present promising strategies for cost‐effective production simultaneous removal of environmental pollutants. However, the advancement this technology is hindered by limited availability affordable, efficient, stable catalysts. Herein, study synthesizes ultrafine ruthenium (Ru) nanoclusters on a substrate iron molybdenum sulfide (FeMo‐S) nanosheets, creating new heterointerface catalyst (FeMo‐S/Ru) reaction (HER) sulfion oxidation (SOR). Experimental theoretical calculations suggest that strong electron interactions between Ru FeMo‐S substrate, optimizing *H adsorption promoting HER activity one side while facilitating sulfur intermediates other side, effectively catalyzing SOR. Additionally, assembled electrocatalytic coupling system with FeMo‐S/Ru displays an ultralow cell voltage 0.57 V at 100 mA cm −2 , achieving high Faradaic efficiencies (>96%) H 2 production, also exhibiting remarkable durability over 1 month (838 h). This work paves way development highly efficient durable supported catalysts, enabling energy‐saving environmentally friendly recycling.

Язык: Английский

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On the Activity and Selectivity of 5-Hydroxymethylfurfural Electrocatalytic Oxidation over Cation-Defective Nickel Hydroxides

ACS Catalysis, Год журнала: 2024, Номер 14(12), С. 9565 - 9574

Опубликована: Июнь 10, 2024

Язык: Английский

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Integrated electrochemical and chemical system for ampere-level production of terephthalic acid alternatives and hydrogen

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

Опубликована: Сен. 14, 2024

Язык: Английский

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Synergistic enhancement of electrochemical alcohol oxidation by combining NiV-layered double hydroxide with an aminoxyl radical

Nature Communications, Год журнала: 2025, Номер 16(1)

Опубликована: Янв. 2, 2025

Electrochemical alcohol oxidation (EAO) represents an effective method for the production of high-value carbonyl products. However, its industrial viability is hindered by suboptimal efficiency stemming from low reaction rates. Here, we present a synergistic electrocatalysis approach that integrates active electrode and aminoxyl radical to enhance performance EAO. The optimal (4-acetamido-2,2,6,6-tetramethylpiperidine 1-oxyl) Ni0.67V0.33-layered double hydroxide (LDH) are screen as cooperative electrocatalysts integrating theoretical predictions experiments. Ni0.67V0.33-LDH facilitates adsorption activation N-(1-hydroxy-2,2,6,6-tetramethylpiperidin-4-yl)acetamide (ACTH) via interactions with ketonic oxygen, thereby improving selectivity yield at high current densities. electrolysis process scaled up produce 200 g steroid product 8b (19-Aldoandrostenedione), achieving 91% productivity 243 h-1. These results represent promising accelerating electron transfer oxidation, highlighting potential practical electrosynthesis applications. electrooxidation due authors report (Ni0.67V0.33-layered hydroxide) alcohols

Язык: Английский

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Regulating Intermediate Adsorption and Promoting Charge Transfer of CoCr‐LDHs by Ce Doping for Enhancing Electrooxidation of 5‐Hydroxymethylfurfural

Small, Год журнала: 2025, Номер unknown

Опубликована: Янв. 14, 2025

Abstract Electrochemical oxidation of 5‐hydroxymethylfurfural (HMFOR) to generate high‐value chemicals under mild conditions acts as an energy‐saving and sustainable strategy. However, it is still challenging develop electrocatalysts with high efficiency good durability. Here, nickel foam (NF) supported CoCrCe(7.5%)‐LDH (layered double hydroxides) by doping Ce into CoCr‐LDH show (HMF) conversion (99%), 2,5‐furandicarboxylic acid (FDCA) yield Faraday (100%) at 1.4 V RHE . The also exhibits remarkable stability 97% HMF after 10 cycles. X‐ray absorption near‐edge spectroscopy (XANES) theoretical calculation that beneficial the formation high‐valance Co significantly facilitates electron transfer, regulates adsorption behavior intermediates, reduces Gibbs free energy barrier accelerates reaction rate. This work promotes use rare earth elements promote HMF.

Язык: Английский

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Theoretical Exploration of the Origin of Alkaline Dependence in the Oxidation of 5-Hydroxymethylfurfural Catalyzed by NiO₂H_x

ACS Catalysis, Год журнала: 2024, Номер 14(13), С. 9860 - 9869

Опубликована: Июнь 18, 2024

Alkaline dependence is a common phenomenon in the electrochemical oxidation of biomass, and investigating influence alkalinity on mechanisms crucial for enhancing both activity selectivity biomass oxidation. Herein, we constructed five NiO2Hx catalysts under different alkaline environments (pH ≈ 9–13) employed density functional theory methods to investigate reaction selective platform molecule 5-hydroxymethylfurfural (HMF). The origin HMF was analyzed, results indicate that catalyst determines pathway 2,5-furandicarboxylic acid: weak 9–11), adsorption activation alcohol group are more favorable, resulting preferential group; strong 11–13), aldehyde prone adsorb activate surface, predominant With increase NiO2Hx, there decrease H atom coverage an valence state Ni, transformation from as well transition mechanism direct indirect NiOOH moderately environment effectively reduces Gibbs free energy change C–H/O–H bonds cleavage, lowering energy. It significantly enhances ability groups, exhibiting highest catalytic performance conversion FDCA. study not only provide comprehensive explanation but also offer guidance how rationally design improving oxidative through adjustments.

Язык: Английский

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Constructing Heteronuclear Bridging Atoms toward Bifunctional Electrocatalysis

ACS Catalysis, Год журнала: 2024, Номер 14(11), С. 8414 - 8426

Опубликована: Май 15, 2024

Superseding the oxygen evolution reaction with thermodynamically favorable and economically attractive organic oxidation is crucial to acquiring eco-friendly hydrogen production via an electrochemical process coupled renewable energy. A bifunctional electrocatalyst, Ru@NixCo1–x(OH)2, featuring a dandelion-liked structure assembled into two-electrode configuration, requires voltage of 1.35 V for cathode H2 anode 2,5-furandicarboxylic acid. The heteronuclear bridging atoms at Ru–Ni sites accelerate water splitting through Volmer–Tafel mechanism enhance *H coverage, as demonstrated by in situ spectroscopy analysis. Simultaneously, Ru–Co serve adsorption 5-hydroxymethylfurfural, achieving 100% Faradic efficiency selectivity. Upon upscaling configuration 2 × cm2 membrane electrode assembly reactor, FDCA rate 243 mg/h was achieved, electricity savings approximately 0.67 kWh/m3 (H2). This work offers promising avenue concurrent biomass upgrading industrial practicability.

Язык: Английский

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Nickel Hydroxide‐Based Electrocatalysts for Promising Electrochemical Oxidation Reactions: Beyond Water Oxidation

Small, Год журнала: 2024, Номер 20(33)

Опубликована: Март 20, 2024

Transition metal hydroxides have attracted significant research interest for their energy storage and conversion technique applications. In particular, nickel hydroxide (Ni(OH)

Язык: Английский

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