Enhancing Electrocatalytic Activity Through Targeted Local Electrolyte Micro‐Environment

Advanced Functional Materials, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 10, 2025

Abstract The local electrolyte micro‐environment surrounding the catalyst reaction center, including critical factors such as pH, reactant concentration, and electric field, plays a decisive role in electrocatalytic reactions water splitting. Recently, this topic has garnered significant attention due to its potential significantly enhance catalytic performance. While various strategies optimize processes have been explored, deliberate control over fundamental principles guiding these adjustments remain their early stages of development. This review provides comprehensive examination key efforts aimed at designing tailoring localized micro‐environments improve It discusses advances micro‐environmental design, methodologies for evaluating shifts, mechanistic insights driving developments. Additionally, highlights existing challenges prospective industrial applications strategies. By offering detailed analysis recent developments, aims equip researchers with practical knowledge on controlling micro‐environments, thereby accelerating progress toward real‐world processes.

Language: Английский

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Tuning the Formation Kinetics of *OOH Intermediate with Hollow Bowl-Like Carbon by Pulsed Electroreduction for Enhanced H₂O₂ Production

ACS Nano, Journal Year: 2025, Volume and Issue: unknown

Published: March 28, 2025

The electrochemical synthesis of hydrogen peroxide (H2O2) via the two-electron oxygen reduction reaction (2e- ORR) is a promising alternative to conventional anthraquinone method. However, due local alkalinization near catalyst surface, restricted replenishment and insufficient activated water molecule supply limit formation key *OOH intermediate. Herein, pulsed electrocatalysis approach based on structurally optimized S/N/O tridoped hollow carbon bowl has been proposed overcome this challenge. In an H-type electrolytic cell, method achieves superior H2O2 yield rate 55.6 mg h-1 mgcat.-1, approximately 1.6 times higher than potentiostatic (34.2 mgcat.-1), while maintaining Faradaic efficiency above 94.6%. situ characterizations, finite element simulations, density functional theory analyses unveil that application potentials mitigates OH- concentration, enhances activation proton generation, facilitates production within bowl-like structure. These effects synergistically accelerate kinetics intermediate by efficient generation *O2 *H2O intermediates, leading yields. This work develops strategy tune catalytic environments for diverse applications.

Language: Английский

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Microenvironment Engineering of Heterogeneous Catalysts for Liquid-Phase Environmental Catalysis

Chemical Reviews, Journal Year: 2024, Volume and Issue: 124(20), P. 11348 - 11434

Published: Oct. 9, 2024

Environmental catalysis has emerged as a scientific frontier in mitigating water pollution and advancing circular chemistry reaction microenvironment significantly influences the catalytic performance efficiency. This review delves into engineering within liquid-phase environmental catalysis, categorizing microenvironments four scales: atom/molecule-level modulation, nano/microscale-confined structures, interface surface regulation, external field effects. Each category is analyzed for its unique characteristics merits, emphasizing potential to enhance efficiency selectivity. Following this overview, we introduced recent advancements advanced material system design promote (e.g., purification, transformation value-added products, green synthesis), leveraging state-of-the-art technologies. These discussions showcase was applied different reactions fine-tune regimes improve from both thermodynamics kinetics perspectives. Lastly, discussed challenges future directions engineering. underscores of intelligent materials drive development more effective sustainable solutions decontamination.

Language: Английский

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Oxide-modified bifunctional carbonaceous cathode: oxygen-rich alkaline-like microenvironment strengthened hydrogen peroxide as an electron donor to enhance Fe3+ reduction in Fe(III) electro-Fenton

Process Safety and Environmental Protection, Journal Year: 2025, Volume and Issue: 196, P. 106847 - 106847

Published: Feb. 7, 2025

Language: Английский

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Metalloenzyme‐Inspired Cluster Fabrication within Mesoporous Channels Featuring Optimized Catalytic Microenvironments for Efficient Neutral pH H₂O₂ Electrosynthesis

Advanced Materials, Journal Year: 2025, Volume and Issue: unknown

Published: March 17, 2025

Abstract In nature, some metalloenzymes facilitate highly efficient catalytic transformations of small molecules, primarily attributed to the effective coupling between their metal cluster active sites and surrounding microenvironment. Inspired by this, a thermotropic redispersion strategy incorporate bismuth nanoclusters (Bi NCs) into mesoporous channels, mimicking metalloenzyme‐like catalysis enhance two‐electron oxygen reduction reaction (2e − ORR) for neutral pH H 2 O electrosynthesis, is developed. This model electrocatalyst exhibits exceptional 2e ORR performance with >95% selectivity across 0.2–0.6 V vs RHE in electrolyte. Notably, system produces up 7.2 wt% solution at an industrially relevant current density ≈320 mA cm −2 , 90% Faradaic efficiency over 120 h flow cell, demonstrating significant practical potential. Mechanistic insights reveal that introduction Bi NCs enhances adsorption *OOH intermediate, facilitating process. Moreover, channels carbon support create favorable microenvironment aeration local alkalinity, further boosting productivity. catalyst design mimics optimal integration site microenvironment, offering valuable rational nature‐inspired small‐molecule catalysts.

Language: Английский

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Hydrogen Peroxide Electrosynthesis via Selective Oxygen Reduction Reactions Through Interfacial Reaction Microenvironment Engineering

Advanced Materials, Journal Year: 2024, Volume and Issue: unknown

Published: Nov. 28, 2024

Abstract The electrochemical two‐electron oxygen reduction reaction (2e − ORR) offers a compelling alternative for decentralized and on‐site H 2 O production compared to the conventional anthraquinone process. To advance this electrosynthesis system, there is growing interest in optimizing interfacial microenvironment boost electrocatalytic performance. This review consolidates recent advancements engineering selective conversion of . Starting with fundamental insights into mechanisms, an overview various strategies constructing favorable local environment, including adjusting electrode wettability, enhancing mesoscale mass transfer, elevating pH, incorporating electrolyte additives, employing pulsed electrocatalysis techniques provided. Alongside these regulation strategies, corresponding analyses technical remarks are also presented. Finally, summary outlook on critical challenges, suggesting future research directions inspire accelerate practical application delivered.

Language: Английский

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Electronic regulation of metallic nanoparticles in cages enables thermodynamic-limit CO2-to-CH4 conversion

Nano Energy, Journal Year: 2025, Volume and Issue: unknown, P. 110650 - 110650

Published: Jan. 1, 2025

Language: Английский

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Balancing the Aggregation of Cobalt Phthalocyanine on Carbon Nanohorn for Efficient H₂O₂ electrosynthesis in Neutral Electrolyte

ChemElectroChem, Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 7, 2025

Abstract Oxygen reduction reaction (ORR) driven by renewable electricity in neutral electrolyte presents a promising way for generating H 2 O , which is suitable daily sanitation and hygiene management. Cobalt phthalocyanine (CoPc) serves as an effective molecular electrocatalyst, providing active sites to facilitate generation during ORR through uniform distribution on carbon supports. However, the catalytic performance currently falls short of industrial application requirements. Herein, we employed nanohorns with abundant oxygen functional groups (CNH(O)) support CoPc, thereby optimizing CoPc enhancing electron‐deficient Co centres. Control experiments characterizations demonstrate centres dependent degree aggregation, highlighting trade‐off between loading weight CoPc. Then, 4% CNH(O) exhibited optimal generation, achieving current density 483 mA cm −2 at potential 0.3 V vs RHE Faradaic efficiency 64 %.

Language: Английский

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Sub-Nano Gaδ+ clusters confined by porous carbon spheres and coupled with SnS2 for efficient photocatalytic extraction of uranium

Separation and Purification Technology, Journal Year: 2025, Volume and Issue: unknown, P. 132195 - 132195

Published: Feb. 1, 2025

Language: Английский

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Co–Fe–Mo Phosphides’ Triphasic Heterostructure Loaded on Nitrogen-Doped Carbon Nanofibers by Electrospinning as Efficient Bifunctional Electrocatalysts for Overall Water Splitting

ACS Applied Materials & Interfaces, Journal Year: 2025, Volume and Issue: unknown

Published: March 3, 2025

The rational design of efficient and stable bifunctional electrocatalysts for the hydrogen evolution reactions (HER) oxygen (OER) poses a significant challenge in realizing environmentally friendly production through electrocatalytic water splitting. construction heterostructure catalysts, coexisting multiple components, represents favorable approach increasing active sites, modulating electronic structure, accelerating charge transfer, decreasing reaction energy barriers, synergistically enhancing performance. In this study, triphasic metal phosphides' among CoP, FeP, MoP4 loaded on nitrogen-doped carbon nanofibers (labeled as CoP-FeP-MoP4@NC) was successfully synthesized electrospinning other subsequent steps electrocatalyst material Benefiting from strong interaction synergistic effect these CoP-FeP-MoP4@NC exhibits facile kinetics high activity under alkaline conditions with overpotentials (η) 222 75 mV at current density 10 mA cm-2 OER HER, respectively, well low cell voltage 1.47 V overall Moreover, catalyst shows great long-term stability about 100 cm-2. functional theory calculations revealed that CoP-FeP-MoP4 can reduce Gibbs free associated H2O dissociation adsorption during rate-determining step OER, increase states near Fermi level, optimize work function electrons, improving electrical conductivity capacity. This study presents an splitting, concept provides insights future advanced electrocatalysts.

Language: Английский

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