Regulating the Local Reaction Microenvironment at Chromium Metal–Organic Frameworks for Efficient H₂O₂ Electrosynthesis in Neutral Electrolytes

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

Published: March 30, 2025

Abstract The electrochemical synthesis of hydrogen peroxide represents a promising alternative to the traditional anthraquinone process, aiming for zero pollution. However, achieving efficient in neutral electrolytes is challenging due sluggish kinetics two‐electron oxygen reduction reaction. To address this issue, unique metal–organic framework (MOF) featuring Cr metal sites coordinated with tetrabromoterephthalic acid (Cr‐TBA) synthesized. This specially designed MOF exhibits distinctive paper‐clip‐like structure and remarkably enhanced Lewis acidity. Experimental results demonstrate that obtained can facilitate attraction OH − ions solution, promoting their accumulation on catalyst surface. enhancement leads excellent performances Cr‐TBA electrolytes, Faradaic efficiencies 96–98% production rate 13.4 mol g cat −1 h at current density 150 mA cm −2 . Operando spectroscopy functional theory calculations indicate modified microenvironment effectively facilitates conversion * OOH intermediates H 2 O

Language: Английский

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Industrial‐Level H₂O₂ Electrosynthesis via Defect‐Induced Strain in Laser‐Fabricated Nickel‐Carbon Catalysts and Gas‐Diffusion Electrodes

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

Published: April 25, 2025

Abstract Industrial‐level hydrogen peroxide (H 2 O ) electrosynthesis is a promising alternative for the energy‐intensive anthraquinone process. However, during repeated H synthesis under harsh electrochemical conditions, active species could be leached away, undergo compositional segregation, or suffer from reconstruction, resulting in loss catalytic activity and efficiency. Besides, typical powder‐form catalysts inevitably limit their performance enhancement, owing to large interface resistance peeling‐off of powder electrodes. Addressing these, fine nickel particle catalyst that with high‐density defects embedded thin carbon substrates, via rapid ultraviolet laser treatment, reported. The (i.e., twin boundaries, vacancies, dislocations) Ni particles induce subtle strong strain, which optimizes electrocatalytic prevents deactivation effectively. By fabricating into free‐standing form, electronic conductivity durability electrode can significantly improved, therefore achieving stable production at an industrial‐level current density 250 mA cm −2 over 100 h Faradaic Efficiency 90% high yield 4.27 mmol −1 . These results provide pathway industrial large‐scale electrosynthesis, highlight potential application electro‐synthesized , such as dye degradation.

Language: Английский

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Approaching efficient H2O2 electrosynthesis on ZnO nanorod via a combined strategy of crystal facet-engineering and surface amorphization

Journal of Colloid and Interface Science, Journal Year: 2025, Volume and Issue: unknown, P. 137718 - 137718

Published: April 1, 2025

Language: Английский

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Unique electronic regulation in bimetallic MOF for efficient electrochemical synthesis of H2O2 at 500 mA cm-2

Nano Energy, Journal Year: 2025, Volume and Issue: unknown, P. 111096 - 111096

Published: May 1, 2025

Language: Английский

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Efficient Neutral H2O2 Electrosynthesis from Favorable Reaction Microenvironments via Porous Carbon Carrier Engineering

Angewandte Chemie, Journal Year: 2024, Volume and Issue: 136(32)

Published: May 20, 2024

Abstract The efficient electrosynthesis of hydrogen peroxide (H 2 O ) via two‐electron oxygen reduction reaction (2e − ORR) in neutral media is undoubtedly a practical route, but the limited comprehension electrocatalysts has hindered system advancement. Herein, we present design model catalysts comprising mesoporous carbon spheres‐supported Pd nanoparticles for H at near‐zero overpotential with approximately 95 % selectivity electrolyte. Impressively, optimized Pd/MCS‐8 electrocatalyst flow cell device achieves an exceptional yield 15.77 mol g catalyst −1 h , generating solution accumulated concentration 6.43 wt %, level sufficiently high medical disinfection. Finite element simulation and experimental results suggest that carriers promote enrichment localized pH elevation, establishing favorable microenvironment 2e ORR media. Density functional theory calculations reveal robust interaction between adsorption OOH* edge, ensuring active process. These findings offer new insights into carbon‐loaded media, emphasizing role carrier engineering constructing microenvironments synergizing sites.

Language: Английский

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