Electronic Metal‐Support Interactions Boost *OOH Intermediate Generation in Cu/In₂Se₃ for Electrochemical H₂O₂ Production

Angewandte Chemie International Edition, Год журнала: 2024, Номер 63(23)

Опубликована: Апрель 3, 2024

Abstract Two‐electron oxygen reduction reaction (2e − ORR) is a promising method for the synthesis of hydrogen peroxide (H 2 O ). However, high energy barriers generation key *OOH intermediates hinder process 2e ORR. Herein, we prepared copper‐supported indium selenide catalyst (Cu/In Se 3 ) to enhance selectivity and yield ORR by employing an electronic metal–support interactions (EMSIs) strategy. EMSIs‐induced charge rearrangement between metallic Cu In conducive intermediate generation, promoting H production. Theoretical investigations reveal that inclusion significantly lowers barrier impedes 4e pathway, thus favoring formation . The concentration produced Cu/In ~2 times than , shows applications in antibiotic degradation. This research presents valuable approach future utilization EMSIs

Язык: Английский

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Enhanced Charge Transfer via Heterogeneous Doping Promotes Hematite Photoelectrodes for Efficient Solar H₂O₂ Synthesis

ACS Catalysis, Год журнала: 2024, Номер 14(7), С. 4369 - 4378

Опубликована: Март 7, 2024

Photoelectrochemical (PEC) water splitting into hydrogen peroxide (H2O2) and (H2) is a promising alternative to energy environmentally intensive production. Bulk electronic surface structures affect the charge transport efficiency catalytic activity of photoelectrode. Herein, we design investigate hematite (Fe2O3) nanorod photoelectrode with hafnium titanium binary dopants for highly selective H2O2 The resultant photoanode shows yield 0.41 μmol min–1 cm–2 at 1.5 VRHE Faradaic 72.2%. Experimental investigations theoretical calculations demonstrate synergistic effect Hf gradient Ti doping on performance. effectively improves crystallinity Fe2O3, which favors improving reducing recombination. Gradient inhibits collapse structure, increases specific area, introduces large number active sites surface. Ti- Hf-codoped Ti/Hf:Fe2O3 kinetics generation, leading high selectivity production suppression O2 This work provides importance hematite-based photoanodes toward regulation competition reactions

Язык: Английский

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Polydopamine-Loaded ZnIn₂S₄ Photocatalyst for H₂O₂ Production in Water

ACS Applied Nano Materials, Год журнала: 2024, Номер 7(4), С. 4481 - 4490

Опубликована: Фев. 15, 2024

Reasonably utilizing solar energy to synthesize hydrogen peroxide (H2O2) from oxygen and water is a promising sustainable solution. In this work, we constructed an S-scheme photocatalyst ZnIn2S4/PDA (ZIS/PDA) by loading polydopamine (PDA) on the surface of ZnIn2S4, which significantly enhanced separation transfer photogenerated charge carriers while retaining excellent oxidation reduction abilities exhibited outstanding H2O2 production performance (1747 μmol·g–1·h–1) under visible light in pure water, 39 times yield ZnIn2S4. The presence PDA coating adsorption capacity catalysts for improved selectivity direct two-electron reaction (2e–ORR) formation rate effectively reducing Gibbs free (ΔG) *OOH. addition, ZIS/PDA inhibited decomposition promoting rapid desorption H2O2, conducive stable accumulation H2O2. summary, innovative demonstrates remarkable efficiency production, offering potential solution synthesis.

Язык: Английский

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Structurally Locked High-Crystalline Covalent Triazine Frameworks Enable Remarkable Overall Photosynthesis of Hydrogen Peroxide

Journal of the American Chemical Society, Год журнала: 2024, Номер 146(43), С. 29943 - 29954

Опубликована: Окт. 17, 2024

The development of green and efficient hydrogen peroxide (H

Язык: Английский

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Enhancing photocatalytic hydrogen peroxide generation by tuning hydrazone linkage density in covalent organic frameworks

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

Опубликована: Янв. 8, 2025

The conversion of solar energy into chemical or high-value chemicals has attracted considerable research interest in the context global crisis. Hydrogen peroxide (H2O2) is a versatile and powerful oxidizing agent widely used synthesis medical disinfection. H2O2 also serves as clean source fuel cells, generating electricity with zero-carbon emissions. Recently, sustainable production from water oxygen using covalent organic frameworks (COFs) photocatalysts attention; however, systematic studies highlighting role linkages determining photocatalytic performance are scarce. Under these circumstances, herein, we demonstrate that varying imine hydrazone within framework significantly influences production. COFs high-density linkages, providing optimal docking sites for oxygen, enhance generation activity (1588 μmol g−1 h−1 pure air), leading to highly efficient solar-to-chemical conversion. This work systematically investigates effect linkage density on enhancement hydrogen generation, aim achieving high-performance photocatalysis.

Язык: Английский

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Synergistic Utilization of Photogenerated Electrons and Holes in Carbon Nitride Nanosheet Assembly for Enhanced Photocatalytic H2O2 Production

Applied Catalysis B Environment and Energy, Год журнала: 2025, Номер unknown, С. 124998 - 124998

Опубликована: Янв. 1, 2025

Язык: Английский

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Efficient dual-pathway H2O2 production promoted by covalent triazine frameworks with integrated dual active sites

Applied Catalysis B Environment and Energy, Год журнала: 2023, Номер 344, С. 123629 - 123629

Опубликована: Дек. 16, 2023

Язык: Английский

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Recent Progress on the Catalysts and Device Designs for (Photo)Electrochemical On‐Site H₂O₂ Production

Advanced Energy Materials, Год журнала: 2023, Номер 13(39)

Опубликована: Сен. 4, 2023

Abstract Low‐cost and on‐site H 2 O production is desirable for industrial civilian usage. (Photo)electrochemical proposed to be a safer, greener, cheaper strategy as compared the conventional anthraquinone process direct thermal synthesis. However, efficiency, selectivity, durability of (photo)electrochemical devices are still not satisfactory. Therefore, there an urgent need revisit (photo)electrocatalyst device designs production, thus rationalize research thoughts provide valuable guidance. This review comprehensively summarizes discusses mechanism two‐electron oxygen reduction reaction (2e − ORR) water oxidation WOR) current status on (photo)electrocatalysts devices. In particular, pros cons four types designs, which Type I ORR + evolution reaction), II hydrogen III WOR reaction) IV 2e ORR), discussed in detail. Finally, practical perspective future directions based technical challenges this technique provided.

Язык: Английский

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Carboxylated Hexagonal Boron Nitride/Graphene Configuration for Electrosynthesis of High‐Concentration Neutral Hydrogen Peroxide

Angewandte Chemie International Edition, Год журнала: 2023, Номер 63(7)

Опубликована: Дек. 30, 2023

Abstract The electrosynthesis of hydrogen peroxide (H 2 O ) via two‐electron (2 e − oxygen (O reduction reaction (ORR) has great potential to replace the traditional energy‐intensive anthraquinone process, but design low‐cost and highly active selective catalysts is greatly challenging for long‐term H production under industrial relevant current density, especially neutral electrolytes. To address this issue, work constructed a carboxylated hexagonal boron nitride/graphene ( h ‐BN/G) heterojunction on commercial activated carbon through coupling B, N co‐doping with surface groups functionalization. champion catalyst exhibited high ORR selectivity (>95 %), rate (up 13.4 mol g −1 ), Faradaic efficiency (FE, >95 %). density 100 mA cm −2 caused cumulative concentration as 2.1 wt %. combination in situ Raman spectra theoretical calculation indicated that h‐ BN/G configuration promotes adsorption stabilization key intermediates, allowing low energy barrier rate‐determining step HOOH* release from site thus improving performance. fast dye degradation by using electrochemical synthesized further illustrated promising practical application.

Язык: Английский

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Hollow Spherical Heterostructured FeCo‐P Catalysts Derived from MOF‐74 for Efficient Overall Water Splitting

Advanced Science, Год журнала: 2023, Номер 11(2)

Опубликована: Ноя. 20, 2023

Abstract The design of catalysts with tunable active sites in heterogeneous interface structures is crucial for addressing challenges the water‐splitting process. Herein, a hollow spherical heterostructure FeCo‐P successfully prepared by hydrothermal and phosphorization methods. This structure, along between Co 2 P FeP, not only facilitates exposure more sites, but also increases contact area catalyst electrolyte, as well shortens distance mass/electron transfer. enhancement promotes electron transfer to facilitate water decomposition. exhibits excellent hydrogen evolution (HER) oxygen (OER) performance when reaching @ 10 mA cm −2 1 mol L −1 KOH, overpotentials 131/240 mV HER/OER. Furthermore, used both cathode anode overall splitting (OWS), it requires low voltages 1.49, 1.55, 1.57 V achieve CDs 10, 100, 300 , respectively. Density functional theory calculations indicate that constructing FeP good lattice matching can redistribution, thereby enhancing electrocatalytic OWS. work opens up new possibilities rational efficient electrolysis derived from MOFs.

Язык: Английский

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