Photothermal‐Catalyzed Hydrogen Peroxide Production Enabled by Gold‐Organic Frameworks

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

Published: Jan. 20, 2025

Abstract Gold catalysts are extensively utilized in photothermal processes that rely on localized surface plasmon resonance effects. However, the development of novel gold(I)‐organic frameworks function as highly efficient for production hydrogen peroxide from water and oxygen presents a fascinating challenging research opportunity. Herein, three gold(I) cyclic trinuclear complexes (Au‐CTCs) based metal–organic (MOFs) prepared, exhibiting good conversion efficiency H 2 O evolution rates. Utilizing optimized Au‐TFPT, rates H₂O₂ can reach high 51,987 µ m g⁻¹ h⁻¹, surpassing performance most reported (MOFs), even with use sacrificial agents to accelerate reaction. The thermal‐assisted photocatalytic mechanism is comprehensively studied by transient photocurrent response, electrochemical impedance, electron paramagnetic resonance, rotating ring disk electrode test, catalytic among others, demonstrating thermal energy enhance mobility photogenerated carriers apparent quantum yield, regulate reactive species ratio selectivity, reduce activation photocatalysis, improve mass transfer rates, thereby accelerating reaction process. This study offers new insights into .

Language: Английский

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Reprogram Local Electronic Configuration in Multicomponent Covalent–Organic Frameworks for Efficient Hydrogen Peroxide Photoproduction

Chemistry of Materials, Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 19, 2025

Covalent organic frameworks (COFs) have recently demonstrated significant potential for photocatalysis. Optimizing the local electronic environment in COFs has been considered to be critical enhancing photocatalytic activity. Here, we report a one-pot "grafting-to" strategy reprogram configurations of series isoreticular multicomponent by introducing electron-donating or electron-withdrawing groups into pores transform photoinert photoactive and form intramolecular donor–acceptor (D-A) structures. Such D-A structures enhanced overall hydrogen peroxide photoproduction facilitating charge carrier separation optimizing band achieve oxygen reduction reaction water oxidation simultaneously. Notably, one incorporated with 2-aminothiazole exhibits production rate 3701 μmol g–1 h–1 solar-to-chemical conversion efficiency 0.13% without use any sacrificial reagents, it 100% bacterial killing rates remarkable >90% biofilm removal capability. This COF modification strategy, which not reported before, offers unique approach constructing highly active photocatalysts containing great future design antibacterial therapies.

Language: Английский

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Synergistic Zn-Cd Bimetallic Engineering in ZIFs for High-Chloride 2e− ORR to H2O2 in Simulated Neutral Seawater

Materials, Journal Year: 2025, Volume and Issue: 18(8), P. 1786 - 1786

Published: April 14, 2025

Marine biofouling causes significant economic losses, and conventional antifouling methods are often associated with environmental pollution. Hydrogen peroxide (H2O2), as a clean energy source, has gained increasing attention in recent years. Meanwhile, electrocatalytic 2e− oxygen reduction reaction (ORR) for H2O2 production received growing interest. However, the majority of current studies conducted on acidic or alkaline electrolytes, research ORR neutral NaCl solutions remains rare. Here, bimetallic Zn-Cd zeolitic imidazolate framework (ZnCd-ZIF) is rationally designed to achieve chloride-resistant catalysis under simulated seawater conditions (pH 7.5, 3.5% Cl−). Experimental results demonstrate that ZnCd-ZIF catalyst exhibits an exceptional selectivity 70% at 0.3 VRHE, surpassing monometallic Zn-ZIF (60%) Cd-ZIF (50%). Notably, reaches 120 mmol g−1 Cl−-containing electrolyte, exhibiting strong resistance structural corrosion Cl− poisoning. This work not only pioneers effective strategy designing catalysts adapted marine environments but also advances practical implementation seawater-based electrochemical synthesis.

Language: Английский

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Porphyrin-Based Covalent Organic Framework Encapsulating Multiwalled Carbon Nanotubes: A High-Performance Electrocatalyst for Oxygen Reduction Reaction

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

Published: April 17, 2025

The development of efficient and cost-effective oxygen reduction reaction (ORR) catalysts is crucial for advancing fuel cell technologies, given the limitations platinum-based catalysts. Here, we present a novel nanocomposite, cobalt-based porphyrinic covalent organic framework wrapped on multiwalled carbon nanotubes (Co-pCOF@MWCNTs), synthesized via template-directed in situ polymerization. This composite combines high porosity tunable catalytic properties COFs with excellent electrical conductivity MWCNTs. Co-pCOF@MWCNT demonstrates superior ORR activity, exhibiting an onset potential (Eonset) 0.86 V vs RHE 0.1 M KOH, surpassing performance its individual components (Co-pCOF MWCNT) other related materials. enhanced efficiency attributed to synergistic interactions between conductive MWCNT scaffold active COF nanolayers, which facilitate charge transfer increase site exposure. Furthermore, nanocomposite exhibits stability methanol tolerance, establishing as cathodic material cells. work highlights promise integrating materials opens new avenues design advanced energy conversion applications.

Language: Английский

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A Dimolybdenum Paddlewheel Embedded Covalent Organic Framework for Photocatalytic Hydrogen Peroxide Generation

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

Published: May 24, 2025

Abstract In the midst of global energy crisis, conversion solar into chemical or high‐value chemicals has become critical. Hydrogen peroxide (H 2 O ), a versatile oxidizing agent, plays an important role in synthesis, medical disinfection, and clean generation via fuel cells. Recently, photocatalytic H from water oxygen using covalent organic frameworks (COFs) metal–organic (MOFs) emerged as sustainable approach. this context, novel dimolybdenum paddlewheel‐embedded COF (Mo‐DHTA COF) is presented synthesized for generation. It observed that Mo sites help to bind molecule, while high‐energy valence band electrons localized on α‐hydroquinone moiety facilitate efficient photoelectron transfer reduction. Simultaneously, reduced electron density above hydroxy groups conduction serves proton source during production. Due these synergistic effects, Mo‐DHTA exhibited production rate 626 µmol g −1 h aqueous ethanol 4084 benzyl alcohol, which found be higher than polymeric counterpart (Mo‐DHTA‐P). This innovative design highlights potential metal‐embedded crystalline porous COFs advanced applications.

Language: Английский

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