Synthesis of H2O2 and high-value chemicals by covalent organic framework-based photocatalysts

CHINESE JOURNAL OF CATALYSIS (CHINESE VERSION), Journal Year: 2024, Volume and Issue: 61, P. 97 - 110

Published: June 1, 2024

Language: Английский

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Atomically Dispersed Iron Active Sites on Covalent Organic Frameworks for Artificial Photosynthesis of Hydrogen Peroxide

Advanced Energy Materials, Journal Year: 2024, Volume and Issue: 14(7)

Published: Jan. 11, 2024

Abstract Artificial photosynthesis has been regarded as a promising solution toward solar energy conversion, generating storable and transportable chemical fuels such hydrogen (H 2 ) peroxide O ). However, the design of robust catalytic sites not only affects activity, but also identify atomic‐level correlation between active natural performance. Herein, synthesis method single‐atomic Iron (Fe) anchored on novel covalent organic framework (COF) for production H under visible light irradiation. When benzyl alcohol is most sacrificial agent, state‐of‐the‐art Fe‐based COF exhibits an excellent generation rate 4130 µmol g −1 h , over 5.3 times higher than that pristine COF, achieving apparent quantum yield 6.4% at 420 nm. The enhanced photocatalytic performance ascribed to synergistic effect atomically dispersed Fe hosts, reducing reaction barrier formation * OOH intermediates optimizing adsorption thus promoting two‐electron oxygen reduction (ORR). This work establishes engineering approach build photocatalysts provides in‐depth insight upon ORR mechanism artificial .

Language: Английский

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Hydroxyl‐Bonded Co Single Atom Site on Boroncarbonitride Surface Realizes Nonsacrificial H₂O₂ Synthesis in the Near‐Infrared Region

Advanced Materials, Journal Year: 2024, Volume and Issue: 36(30)

Published: May 14, 2024

Photocatalytic synthesis of hydrogen peroxide (H

Language: Английский

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Carbon dots bridged Zn0.5Cd0.5S with interfacial amide bond facilitating electron transfer for efficient photocatalytic hydrogen peroxide production

Applied Catalysis B Environment and Energy, Journal Year: 2024, Volume and Issue: 346, P. 123721 - 123721

Published: Jan. 10, 2024

Language: Английский

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The evolution of photocatalytic H₂O₂ generation: from pure water to natural systems and beyond

Energy & Environmental Science, Journal Year: 2024, Volume and Issue: 17(18), P. 6482 - 6498

Published: Jan. 1, 2024

Exploring advancements in photocatalytic hydrogen peroxide production, emphasizing technological breakthroughs pure water, natural microdroplets and coupling systems.

Language: Английский

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Enhancing Photosynthesis Efficiency of Hydrogen Peroxide by Modulating Side Chains to Facilitate Water Oxidation at Low‐Energy Barrier Sites

Advanced Materials, Journal Year: 2024, Volume and Issue: 36(18)

Published: Jan. 27, 2024

Abstract Hydrogen peroxide (H 2 O ) is a crucial oxidant in advanced oxidation processes. In situ, photosynthesis of it natural water holds the promise practical application for remediation. However, current H systems primarily relies on oxygen reduction, leading to limited performance with low dissolved or anaerobic conditions found polluted water. Herein, novel photocatalyst based conjugated polymers alternating electron donor–acceptor structures and electron‐withdrawing side chains donors introduced. Specifically, carbazole functions as donor, triazine serves acceptor, cyano acts chain. Notably, exhibits remarkable solar‐to‐chemical conversion 0.64%, highest reported Furthermore, even conditions, achieves an impressive photosynthetic efficiency 1365 µmol g −1 h , surpassing all . This improvement attributed effective relocation active site from high‐energy low‐energy acetylene mediated by chains, resulting enhanced generation breakthrough offers new avenue efficient remediation using technologies oxygen‐limited environments, holding significant implications environmental restoration.

Language: Английский

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One‐Pot Synthesis of Fully Conjugated Covalent Organic Frameworks via the Pictet–Spengler Reaction for Boosting H₂O₂ Photogeneration in Real Seawater

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

Published: Jan. 24, 2025

Abstract Photosynthesizing H 2 O from real seawater is a promising and green avenue but suffers salt‐deactivated effects with limitations on stability photocatalytic activity. Herein, by the Pictet–Spengler reaction, two fully conjugated thieno[3,2‐c]pyridine‐linked covalent organic frameworks (named TBA‐COF TCA‐COF) are synthesized for photoproduction first time. Without sacrificial agents in , TCA‐COF exhibit impressive generation rates of 8878 6023 µmol g −1 h solar‐to‐chemical conversion efficiency 0.62% 0.42%, respectively, superior to their Schiff base analogs. Further experimental theoretical investigations reveal that, compared imine‐linkage counterparts, one‐pot cyclized TCA‐COF, reaction improves charge carrier separation efficiency, alters photoreduction center triazine benzene parts pyridine units, modulates energy band structures drive 2e − oxygen reduction water oxidation thereby enhances photosynthetic Notably, seawater‐produced flow reactors packed can be directly utilized E. coli sterilization. The present study highlights construction robust COFs thieno[3,2‐c]pyridine linkage via sustainable producing seawater.

Language: Английский

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Enhanced Three-Component Chloro-/Azido-Fluoroalkylation of Unactivated Alkenes via the Proximity Effect in a Heterogenous Metallaphotocatalyst

ACS Catalysis, Journal Year: 2025, Volume and Issue: 15(3), P. 2180 - 2191

Published: Jan. 22, 2025

Heterogeneous metallaphotocatalytic chemical transformations employing a recyclable catalyst are highly desirable for organic synthesis. However, the rational design and controlled preparation of well-defined, site-isolated metal/photo bifunctional heterogeneous catalysts to achieve this goal remain significant challenge. In study, we demonstrate covalent attachment homogeneous molecular MnSalen complex (where Salen = N,N′-bis(salicylidene)ethylenediamine) onto surface graphitic carbon nitride (CN) via an amide bond visible-light-driven chloro- azido-fluoroalkylation unactivated alkenes. The linkage between CN not only facilitates electron delocalization enhances light-harvesting capabilities photosensitizer but also exerts proximity effect that markedly ability Mn sites capture alkyl radical intermediates during reaction process. A diverse set alkenes could be efficiently azido-fluoroalkylated their corresponding difunctionalized products in moderate high yields with good functional group compatibility. Furthermore, practicability protocol is illustrated through late-stage diversification various bioactive compounds pharmaceuticals. Notably, integrated photocatalyst demonstrates stability can recycled at least 10 times without loss activity selectivity.

Language: Английский

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Challenges and Prospects of Catalyst Design and Environmental Applications for On‐Site Hydrogen Peroxide Production via Diverse (Photo)Electrochemical Reaction Pathways

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

Published: Feb. 9, 2025

Hydrogen peroxide (H2O2) is an environmentally friendly and efficient oxidant with diverse applications in the chemical industry, medicine, energy, environmental protection. While anthraquinone oxidation process has traditionally dominated industrial H2O2 production, its complexity high pollution levels present significant challenges. In response, alternative methods such as electrochemical, photochemical, photoelectrochemical pathways have emerged, providing greener more sustainable solutions. These innovative approaches leverage only water, oxygen, solar or electrical positioning them viable substitutes for energy-intensive process. This review delves into latest advancements production through twoelectron oxygen reduction reaction (2e-ORR), water (2e-WOR), synergistic two-channel pathway (2e-ORR + 2e-WOR) (photo)electrochemical systems, focusing on pathways. It discusses underlying mechanisms, evaluation parameters, design of high-performance catalysts on-site applications. Recent developments advanced (photo)electrocatalysts over past five years are highlighted, including key strategies that enhance catalytic performance. The also addresses future challenges prospects catalyst practical systems serving a valuable reference researchers field.

Language: Английский

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Exploring the Roles of Single Atom in Hydrogen Peroxide Photosynthesis

Nano-Micro Letters, Journal Year: 2023, Volume and Issue: 16(1)

Published: Nov. 20, 2023

This comprehensive review provides a deep exploration of the unique roles single atom catalysts (SACs) in photocatalytic hydrogen peroxide (H

Language: Английский

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