Efficient photocatalytic H2O2 production over K+-intercalated crystalline g-C3N4 with regulated oxygen reduction pathway

Chemical Engineering Journal, Journal Year: 2024, Volume and Issue: 482, P. 148844 - 148844

Published: Jan. 21, 2024

Language: Английский

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Unveiling the Dynamic Evolution of Single-Atom Co Sites in Covalent Triazine Frameworks for Enhanced H₂O₂ Photosynthesis

ACS Catalysis, Journal Year: 2024, Volume and Issue: 14(5), P. 2847 - 2858

Published: Feb. 8, 2024

Unraveling the structural evolution and mechanism of active sites in single-atom catalysts (SACs) during H2O2 production under operational conditions remains challenging due to transient elusive nature underlying reaction processes. Herein, we employ operando X-ray absorption spectroscopy ab initio molecular dynamics simulations unveil dynamic reconstruction behavior Co single atom-loaded covalent triazine framework (CoSA/Py-CTF) photocatalytic production. The unique Py-CTF substrate provides reasonable flexibility atom site. Under light irradiation O2 adsorption, atoms are dynamically released from then form atom-pairs with neighboring atoms, serving as authentic shuttling subnanometer domains between single-atoms facilitates transition adsorption configurations Pauling type Yeager type, resulting a record yield (2898.3 μmol·h–1·g–1). These findings provide insightful observations into photochemical SACs present an fresh paradigm for design intelligent "adaptive catalysts".

Language: Английский

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BiVO₄-Based Heterojunction Photocathode for High-Performance Photoelectrochemical Hydrogen Peroxide Production

Nano Letters, Journal Year: 2024, Volume and Issue: 24(20), P. 6051 - 6060

Published: April 29, 2024

Photoelectrochemical (PEC) cells provide a promising solution for the synthesis of hydrogen peroxide (H2O2). Herein, an integrated photocathode p-type BiVO4 (p-BVO) array with tetragonal zircon structure coupled different metal oxide (MOx, M = Sn, Ti, Ni, and Zn) heterostructure NiNC cocatalyst (p-BVO/MOx/NiNC) was synthesized PEC oxygen reduction reaction (ORR) in production H2O2. The p-BVO/SnO2/NiNC achieves rate 65.46 μmol L–1 h–1 H2O2 Faraday efficiency (FE) 76.12%. Combined generation water oxidation from n-type Mo-doped (n-Mo:BVO) photoanode, unbiased photoelectrochemical cell composed n-Mo:BVO photoanode total FE 97.67% generation. large area BiVO4-based tandem 3 × cm2 can reach yield 338.84 L–1. This work paves way rational design fabrication artificial photosynthetic liquid solar fuel.

Language: Английский

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Insights into excitonic behavior in single-atom covalent organic frameworks for efficient photo-Fenton-like pollutant degradation

Nature Communications, Journal Year: 2025, Volume and Issue: 16(1)

Published: Jan. 17, 2025

The generation of radicals through photo-Fenton-like reactions demonstrates significant potential for remediating emerging organic contaminants (EOCs) in complex aqueous environments. However, the excitonic effect, induced by Coulomb interactions between photoexcited electrons and holes, reduces carrier utilization efficiency these systems. In this study, we develop Cu single-atom-loaded covalent frameworks (CuSA/COFs) as models to modulate effects. Temperature-dependent photoluminescence ultrafast transient absorption spectra reveal that incorporating acenaphthene units into linker (CuSA/Ace-COF) significantly exciton binding energy (Eb). This modification not only enhances peroxymonosulfate adsorption at active sites but also facilitates rapid electron transfer promotes selective hydroxyl radical generation. Compared CuSA/Obq-COF (Eb = 25.6 meV), CuSA/Ace-COF 12.2 meV) shows a 39.5-fold increase pseudo-first-order rate constant sulfamethoxazole degradation (0.434 min-1). work provides insights modulating behavior single-atom catalysts via engineering EOCs degradation.

Language: 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, Journal Year: 2023, Volume and Issue: 344, P. 123629 - 123629

Published: Dec. 16, 2023

Language: Английский

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An efficient photo-Fenton In2O3@FeIn2S4 composite catalyst for tetracycline degradation

Chemical Engineering Journal, Journal Year: 2024, Volume and Issue: 491, P. 151549 - 151549

Published: April 22, 2024

Language: Английский

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Polymer photocatalysts for photocatalytic hydrogen peroxide production

Green Chemistry, Journal Year: 2024, Volume and Issue: 26(11), P. 6382 - 6403

Published: Jan. 1, 2024

Hydrogen peroxide (H 2 O ), as a mild oxidant and promising liquid fuel, has widespread application potential in energy environment fields.

Language: Английский

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Photocatalytic hydrogen peroxide production: Advances, mechanistic insights, and emerging challenges

Journal of environmental chemical engineering, Journal Year: 2024, Volume and Issue: 12(5), P. 114143 - 114143

Published: Sept. 16, 2024

Language: Английский

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Transformable Tumor Microenvironment‐Responsive Oxygen Vacancy‐Rich MnO₂@Hydroxyapatite Nanospheres for Highly Efficient Cancer Sonodynamic Immunotherapy

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

Published: Feb. 17, 2025

Despite the promise of sonodynamic therapy (SDT)-mediated immunotherapy, anticancer efficacy current sonosensitizers is greatly limited by immunosuppressive tumor microenvironment (TME) and their inability to selectively respond it. Herein, oxygen vacancy-rich MnO2@hydroxyapatite (Ca10(PO4)6(OH)2) core-shell nanospheres (denoted as Ov-MO@CPO) an advanced TME-responsive sonosensitizer for immunotherapy demonstrated. The Ov-MO@CPO maintains its structural integrity under neutral conditions but dissolves pH-sensitive hydroxyapatite shell acidic TME release active MnO2 core, which reinvigorates H2O2 consumption hypoxia alleviation due catalase-like activity. Furthermore, introduced vacancies optimize electronic structure Ov-MO@CPO, with states near Fermi level higher d-band center. It results in accelerated electron-hole pair separation lower catalytic energy barriers boost ultrasound (US)-initiated ROS production. These multimodal synergistic effects effectively reverse microenvironment, inhibiting growth metastasis 4T1 tumor-bearing mice. No evident toxic are observed normal mouse tissues. Additionally, when combined immune checkpoint inhibitor, Ov-MO@CPO-mediated SDT further improves effectiveness immunotherapy. This work affords a new avenue developing TME-dependent SDT-mediated

Language: Английский

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Singlet‐Oxygen‐Driven Cooperative Photocatalytic Coupling of Biomass Valorization and Hydrogen Peroxide Production Using Covalent Organic Frameworks

Angewandte Chemie, Journal Year: 2025, Volume and Issue: unknown

Published: March 11, 2025

Abstract Traditional H 2 O photocatalysis primarily depends on photoexcited electrons and holes to drive oxygen reduction water oxidation, respectively. However, singlet ( 1 ), often underappreciated, plays a pivotal role in production. Meanwhile, photocatalytic biomass conversion has attracted attention, yet studies combining synthesis with valorization remain rare typically yield low‐value products. Herein, strategy of furfuryl alcohol (FFA) coupled the efficient co‐production is reported, enabled by covalent organic frameworks (COFs) induced, ‐participated Achmatowicz rearrangement. This study introduces polyimide‐based COF‐N 0‐3 tailored nitrogen content, representing an unprecedently platform for Remarkably, reducing content COF enhances production, significantly boosting generation rate. In FFA, primary pathway production rearrangement, achieving rate ten times higher than that reliant reaction pure water, reaching 4549 µmol g⁻¹ h⁻¹. Mechanism revealed selectively engaged bypassing hole oxidation trigger producing valuable 6‐hydroxy‐(2H)‐pyranone 99% 92% selectivity. work establishes coupling simultaneous biochemicals, offering transformative approach sustainable photocatalysis.

Language: Английский

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