Utilization of Stable and Efficient High‐Entropy (Ni_0.2Zn_0.2Mg_0.2Cu_0.2Co_0.2)Al₂O₄ Catalyst with Polyvalent Transition Metals to Boost Peroxymonosulfate Activation toward Pollutant Degradation

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

Published: Jan. 23, 2025

Abstract A polyacrylamide gel method has been used to synthesize a variety of polyvalent‐transition‐metal‐doped Ni position high entropy spinel oxides (Ni 0.2 Zn Mg Cu Co )Al 2 O 4 ‐800 °C (A ) on the basis NiAl , and catalytic activity is studied under synergistic action peroxymonosulfate (PMS) activation simulated sunlight. The containing polyvalent transition metals 2+ can effectively activate PMS efficiently degrade levofloxacin (LEV) tetracycline hydrochloride (TCH) sunlight irradiation. After 90 min light exposure, degradation percentages LEV (50 mg L −1 TCH (100 by /PMS/vis system reach 87.0% 90.2%, respectively. superoxide radicals, photoinduced holes, singlet dominate process, while hydroxyl radicals sulfate play only small role. adsorption energy charge density difference between different systems are calculated functional theory, efficiency combining with change length O─O bond after adsorption. mechanism proposed, which provides new idea for study in field catalysis.

Language: Английский

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Gold-Modified Covalent Organic Frameworks-Assisted Laser Desorption/Ionization Mass Spectrometry for Analysis of Metabolites Induced by Triclosan Exposure

ACS Applied Materials & Interfaces, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 17, 2025

Matrix-assisted laser desorption/ionization (MALDI) mass spectrometry (MS) holds great promise for the rapid and sensitive detection of biomolecules, but its precise small molecule metabolites is hindered by severe background interference from organic matrix in low molecular weight range. To address this issue, nanomaterials have commonly been utilized as substrates LDI-MS. Among them, covalent frameworks (COFs), known their unique optical absorption structural properties, garnered significant attention. Despite these advantages, ionization efficiency remains a challenge. Herein, composite material COF-S@Au nanoparticles (NPs), incorporating Au NPs into sulfur-functionalized COF (COF-S) through postsynthetic modification, was designed adopted substrates. This hybrid leverages synergistic effects COF-S to improve minimize interference. The demonstrated 5-16-fold improvement MS signals biomolecules along with clean excellent resistance salt protein Their corresponding limits (LODs) were achieved at ∼pmol. Furthermore, applied analyze triclosan (TCS)-exposed mouse model, successfully identifying 10 differential associated TCS toxicity. work provides foundation developing advanced LDI-MS materials high-performance metabolic analysis offers valuable insights toxicity potential applications environmental toxicology.

Language: Английский

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Linkage Microenvironment Modulation in Triazine‐Based Covalent Organic Frameworks for Enhanced Photocatalytic Hydrogen Peroxide Production

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

Published: Jan. 26, 2025

Abstract Covalent organic frameworks (COFs), known for the precise tunability of molecular structures, hold significant promise photocatalytic hydrogen peroxide (H 2 O ) production. Herein, by systematically altering quinoline (QN) linkages in triazine (TA)‐based COFs via multi‐component reactions, six R‐QN‐TA‐COFs are synthesized with identical skeletons but different substituents. The fine‐tuning optoelectronic properties and local microenvironment is allowed, thereby optimizing charge separation improving interactions dissolved oxygen. Consequently, MeO‐QN‐TA‐COF customized to achieve an impressive rate H production up 7384 µmol g⁻ 1 h⁻ under air atmosphere water without any sacrificial agents, surpassing most reported COF photocatalysts. Its high stability demonstrated through five consecutive recycling experiments characterization recovered COF. reaction mechanism further investigated using a suite quenching experiments, situ spectroscopic analysis, theoretical calculations. enhanced over 2e⁻ oxygen reduction oxidation pathways. Overall, crucial role linkage modulation design solar‐driven effective

Language: Английский

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A Covalent Organic Framework as Photocatalyst for Smart Conversion Between Photooxidation and Photoreduction and H₂O₂ Production in Full pH Environment

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

Published: Feb. 7, 2025

Abstract Developing multifunctional photocatalysts with intelligent self‐adjusting is of great significance in the photocatalytic process. Herein, a smart covalent organic framework (Por‐HQ‐COF) phenol‐quinone conversion structure pH changes constructed for photooxidation, photoreduction, and H 2 O production. As photocatalyst, Por‐HQ‐COF can convert into Por‐BQ‐COF intelligently trigger including solution pH, vice versa. The reconstruction not only significantly alters morphologies specific surface areas COF, but also leads to an entirely change band energy charge distribution influence photoelectric properties. result, under acidic conditions, converts automatically photoreduce high concentration Cr(VI) Cr(III) efficiently. Under neutral superoxide anions (·O − ) initiate accelerate photooxidation degrade high‐concentration TC. alkaline Por‐BQ‐COF, effectively photosynthesize (1525 µmol h −1 g at λ > 420 nm) absence any sacrificial reagents, reveal strong alkalinity lower barrier hydrogen extraction from clarify active sites This work provides new strategy developing fulfill application across full environment.

Language: Английский

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Dual‐Functional Benzotrithiophene‐Based Covalent Organic Frameworks for Photocatalytic Detoxification of Mustard Gas Simulants and Antibacterial Defense

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

Published: Feb. 17, 2025

Abstract The persistent threats posed by toxic chemical warfare agents (CWAs) such as mustard gas (bis(2‐chloroethyl) sulfide, HD) and bacterial contaminants demand the development of innovative, sustainable mitigation strategies. Photocatalytic processes that generate reactive oxygen species (ROS) offer a promising dual‐functional approach for both detoxification antibacterial defense. In this study, two structurally analogous covalent organic frameworks (COFs), BPY‐COF BD‐COF, are synthesized using benzotrithiophene donor unit paired with bipyridine biphenyl, respectively. These COFs exhibit high crystallinity, broad‐spectrum light absorption, efficient charge carrier transport, demonstrating superior performance due to incorporation heteroatoms. achieved ultrafast simulant 2‐chloroethyl ethyl sulfide (CEES) half‐life 35 min 100% selectivity sulfoxide (CEESO) under white LED light, outperforming BD‐COF. Additionally, electrospun composite fibers containing 40 wt.% maintained comparable CEES degradation rates exhibited over 99% efficiency against Escherichia coli Bacillus subtilis within 60 min. findings highlight potential multifunctional photocatalyst integrated applications in defense, addressing critical challenges public health safety.

Language: Английский

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Functionalized Modification of Conjugated Porous Polymers for Full Reaction Photosynthesis of H₂O₂

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: unknown

Published: Oct. 16, 2024

Abstract Modulating the molecular structure to achieve full reaction including oxygen reduction and water oxidation is a promising strategy for efficient photosynthesis of hydrogen peroxide (H 2 O ) but remains challenge. Herein, triphenylamine naphthalimide‐based conjugated porous polymers are synthesized with photo oxidation‐reduction structures, then sulfonate (─SO 3 H) quaternary ammonium groups introduced via post‐modification produce two photocatalysts named NI‐TPA‐NI‐SO H NI‐TPA‐NI‐N, respectively. Introducing charged functional has improved hydrophilicity (O adsorption, beyond that, ─SO further stabilizes adsorbed bonding as well accelerates photogenerated carrier separation electron/proton transport that enables . Therefore, motivated by charge separation, stabilized boosted proton‐coupled electron transfer, exhibits highest light‐driven production rate among three photocatalysts, reaching 3.40 mmol g −1 h , which 4.9‐fold NI‐TPA‐NI. Remarkably, in presence ethylenediaminetetraacetic acid disodium salt, its significantly enhances 14.5 superior most reported organic best knowledge.

Language: Английский

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Thiazolo[5,4-d]thiazole-Based Covalent Organic Frameworks for the Rapid Removal of RhB

Catalysts, Journal Year: 2025, Volume and Issue: 15(1), P. 42 - 42

Published: Jan. 5, 2025

Two thiazolo[5,4-d]thiazole(TzTz)-based donor(D)-acceptor(A) COFs (TPTZ-COF and TBTZ-COF) are synthesized for the photocatalytic degradation of RhB in water. The D-A structure with weak deficient electron TzTz as an acceptor promotes separation photo-generated charge carriers. rigid can enhance π–π dipole–dipole interactions, which improve mobility carriers result enhancement performance COFs. Optical electrical tests show that TBTZ-COF has more efficient electron–hole transfer degrades 99.76% (10 mg/L) 60 min under visible light irradiation, while hydroxyl groups on TPTZ-COF surface enable formation a large number hydrogen bonds RhB, so exhibits excellent adsorption ability RhB. Furthermore, maintains high activity after five consecutive cycles, making it promising photocatalyst rapid removal

Language: Английский

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Flower-like spherical g-C3N4/Ag/BaTiO3 nanocomposites for enhanced photocatalytic in nitrogen fixation and tetracycline degradation

Journal of Alloys and Compounds, Journal Year: 2025, Volume and Issue: 1016, P. 178968 - 178968

Published: Feb. 1, 2025

Language: Английский

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Thiadiazole/Triazole-Based Covalent Organic Frameworks for Efficient Photocatalytic Reduction of U(Vi): Isomeric Effect and Delocalization Degree

Published: Jan. 1, 2025

Language: Английский

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Enhanced built-in electric fields in alkali metal-doped C3N5 enable sustainable molecular oxygen activation for water purification

Chemical Engineering Journal, Journal Year: 2025, Volume and Issue: unknown, P. 161236 - 161236

Published: March 1, 2025

Language: Английский

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