Deciphering the Origin of Higher Shell Coordination on Single Iron Catalysts for Resilient Modulating Persulfate Oxidation Into Singlet Oxygen Pathway

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

Published: Jan. 28, 2025

Abstract Precise manipulation of coordination structure single‐atom sites and establishment schematic microenvironment‐oxidation pathway relations remain significant challenges in Fenton‐like chemistry. Herein, incorporating sulfur heteroatoms into the higher shell FeN 4 (Fe‐NSC) exhibited a volcano trend p ‐hydroxybenzoic acid oxidation, aligning with number positions dopant. Specifically, S moderate electronegativity larger atomic radii triggers long‐range electronic interactions, which provoke Fe 3d orbital splitting spin electron rearrangement, resulting crossover states d xy 2 yz 1 xz z 21 . As result, partial filling e g t orbitals σ/π antibonding between 2p optimized adsorption–desorption behaviors key oxygenated intermediates from peroxymonosulfate activation. Thus, optimal binding configuration weakens Fe─O bonding accelerates PMS dissociation to yield C‐S‐N Fe‐O*, subsequently couples form O nearly 100% selectivity. The Fe‐NSC‐functionalized membrane outstanding long‐term reusability continuous flow reactor further validated practical application perspective. This study provides insight at both levels for rational design spin‐polarized catalysts its functions fine‐tuning oxidation pathways environmental catalysis.

Language: Английский

---

Engineering defects in heterogeneous catalytic persulfates for water purification: An overlooked role?

Coordination Chemistry Reviews, Journal Year: 2024, Volume and Issue: 507, P. 215749 - 215749

Published: March 8, 2024

Language: Английский

---

Remediation of characteristic contaminants in groundwater of chemical industrial by the activation of PMS: Recent developments and challenges-a mini-review

Chinese Chemical Letters, Journal Year: 2025, Volume and Issue: unknown, P. 111120 - 111120

Published: March 1, 2025

Language: Английский

---

Construction of surface micro-electric fields on common metal Fe/Mg co-doped g-C3N4 with surface acidification for synergistic activation of peroxymonosulfate

Chemical Engineering Journal, Journal Year: 2024, Volume and Issue: 496, P. 153950 - 153950

Published: July 14, 2024

Developing low-cost, sustainable catalysts is critical to meet the green-transition goal in water treatments. Herein, a common metal modified g-C3N4 material (FeMg-O-g-C3N4) was designed improve electron mobility and peroxymonosulfate (PMS) utilization. Likewise, surface acidification of has introduced extra porous structure, anchor sites for metals, activate sites. This new catalyst free expensive rare-earth metals creates numerous micro-electric fields through: 1) large difference electronegativity Fe (1.83) Mg (1.31); 2) cation-π effect formed between benzene-like ring structure g-C3N4; 3) added PMS pollutant (tetracycline (TC)) as provider promoting transfer electrons electron-rich Both non-radical (1O2) radical (surface-bound ·OH SO4·−) pathways contribute degradation. Given promising results stability catalyst, this study opens horizons apply over expensive, toxic rare PMS-based

Language: Английский

---

Unveiling the fundamental understanding of two dimensional π-conjugated FeN₄₊₄ sites for boosting peroxymonosulfate activation

Journal of Materials Chemistry A, Journal Year: 2024, Volume and Issue: 12(19), P. 11310 - 11321

Published: Jan. 1, 2024

The precisely defined FeN 4+4 active sites in fully π-conjugated polyphthalocyanine frameworks establish a dual-pump-driven electron fast shuttle path—electron-rich Fe centers and electron-poor C atoms—ensuring continuous production of 1 O 2 .

Language: Английский

---

Enhanced peroxymonosulfate activation for emerging contaminant degradation via defect-engineered interfacial electric field in FeNC

Journal of Colloid and Interface Science, Journal Year: 2024, Volume and Issue: 678, P. 713 - 721

Published: Aug. 28, 2024

Language: Английский

---

Photo‐Responsive Nanozyme Disrupts Bacterial Electron Transport Chain for Enhanced Anti‐Biofilm Therapy

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

Published: Dec. 23, 2024

Abstract The bacterial electron transport chain (ETC) plays a crucial role in biofilm energy metabolism and redox balance, making it potential target for anti‐biofilm treatment. Herein, mesoporous nanocarbon spheres loaded with Pt nanoparticles (CS‐Pt) are developed to disrupt the ETC photo‐enhanced anti‐biofilm. Under near‐infrared laser irradiation, CS‐Pt‐treated biofilms show positive shift of 0.6 eV 4f binding 1.76‐fold increase anodic current density, demonstrating that loss from CS‐Pt results an enhanced transfer biofilm. Adding quencher NH 4 Cl CS‐Pt‐containing sample reduced clearance, highlighting critical effective eradication. Due multifunction inducing hyperthermia, reactive oxgen species generation, interrupting ETC, component extracellular DNA, methicillin‐resistant Staphylococcus aureus (MRSA) is by 89.8%, ultimately leading clearance 90.3%. Additionally, achieve 99.5% eradication expedites wound healing rate 78.1% MRSA‐infected model. We present attractive approach disintegrating through synergistic effect disrupting enzyme‐like activity, phototherapy, offering innovative perspective on combating biofilm‐associated infections.

Language: Английский

---

Effective Activation of Peroxymonosulfate by Oxygen Vacancy Induced Musa Basjoo Biochar to Degrade Sulfamethoxazole: Efficiency and Mechanism

Toxics, Journal Year: 2024, Volume and Issue: 12(4), P. 283 - 283

Published: April 12, 2024

Biochar materials have garnered attention as potential catalysts for peroxymonosulfate (PMS) activation due to their cost-effectiveness, notable specific surface area, and advantageous structural properties. In this study, a suite of plantain-derived biochar (MBB-400, MBB-600, MBB-800), possessing well-defined pore structure substantial number uniformly distributed active sites (oxygen vacancy, OVs), was synthesized through facile calcination process at varying temperatures (400, 600, 800 °C). These were designed the PMS in degradation sulfamethoxazole (SMX). Experimental investigations revealed that OVs not only functioned enriched pollutants, enhancing opportunities free radicals (•OH/SO4•−) surface-bound (SBRs) attack but also served channels intramolecular charge transfer leaps. This role contributed reduction interfacial resistance, expediting electron rates with PMS, thereby accelerating decomposition pollutants. Capitalizing on these merits, MBB-800/PMS system displayed 61-fold enhancement conversion rate SMX compared inactivated MBB/PMS system. Furthermore, MBB-800 exhibited less cytotoxicity towards rat pheochromocytoma (PC12) cells. Hence, straightforward synthesis emerges promising catalyst vast sustainable efficient wastewater treatment environmental remediation.

Language: Английский

---

Degradation of Sodium Acetate by Catalytic Ozonation Coupled with MnOx/NiOOH-Modified Fly Ash

Toxics, Journal Year: 2024, Volume and Issue: 12(6), P. 412 - 412

Published: June 4, 2024

Fly ash, a type of solid waste generated in power plants, can be utilized as catalyst carrier to enhance its value-added potential. Common methods often involve using large amount alkali for preprocessing, resulting stable quartz and mullite forming silicate dissolution. This leads an increased specific surface area pore structure. In this study, we produced composed MnOx/NiOOH supported on fly ash by directly employing nickel hydroxide potassium permanganate generate metal active sites over the while simultaneously creating larger The ozone catalytic oxidation performance was evaluated sodium acetate target organic matter. experimental results demonstrated that optimal removal efficiency 57.5% achieved, surpassing even γ-Al2O3. After loading MnOx/NiOOH, oxygen vacancy is formed which plays indirect effect due transformation •O2− •OH vacancy. reaction process parameters, including varying concentrations ozone, acetate, dosage, well pH value quantitative analysis free radicals, were examined detail. work could used viable material wastewater treatment provided new solution added ash.

Language: Английский

---

Hydroxyl Defects‐Mediated Hydrolytic Activation of Peroxydisulfate Under Nanoconfinement: Role of Lewis Basic Sites for Altering the Photosensitized Species and Pathways

Small, Journal Year: 2024, Volume and Issue: unknown

Published: Oct. 6, 2024

Herein, the pivotal mechanism of defect engineering-mediated triazine-based conjugated polymers (TCPs) is comprehensively elucidated for photosensitized activation peroxydisulfate (PDS) under nanoconfinement by encapsulating defective polymer framework into nanochannel SBA-15 (d-TCPs@SBA-15). The incorporated hydroxyl defects (-OH defects) substantially accelerate accumulation electrons at -OH defects, forming Lewis basic sites. Due to facilitated elongation S─O bond and reduced energy barrier SO

Language: Английский

---