JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2025
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IF 9.7
Min Tang,Wu Liu,Jinquan Wan,Shiyu Zuo,Zhiyong Wang,Rui Peng
Fenton-like oxidation is often hampered by high energy barriers, uncontrolled oxidation pathways, and inefficient reactive oxygen species (ROS) utilization. Here, we report an energy-driven confined catalytic nanoreactor that leverages the in-situ confinement energy generated within nanopores to fundamentally regulate degradation thermodynamics. Taking sulfamethoxazole (SMX) as a model contaminant, the confined nanoreactor exhibited a 22.11-fold higher kinetic constant (0.157 min −1 ) and 40 % enhanced mineralization efficiency compared with its non-confined system. The imprinting channel of confined nanoreactor enabled selective adsorption of SMX within the nanochannel, inducing pronounced confinement effects. The resulting confinement energy triggered a low-entropy degradation pathway (ΔS reduced by 3.2 × 10 3 -fold), which broke thermal equilibrium constraints and redirected SMX oxidation along a low-energy-barrier route. The in-situ confinement-induced low-entropy reaction not only accelerated pollutant degradation but also improved ROS conversion efficiency. This study demonstrated a green and sustainable approach to overcome the intrinsic efficiency bottleneck of Fenton-like processes and provide a new perspective on exploiting nanoconfinement effects for environmental remediation.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Guanhua Zhang,Shengjie Xia,Huimin Li,Hao Du,Tiantian Li,Yongyong Cao,Yue Meng,Juan Wang,Chenglin Zhong,Woon-Ming Lau
The synergistic treatment of pollutants in water by radical and non-radical pathways based on photo-like Fenton-activated peroxydisulfate (PDS) has received much attention from researchers. However, clarifying the structure–activity relationship between the photocatalyst structure and the dual-pathway degradation mechanism is difficult. Herein, the flower-like nickel–iron layered double hydroxide containing oxygen vacancy (NiFe-LDH-V O ) was constructed by dual-hydrothermal method. The NiFe-LDH-V O /PDS/light system exhibited excellent degradation performance (93.1%) for norfloxacin (NOR). Notably, the apparent rate constant exceeded pristine NiFe-LDH by 2.6 times. The results of experiments, characterization and DFT calculations indicated that the enhanced degradation activity was attributed to the dual-pathway of radical and non-radical induced by V O on the catalyst surface. V O can not only improve the migration and separation efficiency of photogenerated carriers, which ensures the energy base of PDS activation, but also act as the active site of both radical pathway and non-radical pathway. In particular, V O can change the adsorption conformation of PDS, which enhances the adsorption of PDS on the catalyst and significantly reduces the energy barriers of the two activation pathways of PDS. The reasonable pathways for NOR degradation were proposed based on HPLC-MS and DFT calculations. In addition, the toxicity analysis of intermediates indicated lower developmental toxicity and mutagenicity compared to NOR. The present work provides innovative insights into the study of photocatalysts with dual degradation pathways and their mechanistic elaboration.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2025
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IF 9
Bolong Zhao,Yonggang Sun,Guangsuo Yu,Min Xu,Juan Zhang,Duoning Zhao,Yulong Ma
Nitrogen doping plays a crucial role in activating the Fenton catalytic activity of transition metal oxides. However, the mechanism by which nitrogen doping sites influence the properties of these oxides remains unclear. We successfully incorporated nitrogen atoms into the internal lattice of MnFe 2 O 4 spinel through thermal activation and identified two major doping sites: interstitial nitrogen (N int ) and substitutional nitrogen (N sub ). Through in-situ DIRFTS experiments and DFT calculations, we proposed a unique mechanism. Both sites can effectively activate the catalytic activity of the oxides, but N sub is particularly effective in altering the electron distribution of Mn elements within the lattice. This alteration promotes the transformation of superoxide (•O 2 – /•OOH) to H 2 O 2 , thereby further enhancing catalytic activity. Compared to un-doped MnFe 2 O 4 , experimental results obtained using MnFe 2 O 4 N 0.4 as the catalyst demonstrated that the degradation rate constant of tetracycline in simulated wastewater increased from 0.0072 min −1 to 0.2745 min −1 . Furthermore, the degradation rate of tetracycline reached 98.7 %. For real wastewater experiments, the COD removal rate was 77.4 %, and the mineralization rate was 62.5 %. This study offers new insights into the design of nitrogen-doped transition metal oxide catalysts.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2026
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IF 9.1
Lingzhen Miao,Siqi Luo,Ziru Liang,Ming Lu,Pengcheng Wang
The treatment of wastewater laden with energetic compounds, particularly 2,2′,4,4′,6,6′-hexanitrostilbene (HNS), remains highly challenging owing to the environmental persistence and inherent toxicity of nitroaromatic derivatives. Herein, we reported a CoFe 2 O 4 /PMS system for the first-time efficient degradation of HNS. The CoFe 2 O 4 /PMS process afforded 96.3% removal of HNS within 150 min, together with 89.3% chemical oxygen demand (COD) removal and 49.5% total organic carbon (TOC) removal, indicating substantial deep oxidation and partial mineralization. Mechanistic studies combining quenching experiments, EPR spectroscopy, electrochemical analysis, and DFT calculations disclosed a synergistic radical/non-radical pathway dominated by 1 O 2 , with Fe incorporation enhancing PMS adsorption, charge transfer, and catalytic activation. HPLC-MS revealed degradation intermediates and supported three plausible degradation pathways, whereas QSAR analysis indicated progressive detoxification during oxidation. The catalyst further exhibited excellent stability, negligible metal leaching, and broad applicability toward actual HNS production wastewater and other energetic organic pollutants. These findings identify CoFe 2 O 4 /PMS as a promising platform for the efficient remediation of hazardous energetic compound wastewater.
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Journal of Water Process Engineering
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2026
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IF 6.6
Jingrong Li,Song Sun,Xuehui Zhu,Xue Zhang,Hao Shi,Yuanhong Xu
An ORR/EO-Cl system using commercial electrodes achieves efficient disinfection at 5 mA/cm 2 . • Cathodic H 2 O 2 consumes anodic free chlorine to generate 1 O 2 as the dominant bactericide. • The system suppresses chlorate and chlorite formation in real medical wastewater. • Multi-level oxidative damage to membranes, DNA, proteins and lipids causes irreversible inactivation. Electrochemical disinfection of chloride-rich medical wastewater faces an inherent trade-off: killing pathogens efficiently while avoiding toxic chlorate and chlorite formation. Here we show that coupling oxygen reduction at a commercial carbon felt cathode with chlorine evolution at a DSA@Ru/Ir anode breaks this trade-off. At 5 mA/cm 2 , cathodic H 2 O 2 rapidly consumes anodic free chlorine, generating singlet oxygen ( 1 O 2 ) as the dominant bactericidal species while suppressing chlorate and chlorite. In real hospital wastewater, chlorate drops from 0.66 to 0.39 mg/L, and the system inactivates 10 7 CFU/mL Escherichia coli in 5 min and Staphylococcus aureus in 10 min-using, the energy consumption was 0.1169 kWh/m 3 and 0.2338 kWh /m 3 , respectively. Quenching, flow cytometry, DNA electrophoresis, protein carbonylation and lipid peroxidation collectively confirm that 1 O 2 -driven oxidative stress causes irreversible membrane, DNA, protein and lipid damage. This work offers a low-energy, commercially viable strategy for electrochemical disinfection of real medical wastewater with intrinsic byproduct suppression. Download: Download high-res image (85KB) Download: Download full-size image
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JOURNAL OF CATALYSIS
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2026
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IF 6
Xiaoyuan Qin,Chang Zhou,Zerui Su,Jianbing Huang,Jian Zhang
The selective hydrogenolysis of biomass-derived furfuryl alcohol (FOL) to 1,5-pentanediol (1,5-PeD) is a crucial yet challenging transformation in biorefinery. Herein, a NiPr-CTS-F catalyst synthesized via a formic acid-assisted carbothermal shock (CTS) strategy, which features an ultrafast, energy-efficient, and low-pollution process with minimal carbon residue, is reported for this reaction. Comprehensive characterization confirms the successful construction of an intimate Ni–PrO x interface accompanied by oxygen vacancies. This structure creates synergistic ternary active centers, integrating metallic Ni sites for H 2 activation, interfacial oxygen vacancies for adsorbing the O atom of C–O–C in the furan ring, and basic sites for anchoring the hydroxyl group. Mechanistic studies reveal that this synergistic site steers the key intermediate, tetrahydrofurfuryl alcohol (THFA), into a bidentate adsorption configuration that selectively stretches and polarizes the C 2 –O 1 bond, thereby facilitating its selective cleavage. Furthermore, the isopropanol (IPA) solvent participates via a Meerwein–Ponndorf–Verley (MPV) mechanism, supplying hydride ions (H ⁻ ) and dynamically regulating the surface hydrogen concentration to ensure high selectivity while suppressing over-hydrogenolysis. Under optimal conditions (180 °C, 3 MPa of H 2 , 24 h), a high 1,5-PeD yield of 72.1% is achieved with FOL conversion of 99.4%. The catalyst also exhibits excellent stability over five consecutive cycles with negligible activity loss. This work not only provides an efficient catalyst for 1,5-PeD synthesis but also offers molecular-level insights into selective C–O bond cleavage, demonstrating how rationally designed interfacial sites and solvent participation can cooperatively govern reaction pathways. These findings present a new paradigm for designing multifunctional catalytic interfaces for biomass valorization.
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EUROPEAN POLYMER JOURNAL
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2026
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IF 6.8
Bo Zhu,Shijie Xu,Yu Feng,Ji Liu,Xu Weijie
Dynamic covalent networks provide a practical route to repairable coatings, but combining damage recovery with surface charge regulation remains difficult in fluoropolymer systems. Here, fluoroethylene vinyl ether copolymer (FEVE) coatings were crosslinked through NCO–OH reactions using isophorone diisocyanate (IPDI)-based curing agents containing Diels–Alder (DA) and disulfide (S–S) structures. Variable-temperature Fourier transform infrared spectroscopy (FTIR) and differential scanning calorimetry (DSC) showed clear temperature-responsive behavior in the cured networks. The DA7-2S3 coating, prepared at a 7:3 M ratio of DA-type to S–S-type curing components, had a glass-transition temperature of 27.3 °C, below the healing temperature of 70 °C. Quantum chemical calculations and surface electrical measurements showed that the dynamic structures altered localized states and charge-transport behavior. Pure DA exhibited deeper trap characteristics and the highest initial characteristic flashover voltage of 11.51 kV, but retained 92.98% after damage–healing. DA7-2S3 reached an apparent scratch-healing efficiency of 86.8%, while its characteristic flashover voltage decreased only from 11.28 to 11.02 kV, corresponding to 97.67% retention. Adjusting the DA/S–S ratio therefore improved the balance among charge regulation, damage recovery, and post-healing insulation retention.
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CHEMICAL PAPERS
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2026
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IF 2.7
Wu Yanlin,Qin Pixian,Li Yuan,Dong Wenbo,Monfort Olivier,Zeng Yilan
In this study, trace chlorogenic acid (CGA) was introduced as a natural reductant and ligand to facilitate the activation of Fe(III) in a sulfate radical-based advanced oxidation process (SR-AOP), enabling effective Fenton-like degradation of ofloxacin (OFL) under mild conditions. The CGA/Fe(III)/PMS system exhibited excellent performance in the degradation of ofloxacin (OFL) at near-neutral pH. The presence of CGA effectively promoted Fe(III)/Fe(II) cycling via dual redox and chelation effects, thereby enhancing PMS activation. Reactive oxygen species (ROS) analysis suggested that sulfate radicals (SO 4 ·− ) were the dominant contributors to OFL degrdation, while other reactive species played minor roles. The system maintained high activity in the presence of common coexisting anions in water (e.g., Cl − , and SO 4 2− ), whereas HCO 3 − and HPO 4 2− significantly suppressed degradation. These findings demonstrated the promising potential of CGA as an environmentally compatible additive for Fe(III)-based AOPs, providing useful mechanistic insight for mitigating antibiotic contamination in aquatic environments. Graphical abstract
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JOURNAL OF CATALYSIS
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2026
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IF 6
Zhouxuan Zang,Wenjie Shi,Feifan Zheng,Bolun Mei,Ouyang Liu,Yi Yu,Chunmei Cao,Li Xu
The precise regulation of Fe spin states and correlation with catalytic activity remain a challenging frontier in heterogeneous catalysts. Herein, we report an Fe-based spinel oxide with iron atoms solely occupying octahedral sites, prepared from layered double hydroxide (MgFe-LDH) precursor. The Fe spin configuration has been precisely regulated from low- to high-spin states by controlling the calcination temperature. The catalyst prepared at 700 °C (MgFeO-700) exhibits a medium-spin Fe state, which optimally balances reactant activation and six-member-ring transition state formation, delivering superior catalytic transfer hydrogenation (CTH) performance with a stable 95% yield in the transformation of furfural (FF) to furfuryl alcohol (FOL). Combined in situ DRIFTs and density functional theory (DFT) calculations reveals that the hybridization strength of Fe 3d and O 2p orbitals governs the spin-dependent reaction kinetics. The moderate d-p orbital coupling in the medium-spin state reduces the six-membered-ring transition state barrier, driving higher catalytic efficiency This work uncovers a direct structure–activity correlation between Fe spin state and catalytic performance, providing a general strategy for spin-state engineering of Fe-based oxides toward economical and robust catalysts.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2026
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IF 9.6
Xiaobo Feng,Boding Zhang,Tong Wu,Hao Jin,Deju Yuan,Anjia Deng,Dong Liu,Likun Pan,Tianjun Ni
Co Fe dual single-atom sites tailor electronic structure to boost PMS activation. • 97.7% ± 2.6% tetracycline removal in 15 min ( k = 0.22 min −1 ), outperforming single-atom catalysts. • Fixed-bed reactor sustains ∼95% tetracycline removal for 120 h with lower ecotoxicity. Single-atom catalysts (SACs) for peroxymonosulfate (PMS) activation are often constrained by the limited electronic tunability of isolated mono-metal centers, which weakens oxidant adsorption and interfacial charge transfer. Herein, we overcome this limitation by constructing a Co Fe dual single-atom catalyst anchored on a nitrogen-doped carbon aerogel (Co–Fe/NCNA) for visible-light-assisted tetracycline degradation. Spectroscopic and synchrotron analyses confirm that atomically dispersed Co N 3 and Fe N 4 sites coexist within a hierarchically porous three-dimensional carbon framework, ensuring high active-site accessibility and rapid mass transport. The Co–Fe/NCNA system achieves 97.7% ± 2.6% tetracycline (TC) removal within 15 min ( k = 0.22 min −1 ), dramatically outperforming single-metal and metal-free analogues. Density functional theory calculations indicate that the coupled Co Fe sites reconstruct the local electronic structure, elevate the d-band center, strengthen PMS adsorption, and reduce the activation barrier for PMS conversion to 0.30 eV. The TC degradation proceeds through a cooperative radical/nonradical oxidation network, in which h + -mediated oxidation acts as the primary apparent pathway, while 1 O 2 , ·O 2 − , ·OH, SO 4 · − , and possible high-valent metal-oxo-like species contribute synergistically or serve as auxiliary pathways. Notably, a fixed-bed continuous-flow reactor sustains ∼95% tetracycline removal over 120 h, and outstanding activity is retained under natural sunlight. This work establishes electronic structure engineering of dual single-atom sites as a powerful strategy to boost visible-light-driven PMS activation for sustainable water remediation. Under visible-light irradiation, the Co Fe dual single-atom sites regulate the local electronic structure, optimize the d-band center, and promote photogenerated charge separation and interfacial electron transfer, thereby enabling efficient peroxymonosulfate (PMS) activation. Through the synergistic cooperation of electron-mediated PMS reduction, hole-mediated PMS oxidation, and Co/Fe self-cycling, radical and non-radical reactive species are generated to construct an integrated oxidation network, which drives the efficient degradation and mineralization of tetracycline. Download: Download high-res image (401KB) Download: Download full-size image
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JOURNAL OF HAZARDOUS MATERIALS
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2026
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IF 10.6
Lan Li,Hui Chen,Yuheng Chen,Baiyang Chen
Singlet oxygen ( 1 O 2 ) is a key reactive species in environmental, chemical, and biological systems. For decades, furfuryl alcohol (FFA) has been used as a probe for quantifying 1 O 2 based on the assumption that it reacts selectively with 1 O 2 but is inert toward other oxidants. However, we demonstrate that this assumption is fundamentally flawed in the chlorine-hydrogen peroxide (H 2 O 2 ) system-one of the most common contexts for 1 O 2 generation. Results demonstrate that chlorine alone can degrade FFA significantly, implying that previous studies may have systematically overestimated 1 O 2 yields. Specifically, raising pH facilitated the decay of chlorine but hindered FFA degradation, suggesting that 1 O 2 formation is unfavorable under alkaline conditions. Increasing the dosage of chlorine enhanced FFA degradation, but decreased the relative contribution of 1 O 2 to FFA degradation. More strangely, increasing the FFA dosage unexpectedly reduced the kinetics of FFA degradation, implying that the concentration of 1 O 2 was not constant under fixed chlorine-H 2 O 2 condition. Maintaining low dissolved oxygen enhanced FFA decay, suggesting that superoxide is not an intermediate for 1 O 2 formation. Furthermore, pyranone was not formed during FFA degradation processes, invalidating it as a characteristic product. These evidences together challenge the accountability regarding FFA selectivity, pyranone formation, and 1 O 2 formation mechanisms before using FFA for 1 O 2 quantification in chlorine-involved systems.
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Surfaces and Interfaces
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2026
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IF 6
Qiubai Jiang,Tianle Tan,Hui Deng,Jiang Wan,Long Wang,Min Li,Yang Wang,Guangxu Liu
Solar-driven interfacial evaporation (SDIE) is a low-energy and environmentally friendly technology for clean-water production. However, when applied to complex waters, volatile organic compounds (VOCs) can readily enter the condensate. In this study, a sequential strategy involving carbonization followed by composite fabrication was used to construct a CuO@Fe 2 O 3 @CC-SA (CFCC-SA) bimetallic oxide aerogel evaporator with both mechanical stability and flexibility for efficient water evaporation and VOC degradation. Synergistic interactions between Fe and Cu enhanced both the photothermal conversion efficiency and Fenton-like catalytic activity of the material. Meanwhile, the porous aerogel network provided excellent hydrophilicity and rapid water transport, thereby promoting efficient evaporation. Under 1.0 kW m –2 irradiation, the CFCC-SA evaporator exhibited an evaporation rate of 2.06 kg·m –2 ·h –1 , corresponding to an approximately 20% increase relative to the monometallic CuO@CC-SA evaporator. For phenol, CFCC-SA achieved removal efficiencies of 98.4% in the condensate and 63.8% in the raffinate. Furthermore, CFCC-SA maintained high phenol removal performance over a broad pH range and under highly saline conditions (20 wt% NaCl). Overall, by integrating efficient water transport with synergistic bimetallic catalysis, the CFCC-SA evaporator offers a promising strategy for designing SDIE systems that simultaneously enable high-rate water evaporation and VOC removal. Download: Download high-res image (272KB) Download: Download full-size image
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