COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2026
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IF 5.4
Weiwei Huang,Yuning Zhang,Quan Yuan,Hang Yang,Weiwei Lv,Wenzong Zhou
Understanding membrane fouling mechanisms, particularly the pretreatment-mediated fouling mitigation mechanism, is critical for controlling algal fouling. This study examined the fouling control mechanism of extracellular organic matter (EOM) by combined heat-activated potassium peroxymonosulfate (PMS) and polyaluminum chloride (PACl) treatment using extended Derjaguin-Landau-Verwey-Overbeek (XDLVO)-based interaction energy analysis. Results showed that combined PMS and PACl treatment effectively mitigated membrane fouling, with the fouling control performance being highly dependent on PACl dosage. PACl 5 mg/L under combined PMS treatment worsened membrane fouling, while PACl dosages 10 – 40 mg/L alleviated it, with the best performance achieved at 40 mg/L. XDLVO theory analysis revealed that PMS-PACl (10 – 40 mg/L) treatment enhanced repulsive membrane-foulant interactions and transformed membrane-foulants and foulants-foulants interactions from attractive to repulsive. Moreover, both membrane-foulant and foulant-foulant repulsive interactions increased with increasing PACl dosage. In contrast, although integrated PMS and PACl 5 mg/L weakened foulant-foulant attractive interaction than control EOM, serious membrane fouling was still observed, likely due to stronger attractive membrane-foulant interactions during the initial filtration stage. This research offers new mechanistic insights into fouling control and provides a theoretical basis for algal-laden water treatment. Download: Download high-res image (209KB) Download: Download full-size image
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高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2026
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IF 9.1
Xin Jin,Liu Tian,Keke Wang,Lingxiang Zhao,Tiancheng Li,Yanqing Shi,Huajing Zhou,Liang He,Yunze Ruan,Jingyang Li,Shanshuai Chen
Second-sphere oxygen doping stabilizes high-valent Co(IV) = O active centers. • Co 14 Mn 1 -oxo achieves complete tetracycline removal within 20 s. • Non-radical oxidation pathway driven by Co(IV) = O and singlet oxygen ( 1 O 2 ). • Excellent stability and recyclability in complex water environments. • Provides a new coordination-sphere strategy for advanced oxidation catalysts. Tailoring the local coordination and electronic microenvironment of metal centers is crucial for achieving high efficiency catalysis and maintaining catalyst stability during peroxymonosulfate (PMS) activation. Conventional strategies often introduce a second metal to modulate the oxygen reduction potential, but this typically disrupts coordination symmetry and compromises structural stability. Here, we develop an oxygen-doping strategy within the second coordination sphere to construct structurally robust Co 14 Mn 1 -oxo active centers. Systematic characterization and Density functional theory (DFT) reveals that oxygen doping reduces the electron density of primary Co sites, thereby weakening bonding effects and suppressing structural distortion of Mn N during PMS activation. The optimized catalyst enables complete tetracycline (TC) degradation within 20 s and extends operational lifetime over 2000-fold. Meanwhile, the weakened coordination field decreased the energy level of the Co O σ* orbital, promoting nucleophilic attack by high-valent Co(IV) = O species on TC and increasing the degradation rate by fivefold. Electron paramagnetic resonance (EPR) and quenching experiments confirmed that the TC degradation was predominantly governed by non-radical pathways, mainly mediated by Co(IV) = O species and singlet oxygen ( 1 O 2 ). In addition, the dual-active-site architecture significantly reduced the energy barrier for O O bond cleavage in PMS to form Co(IV) = O. This work offers a feasible design strategy for stabilizing high-valent metal species via second-sphere engineering, offering a new perspective for designing highly efficient and stable environmental catalysts. This work develops an oxygen-doping strategy within the second coordination sphere to construct robust Co 14 Mn 1 -oxo active centers, establishing a non-radical oxidation pathway dominated by high-valent Co(IV) = O species. The optimized catalyst achieves complete tetracycline removal within 20 s, demonstrating an exceptional reaction rate of 0.2273 s −1 . Download: Download high-res image (189KB) Download: Download full-size image
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CHEMICAL ENGINEERING JOURNAL
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2026
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IF 12.5
Yingyi Li,Wei Li,Shangru Zhai,Zuoyi Xiao,Jingai Hao,Qingda An,Xin Zhao,Shuang Shan,Xianquan Li
Cotton-derived Co-CN-X catalysts via dopamine-assisted polymerization–pyrolysis. • Co-CN-24 exhibits superior catalytic activity and robust stability in PMS activation. • Nitrogen doping catalysts coupled PMS system governs non-radical pathways toward electron-rich pollutants degradation. Biomass-derived materials offer renewability and waste valorization for water purification, yet identifying and controlling their precise ROS-driven degradation pathway in peroxymonosulfate (PMS)-based systems remains a fundamental challenge. Herein, we report N-doped cobalt‑carbon catalysts (Co-CN-X) from cotton via polymerization-pyrolysis and show how nitrogen doping tailors PMS activation for pollutant degradation. Upon nitrogen introduction, the optimized Co-CN-24 catalyst achieves efficient carbamazepine degradation, reaching 96.55% within 35 min with a 7.12-fold enhancement in reaction efficiency compared to the Co-C counterpart. Integrated characterization and DFT calculations reveal that Co-CN-24 possessing high pyrrolic N and Co 0 content abundant facilitates 1 O 2 generation, thereby increasing the dominance of non-radical pathways in pollutant degradation. Most importantly, the Co-CN-24/PMS system exhibits selective reactivity toward electron-rich pollutants, broad pH tolerance, and robust performance in complex water matrices, including continuous flow experiments. This work provides mechanistic insight into how nitrogen doping regulates non-radical pathways in biomass-derived catalysts, offering a sustainable strategy for targeted pollutant remediation.
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高影响因子
ENVIRONMENTAL RESEARCH
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2026
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IF 8.2
Shihan Wang,Weike Zheng,Haifeng Shi,Yigang Chen
In peroxymonosulfate (PMS) activation processes, the relatively slow redox kinetics of metal ions have been a key factor limiting both PMS activation efficiency and photocatalytic performance. In this study, a Co 3 O 4 /PTFE composite with integrated piezoelectric and photothermal properties was successfully constructed, which significantly enhanced the Co 3+ /Co 2+ cycle and thereby promoted PMS activation for efficient tetracycline (TC) degradation. Under the dual stimulation of mechanical agitation and visible light irradiation, the Co 3 O 4 /PTFE composite exhibited enhanced photothermal conversion and piezoelectric performance, which significantly promoted the generation of reactive species such as SO 4 •- and •OH. Compared with pristine Co 3 O 4 , CoP-2 demonstrated a superior TC degradation efficiency of up to 83% in the PMS system. X-ray photoelectron spectroscopy (XPS) analysis revealed that the introduction of polytetrafluoroethylene (PTFE) induced interfacial strain, modulated the valence state of cobalt species, and optimized the surface electronic structure, thereby facilitating the formation of active sites and enhancing electron transfer processes. Free radical trapping experiments further identified the dominant reactive species and revealed the underlying synergistic catalytic mechanism. Moreover, CoP-2 maintained excellent stability after multiple degradation cycles. This study provides a novel strategy for the design of multifunctional synergistic catalysts and expands the application potential of piezo-photothermal/PMS systems in environmental purification.
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高影响因子
Journal of Environmental Chemical Engineering
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2026
·Vol. 14
·期 4
·123242
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IF 7.5
Guijuan Liu,Xiaolong Zhang,Lijuan Tan,Weixing Li
The integration of photocatalytic process with peroxymonosulfate (PMS) activation constitutes a promising strategy for eliminating organic pollutants in aqueous solutions. Despite notable advances in CoFe 2 O 4 /g-C 3 N 4 composites, studies on their application in visible-light-responsive PMS-activated tetracycline (TC) degradation remain insufficient, particularly in the systematic elucidation of the quantitative order of ROS contributions and associated mechanisms. To address this knowledge gap, a recyclable CoFe 2 O 4 /g-C 3 N 4 heterojunction photocatalyst was prepared via the sol–gel method. The composites demonstrated outstanding photocatalytic performance with 97.8% TC degradation in 60 min under visible-light irradiation. The kinetic rate constant of 0.056 min −1 , which was 3.7 and 3.2 times that of pure g-C 3 N 4 (0.015 min −1 ) and CoFe 2 O 4 (0.017 min −1 ). Moreover, the developed catalyst exhibited excellent stability along with tolerance to common anions and compatibility with various organic matrices. By coupling radical quenching experiments with ESR spectroscopy, a definitive degradation contribution order for the reactive species in this system was firstly established as: 1 O 2 > SO 4 · - > O 2 · - > h + > · OH. A plausible mechanism for TC degradation was thus put forward. It provides a viable approach for developing high-performance and durable g-C 3 N 4 -derived photocatalytic system, which can be effectively utilized in environmental remediation process.
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高影响因子
Catalysts
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2025
·Vol. 15
·期 5
·419
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IF 4
Longfei Xia,Xilin Wang,Jiahui Li,Dongyan Xu
Mn-based catalysts have been extensively studied in advanced oxidation processes based on peroxymonosulfate (PMS) oxidants, demonstrating their significant potential for treating antibiotic-contaminated wastewater. In this study, an amorphous MnO2-based composite catalyst (MnO2/CN@SiO2) was prepared and used to activate PMS for degrading levofloxacin (LEV). The effects of reaction conditions, such as reaction temperature, catalyst dosage, PMS concentration, and solution pH, on LEV degradation were comprehensively investigated. The interference of water components, e.g.,NO3−,SO42−, Cl−,CO32−, and humic acid, on the degradation efficiency of LEV was analyzed, and the stability of the catalysts was explored by cycling experiments. Finally, radical quenching experiments and electron paramagnetic resonance spectroscopy were employed to elucidate the contribution of active species to the degradation reaction process. A non-radical-based pathway for LEV degradation was proposed based on these results.
研究领域:
环境科学
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催化化学
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废水处理
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高影响因子
MOLECULES
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2025
·Vol. 30
·期 12
·2618
·
IF 4.6
Kaining Sun,Xinyi Yang,Fei Qi,Yingjie Liu,Lijing Wang,Bo Feng,Jiankang Yu,Guangbo Che
Peroxymonosulfate (PMS)-based advanced oxidation technology has emerged as an effective means for removing organic pollutants from water due to its strong oxidizing ability. However, enhancing the activation efficiency of PMS represents a key challenge at present. SrTiO3, a typical perovskite metal oxide, holds potential in the field of the photocatalytic degradation of pollutants, yet its application is limited by the wide bandgap and fast carrier recombination rates. This study optimized the photocatalytic performance of SrTiO3by regulating its electronic structure and optical properties through cobalt (Co) doping. Experimental results (TRPL, TPV, UV–Vis DRS, ESR, etc.) and DFT calculations (GGA-PBE) demonstrated that Co doping shifted the d-band center of SrTiO3upwards, optimized the adsorption energy of SO4−, enhanced the sunlight response range, and significantly improved carrier extraction efficiency. Under visible light irradiation, 2,4-dichlorophenol (2,4-DCP) could be effectively degraded within 60 min in a wide pH range. Through Fukui function calculation (B3LYP/6-31G*) and experimental characterization analysis (HPLC-MS and IC), the possible degradation pathways of 2,4-DCP and the mechanism for photocatalysis were investigated. The toxicity analysis (T.E.S.T) confirmed the reduced toxicity of the degradation products of 2,4-DCPs. This study provides a reference for the catalyst design and optimization strategy of PMS-based advanced oxidation technology.
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高影响因子
ENVIRONMENTAL RESEARCH
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2025
·
IF 7.7
Ye Li,Bai-Hang Zhao,Bao-Yu Zhang,Jia-Hang Liu,Xu-Ming Liu
Peroxymonosulfate (PMS)-based advanced oxidation processes have gained significant attention due to their strong oxidative capacity and rapid reaction kinetics. However, the development of efficient, stable, and eco-friendly catalysts remains a major challenge in realizing practical applications. To address this issue, a novel catalyst, Co 1 Ce 2 O x @PAL, was synthesized via the sol-gel method to enhance PMS activation efficiency by leveraging rare-earth doping and the carrier properties of palygorskite (PAL). Comprehensive characterization (SEM, XRD, FTIR, etc.) confirmed successful synthesis and favorable structural properties. Norfloxacin (NOR) was selected as the target contaminant to evaluate the catalytic performance of Co 1 Ce 2 O x @PAL. Under an optimal condition (30% metal loading, 0.3 g/L catalyst, 0.5 mM PMS, pH 6.2), NOR removal efficiency reached 95%, with an apparent rate constant of 0.15 min -1 . Quenching tests and electron paramagnetic resonance (EPR) analyses revealed that played a dominant role in NOR degradation. and were generated through the redox reactions between Co 2+ /Co 3+ and Ce 3+ /Ce 4+ . Furthermore, oxygen vacancies facilitated electron transfer, thereby promoting radical production and NOR degradation efficiency. DFT calculation, including electrostatic potential and frontier orbital analyses (HOMO/LUMO), identified the quinolone and piperazine rings as the most susceptible sites for radical attack. Four potential degradation pathways were proposed accordingly. The catalyst demonstrated a high stability and reusability, maintaining over 80% NOR removal after five cycles. ECOSAR predicted reduced toxicity for most transformation products. This study highlights the potential of Co 1 Ce 2 O x @PAL as an effective catalyst for sustainable water treatment by enabling efficient degradation of trace emerging contaminants and promoting water resource recycling.
研究领域:
环境化学
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催化科学
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水处理技术
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材料科学
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计算化学
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污染物降解
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高级氧化过程
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高影响因子
Journal of the Taiwan Institute of Chemical Engineers
·
2024
·
IF 5.5
Shengrong Liu,Boyang Wang,Yimeng Huang,Xing Xu,Yujiao Kan,Yanan Shang
Background Advanced oxidation processes (AOPs) based on sulfate radicals (SO 4 •– ) have proven to be highly effective in degrading organics in wastewater. Carbon-based materials have emerged as promising catalysts for activating persulfate, which generates environmentally friendly sulfate radicals (SO 4 •– ), for remediation purposes. The nitrogen doping technique is an effective method for site-specific regulation and can significantly enhance the performance of carbon-based catalysts, which could promote the application of carbon-based catalysts in the future. Endogenous and exogenous nitrogen sources can provide nitrogen sources for N doping. However, there are few reports on the comparison of the structure and catalytic mechanism of these two types of N-doped biochar. It is also of great significance to reveal the mechanisms of constructing catalytic sites using endogenous and exogenous nitrogen. Methods Herein, the preparation of endogenous nitrogen-doped biochar (BC) was achieved by using soybean as the precursor material, which is rich in natural nitrogen-containing components of proteins. Subsequently, the BC was doped by mixing it with urea and pyrolysis, resulting in the preparation of exogenous nitrogen-doped biochar (NBC). Significant findings The characterization of XRD and HRTEM showed that g-C 3 N 4 formed in NBC. The results of catalytic degradation and quenching experiments demonstrate that the exogenous nitrogen-doped catalysts have a better performance than endogenous nitrogen-doped catalysts. The OFL removal rate in BC/PMS was higher than that in the BC/PMS system (71.68% vs. 61.83 %). The k obs in NBC/PMS are also higher than that in BC/PMS (0.00943 min −1 vs. 0.01369 min −1 ). The NBC could be a promising catalyst for PMS activation in practical application. DFT results showed that the g-C 3 N 4 generated from exogenous nitrogen can improve PMS activation performance in the g-C 3 N 4 /graphene bilayer structure. The influence on the charge distribution of surrounding carbon materials makes endogenous nitrogen doping a good choice for optimizing the local performance of the material in the absence of natural nitrogen components.
研究领域:
环境科学
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材料科学
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高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2024
·
IF 8.1
Shishun Wang,Shuang Gai,Kui Cheng,Zhuqing Liu,Markus Antonietti,Fan Yang
The degradation efficiency of organic contaminants using Fenton-like system based on Fe(II) and peroxymonosulfate (PMS) has been hindered by the rapid transformation from Fe(II) to Fe(III) and the slow regeneration of Fe(II). To address this challenge, artificial humic acid (AHA) derived from biomass was incorporated into Fe(III)/PMS system to build AHA/Fe(III)/PMS system. The results demonstrated that the degradation rate of atrazine (ATZ) in AHA/Fe(III)/PMS system (98.83%) is significantly superior to those in Fe(III)/PMS (16.51%) and AHA/PMS system (41.76%) within 90 min. Furthermore, Fe(II) measurement experiments revealed that AHA exhibited more significant iron-reducing potential. The analysis of FTIR, 3D-EEM, and liquid NMR indicated that AHA possessed more structures with reductive potential in comparison to commercial humic acid (CHA) and humic acid extracted from lignite (LHA). The results of persistent free radicals indicated that CHA possessed oxidative potential, which also accounted for the lowest Fe(II) concentration in those system containing CHA. Furthermore, quenching experiments, EPR analysis, and PMSO probe analysis have indicated the presence of reactive species such as •OH, SO 4 •- , and Fe(IV) within AHA/Fe(III)/PMS system. The degradation products from ATZ were identified and determined to exhibit reduced toxicity relative to parent compound. Collectively, these findings presented an in-depth understanding to reactivate Fe(III)/PMS system, offering a promising alternative strategy for efficient degradation of organic pollutants in water treatment processes.
研究领域:
环境科学
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水处理技术
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高影响因子
Small
·
2024
·
IF 13
Yi Shen,Yongliang Pan,Chao Zhu,Haizhong Zhang,Jun Wang,Renlan Liu,Qile Fang,Shuang Song,Baoliang Chen
In the domain of heterogeneous catalytic activation of peroxymonosulfate (PMS), high-valent metal-oxo (HVMO) species are widely recognized as potent oxidants for the abatement of organic pollutants. However, the generation selectivity and efficiency of HVMO are often constrained by stringent requirements for catalyst adsorption sites and electron transfer efficiency. In this study, a single-atom catalyst, Cu SA /CN P&S, is synthesized featuring multiple types (planar/axial) of heteroatom coordination via an H-bond-assisted self-assembly strategy. It is confirmed that CuN 3 active centers with axial S coordination are uniformly distributed in a carbon matrix modified by planar P atoms. Cu SA /CN P&S activated PMS to selectively generate Cu (III) ═OH species as the primary reactive oxygen species (ROS). The pseudo-first-order kinetic rate for bisphenol A degradation reached 1.51 min −1 , a 17.57-fold increase compared to the unmodified Cu SA /CN catalyst. Additionally, the Cu SA /CN P&S catalyst demonstrates high efficiency and durability in removing contaminants from various aqueous matrices. Theoretical calculations and experimental results indicate that the intrinsic electric field generated by distal planar P atoms enhances electron transfer efficiency within the carbon matrix. Meanwhile, axial S coordination elevates the d-band center and tunes the e g * band broadening of Cu, thereby enhancing the adsorption selectivity for the terminal oxygen of PMS. This multitype coordination synergistically mitigates the issues of low selectivity and yield of HVMO species.
研究领域:
环境科学
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催化化学
·
材料科学
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PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Mengxiao Liu,Hanbin Wu,Yiqiao Xie,Li Zeng,Yiyang Xu,Chen Da,Yang Yu
The discharge of pharmaceutical and personal care products (PPCPs)-containing wastewater has caused severe water pollution problems. Herein, an aeration-driven piezoelectric peroxymonosulfate (PMS) activation process using oxygen-vacancy engineered BaTiO 3 (BTO-Ov) is applied for the PPCPs removal from water. About 95 % of amoxicillin (AM) can be removed within 30 min in the presence of aeration and PMS. Compared to other PMS based advanced oxidation processes, the aeration-driven piezoelectric PMS activation process using BTO-Ov exhibits dual superiority in catalytic performance and energy saving capability. During the process, the sufficient dissolved oxygen (DO) originated from the aeration can not only work as the precursor for the reactive oxygen species (ROS) formation, but also the enhancer for the PMS activation. The activation energy of PMS is 26.9 kJ/mol in the proposed system, much lower than most previously reported studies. Moreover, the involvement of ROS in the AM degradation is able to be also regulated by the DO content in solution, achieving better mineralization efficiency of AM. The system also demonstrates good reusability and application potential on the removal of other PPCPs from water. This work offers an excellent method for the wastewater treatment and in-depth mechanism understanding on the aeration-driven piezoelectric PMS activation process.
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高影响因子
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