WATER AIR AND SOIL POLLUTION
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2025
·Vol. 237
·期 1
·9
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IF 3
Liu Yiqing,Hu Hong,Chen Chuanzeng,Xu Linghan
Generally, Fe(II) has an efficiently catalytic activity toward peroxymonosulfate (PMS), but the slow conversion of Fe(III) to Fe(II) and production of iron sludge impede the practical application of Fe(II)/PMS system. In this work, ascorbic acid (AA), a complexing agent and reductant, was introduced to Fe(III)/PMS process to facilitate the Fe(III) reduction. The decoloration of rhodamine B (RhB) was obviously enhanced in Fe(III)/PMS process with the addition of AA. Fe(III)-AA complex was firstly generated in Fe(III)/AA/PMS process via the complexation and then was reduced to Fe(II), which could catalyze PMS to yield oxidative species. Fe(IV), sulfate radical (SO 4 •− ) and hydroxyl radical ( • OH) were the working oxidants for RhB decoloration in this system, and SO 4 •− played a major role. Increasing Fe(III), AA or PMS dosage was beneficial to RhB decoloration, but their excessive concentration would hinder RhB decoloration. The existence of HCO 3 − , SO 4 2− or FA in this system showed an inhibition effect on RhB decoloration, while a facilitation effect was obtained when the high concentration of Cl − was present. This research offers a way to improve PMS activation by Fe(III) and a technology for eliminating the refractory organic pollutants from the contaminated water.
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Journal of the Taiwan Institute of Chemical Engineers
·
2025
·
IF 6.3
Bing Liao,Ziyi Wang,Ruyi Chang,Zhengchun Hu,Qiuyue Ye,Wen Xu,Jiale Wu,Zhuoyuan Zhou,Wu Shen,Na Guo,Lingfeng Huang,Zhicheng Pan
Background Sulfate radical−based advanced oxidation processes (SR-AOPs) show promising prospects for the pretreatment and advanced treatment of ammonia nitrogen in landfill leachate. However, in high chloride ion environments, SR-AOPs often lack selectivity, leading to the over-oxidation of ammonia nitrogen to undesirable nitrate NO 3 − and NO 2 − rather than the desired N 2 , which remains a major challenge. Methods In this study, CoFe 2 O 4 was prepared by a gel-calcination method and the effects of chloride ions (Cl − ) and other parameters on the performance of CoFe 2 O 4 -activated peroxymonosulfate (PMS) oxidation system for the removal of ammonia nitrogen and the selectivity of oxidation products were systematically investigated. Significant findings Cl − played a crucial role in determining the ammonia removal efficiency and nitrogen selectivity. Under the optimum conditions of 30 mM of PMS, 0.1 g/L of catalyst and 20 mM of Cl − , the ammonia removal efficiency of the system was nearly 100 %, and the nitrogen selectivity reached 88.1 %. The main species in the activation process of the PMS was Co(II)-OH, and the formation of this complex was promoted by Fe(III). SO 4 · − , HO · , and chlorine species (Cl · , ClO · , and HClO) were generated in the system. Among them, SO 4 · − and HO · indirectly contributed to ammonia oxidation by reacting with Cl − to produce reactive chlorine species, which subsequently oxidized ammonia nitrogen.
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CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Shuang Zhong,Yu Tian,Chen Chen,Bin Nie,Hongyan Wang,Shengyu Zhang
The utilization of nitrogen and sulfur-codoped biochar-activated peroxymonosulfate (PMS) has emerged as a promising advanced oxidation technology for the degradation of organic pollutants. However, the dominant active sites, especially the specific defect structures governing PMS activation and their subsequent activation mechanism remain ambiguous, posing challenges to the rational design of high-performance biochar catalysts. Herein, a series of nitrogen and sulfur-codoped biochar (NSBC) with varying pyrolysis temperatures and doping levels were synthesized. An investigation into the relationship between their properties and the reaction rate constants of 2,4-dichlorophenol (2,4-DCP) degradation by activated PMS revealed that intrinsic defects, thiophene S, and graphitic N were active sites in the oxidation reaction, with intrinsic defects identified as playing a predominant role. Density functional theory (DFT) calculations combined with electrochemical measurements further revealed the crucial role of single-vacancy defective configuration in mediating a direct electron transfer pathway for 2,4-DCP degradation. Moreover, double-vacancy and topological defects facilitated the transfer of electrons to adsorbed PMS, leading to the release of 1 O 2 and subsequent degradation of 2,4-DCP. The distinctive mechanism enabled the NSBC-activated PMS system to exhibit high selectivity and effectively remove 2,4-DCP from a complex aquatic environment. The findings from this study provide valuable insights into the role of specific structural defects in PMS activation and offer theoretical support for the design of biochar catalysts with heteroatom doping strategies.
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APPLIED CATALYSIS A-GENERAL
·
2026
·
IF 4.8
Kaiqi Zhang,Chao Li,Ming Xu,Chaoyue Wang,Jingyang Luo,Jiashun Cao,Hongqiang Ren
Hollow PBA-derived CoFeO nanocages with well-developed mesoporous structure successfully synthesized. • High Co (II)/Co (III) ratio and oxygen vacancies boost PMS activation. • Efficient tetracycline degradation (96.17%) via radical (•OH, SO 4 •– , O 2 •– ) and non-radical ( 1 O 2 ) pathways. • Good reusability and a certain ionic interference tolerance demonstrated. Antibiotic contamination in the environment poses significant risks to ecosystems and human health. In this study, hollow CoFe oxide nanocages derived from a Prussian blue analog (PBA-CoFeO) were synthesized and used for efficient peroxymonosulfate (PMS) activation toward tetracycline degradation. The catalyst exhibits a high Co (II)/Co (III) ratio (1.74) and a high density of oxygen vacancies, which synergistically enhance PMS activation. Tetracycline (TC) was selected as a model antibiotic to evaluate catalytic performance. Under optimized conditions, the PBA-CoFeO/PMS system achieved a removal efficiency of 96.17% and maintained over 80% efficiency after five consecutive cycles, demonstrating excellent stability and reusability. Notably, the TC removal efficiency remained above 80% in the presence of coexisting anions, suggesting a certain resistance to ionic interference. Radical quenching experiments and electron paramagnetic resonance (EPR) spectroscopy revealed that hydroxyl radicals (•OH), sulfate radicals (SO 4 •– ), superoxide radicals (O 2 •– ) and singlet oxygen ( 1 O 2 ) were involved in the degradation process, confirming the coexistence of radical and non-radical pathways. This work highlights the potential of PBAs-derived catalysts for efficient PMS activation and their application in advanced oxidation processes. Download: Download high-res image (271KB) Download: Download full-size image
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2026
·
IF 5.4
Yumei Xing,Yawei Shi,Keyan Liu,Yan Wang,Ya Sun,Zonglin Pan,Mengqi Li,Mingxing Guo,Guanghui Ding
Composite sponges with opposite wettability were successfully prepared. • ODA-MgFe 2 O 4 -PU can effectively absorb oil. • TA-MgFe 2 O 4 -PU can effectively activate PMS to degrade organic pollutants. • The degradation pathway was proposed by DFT calculation and LC-MS analysis. Dissolved organic pollutants and oils are prevalent wastewater contaminants, and developing efficient remediation technologies remains a research hotspot. Herein, magnesium ferrite (MgFe 2 O 4 ) was synthesized via coprecipitation and immobilized on polyurethane (PU) sponges, followed by hydrophobic octadecylamine (ODA) and hydrophilic tannic acid (TA) modification to fabricate ODA-MgFe 2 O 4 -PU and TA-MgFe 2 O 4 -PU composite sponges. Hydrophobic ODA-MgFe 2 O 4 -PU showed excellent oil absorption capacity of 26.8–50.3 g/g for various oils and stable hydrophobicity under complex water conditions. By contrast, hydrophilic TA-MgFe 2 O 4 -PU activated peroxymonosulfate (PMS) to efficiently degrade Rhodamine B and other pollutants with removal efficiencies of 64.5%–95%, displaying good environmental adaptability and reusability. The RhB degradation mechanism and pathway were clarified via quenching experiments, electrochemical tests, spectral characterization, functional theory calculations and mass spectrometry analysis. Moreover, ECOSAR prediction and Vigna radiata germination tests verified the effective detoxification of degraded RhB. Download: Download high-res image (151KB) Download: Download full-size image
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2026
·
IF 9.1
Bin Wen,Fan Chen,Yi Ran,Dongyun Que,Zhihao Zhang,Youwei Zeng,Yuyuan Yao
Molybdenum disulfide (MoS₂) is a promising inorganic co-catalyst for Fenton processes due to its structural durability and avoidance of secondary organic pollution. However, the conventional 2H-phase MoS₂ suffers from intrinsically low conductivity, severely limiting Fe 3+ reduction in the Fenton reaction. Herein, L-cysteine served as a multifunctional precursor during the preparation of MoS₂, promoting a slow-release sulfur supply, carbon‑nitrogen co-doping, and the prevention of restacking. The carbon and nitrogen co-doped molybdenum disulfide (CN-MoS 2 ) architecture was fabricated via a single-step hydrothermal reaction mediated by sodium molybdate, thiourea, and L-cysteine. Remarkably, benefiting from the introduction of L-cysteine, the resulting CN-MoS 2 exhibited a high 1 T-phase content (68%), abundant sulfur vacancies, and a substantially reduced particle size. CN-MoS 2 accomplished near-complete elimination of carbamazepine (CBZ) within merely 3 min, yielding a prominent apparent rate constant of 0.7111 min −1 , which is a 19-fold kinetic acceleration over thiourea-derived MoS 2 . CN-MoS₂ also exhibited high TOC removal, broad-spectrum degradation, and robust CBZ removal under various water conditions. Additionally, electrochemical analyses further verified that CN-MoS₂ reduced charge-transfer resistance and enriched electron density, thereby facilitating rapid electron shuttling to Fe 3+ . Concurrently, quenching experiments and electron paramagnetic resonance (EPR) diagnostics unambiguously validated SO 4 •- , 1 O 2 and O 2 •- as the driving reactive forces. Moreover, a continuous-flow device incorporating a CN-MoS 2 -based membrane exhibited outstanding performance in wastewater purification. This work offers a new strategy for designing high-activity co-catalysts for advanced oxidation processes.
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Sustainable Materials and Technologies
·
2026
·
IF 9.7
Qiang Chen,Lei Xu,Le Liang,Chen Chen,Xiao-He Wu,Baoling Yuan,Ming-Lai Fu
With the large-scale disposal of spent lithium-ion batteries (SLIBs) and the ongoing accumulation of organic pollutants in water bodies, the resource recovery of solid waste and water pollution control have emerged as critical challenges in the environmental field. To address the dual challenges of SLIBs and persistent organic pollutants, a nickel‑cobalt‑manganese oxide catalyst (NCM-APS) was synthesized via hydrothermal treatment of SLIB leachate with ammonium persulfate (APS) for peroxymonosulfate (PMS) activation. The catalyst featured a nanostructured morphology, large surface area, and abundant hydroxyl groups, enabling efficient PMS activation. Under optimized conditions, nearly complete removal of 10 μmol/L sulfamethoxazole (SMX) was achieved within 20 min, and 82.4% removal of 50 μmol/L SMX occurred within 1 h. The catalyst exhibited favorable stability to a certain extent, maintaining activity in the presence of common coexisting ions (Cl − , NO 3 − , SO 4 2− ) and after repeated cycles. Reactive species analysis suggested the generation of SO 4 • − , HO • , 1 O 2 , and O 2 • − , with 1 O 2 as the predominant oxidant. High-resolution mass spectrometry and Fukui function analysis elucidated the SMX degradation pathway. This work demonstrates a sustainable strategy for SLIB upcycling and highlights the practical potential of PMS-based advanced oxidation processes in wastewater treatment.
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JOURNAL OF POLYMER SCIENCE
·
2026
·
IF 3.9
Guobin Lin,Yongyu Hou,Mengting Song,Wangchuan Xiao,Deshu Cheng,Juxiang Luo
Nitroxide-mediated polymerization (NMP) is a powerful technique, yet achieving precise control over methacrylic esters remains challenging. A novel alkoxyamine initiator, 3-(((2-cyanopropan-2-yl)oxy)(cyclohexyl)amino)-2,2-dimethyl-3-naphthylpropanenitrile (CNDN), featuring bulky naphthyl group, was synthesized via a three-step route (Schiff base reduction, Oxone oxidation, and radical coupling). This alkoxyamine enables well-controlled polymerization of methyl methacrylate (MMA) at 80°C with dispersities below 1.45. The polymerization follows first-order kinetics, and the molecular weight increases linearly with conversion. The high steric hindrance suppresses bimolecular termination, ensuring excellent end-group fidelity and successful chain extension with MMA, ethyl methacrylate, and styrene. Notably, CNDN also mediates controlled MMA polymerization without deoxygenation. This work presents an efficient initiator for controlled methacrylate polymerization under mild conditions and introduces a novel synthetic strategy that could enable general access to structurally diverse alkoxyamines. The resulting naphthyl-terminated polymers hold promise for fluorescent labeling, optical materials, and nanoparticle dispersants. Graphical A naphthyl-containing alkoxyamine initiator (CNDN) enables controlled methacrylate polymerization at 80°C with low dispersity, even without deoxygenation. This novel synthesis strategy could offer a versatile platform for accessing structurally diverse alkoxyamines for precision polymer materials.
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MOLECULES
·
2026
·Vol. 31
·期 16
·2884
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IF 5.1
Yiqiong Yang,Juan Han,Cui Wang,Pingchuan Yang,Panchen Li,Xiaodong Zhang
MOF-derived catalysts have considerable potential for aqueous contaminant control, but their practical application is often constrained by the aggregation and difficult recovery of powder catalysts. In this study, a self-supportingN-doped Fe/Ni-based monolithic catalyst, denoted N-101-NFF, was fabricated through the in situ growth of an Fe-based MOF precursor on nickel–iron foam followed by pyrolysis. Under the conditions of 50 mg/L chlortetracycline (CTC), 0.08 mmol/L peroxymonosulfate (PMS), and an effective catalyst area of 1 cm2, N-101-NFF degraded 90.3% of CTC within 60 min and maintained a degradation efficiency of 88.6% after five consecutive cycles. Quenching experiments and EPR analysis indicated the involvement of •OH, SO4•−, O2•−, and1O2in CTC degradation. Electrochemical measurements indicated improved interfacial charge-transfer characteristics, while post-reaction XPS analysis revealed changes in the Fe and Ni valence states and surface N- and O-containing groups, supporting the involvement of Fe and Ni redox cycling and these surface functionalities in PMS activation. In a fixed-bed reactor, the system maintained more than 86% CTC removal over 24 h of continuous-flow operation at a CTC feed rate of 200 mL/h. These results highlight the potential of N-101-NFF as a recoverable monolithic catalyst for PMS-based treatment of antibiotic-contaminated water.
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Journal of Water Process Engineering
·
2026
·
IF 6.6
Peien Huang,Jiale Zou,Lizhang Liu,Ziming Zhang,Yongzhi Tu,Jianxin Chen,Zhifei Ma
Despite extensive studies on Co-based layered double hydroxide (LDH) catalysts for peroxymonosulfate (PMS) activation, systematic investigations on metal-ion leaching behavior through compositional and structural regulation of LDHs remain scarce. In this work, MgCoFe-LDHs with various cation ratios were synthesized and calcined at different temperatures to obtain MgCoFe-LDOs. While exploring the optimal catalytic performance toward PMS activation, the leaching behaviors of Co and Fe ions were simultaneously evaluated. The results showed that both calcination temperature and the proportion of Co incorporated into the divalent-metal sites significantly affected PMS activation performance and metal-ion release. When 16% of the divalent-metal sites were substituted with Co, the Co-ion concentration after reaction decreased by approximately 57.70% (from 0.3865 mg·L −1 to 0.1635 mg·L −1 ) for the sample calcined at 300 °C compared with the uncalcined precursor. The improved Co leaching levels are significantly lower than the Co emission limit (< 1.0 mg/L) stipulated in The Emission Standard of Pollutants for Copper, Nickel, and Cobalt Industry (GB 25467–2010). Moreover, both the catalytic performance and the leaching control capability are superior to those of representative Co-based catalysts reported under comparable conditions. Additionally, the effects of inorganic anions on MB degradation in the MgCoFe-LDO/PMS system and the catalyst's applicability toward different dye contaminants were examined. Radical-quenching tests and electron paramagnetic resonance (EPR) analyses confirmed that singlet oxygen ( 1 O 2 ) was the dominant reactive species. Based on XPS results and other characterizations, a possible degradation mechanism of MB in the MgCoFe-LDO/PMS system is proposed.
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Coatings
·
2026
·Vol. 16
·期 1
·89
·
IF 2.8
Hao Liu,Haoyue Shi,Qianyu Ma,Liwen Yin,Yuxin Li,Wei Wang,Huijun Yu,Zuoli He
HighlightsWhat are the main findings?A simple and environmentally friendly preparation method for CoZn-ZIFs was proposed.The novel PMS activator Co-CNTs@NC was successfully obtained via pyrolysis of CoZn-ZIFs.What are the implications of the main findings?The Co-CNTs@NC/PMS system achieved efficient degradation of TCH over a wide pH range.The degradation mechanism dominated by1O2for TCH degradation was confirmed.Zeolite imidazolate frameworks (ZIFs)-derived carbon materials have garnered widespread attention as peroxymonosulfate (PMS) activators in removing antibiotics because of their excellent catalytic performance. However, most carbon materials derived from ZIFs exhibit limited efficacy in treating high-concentration (>10 ppm) antibiotic wastewater, and their synthesis methods are environmentally unfriendly. Herein, we develop a simple and environmentally friendly preparation method to synthesize a new type of nitrogen-doped carbon-supported carbon nanotubes coated with cobalt nanoparticle (Co-CNTs@NC) composites via high-temperature calcination of cobalt–zinc bimetallic ZIFs. The material characterization results confirm the successful preparation of Co-CNTs@NC composites featuring a high specific surface area (512.13 m2/g) and a Co content of 5.38 wt%. Across an initial pH range of 3.24–9.00, the Co-CNTs@NC/PMS catalytic system achieved over 84.17% degradation of 20 mg/L tetracycline hydrochloride within 90 min, demonstrating its favorable pH tolerance. The singlet oxygen-dominated degradation mechanism was confirmed by quenching experiments and electron paramagnetic resonance characterization. This work can provide technical guidance and reference significance for the preparation of metal–carbon materials derived from ZIFs with excellent efficiency of removal of high-concentration antibiotics.
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Journal of Environmental Chemical Engineering
·
2026
·Vol. 14
·期 2
·121737
·
IF 7.5
Xixi Di,Xia Zeng,Shujun Meng,Tian Tang,Wei Wang,Hanghang Zhao,Xiaohui Ji,Lingxia Jin,Chao Duan,Xianzhao Shao
s Iron-based heterogenous catalysts play an important role in Fenton-like reactions, but their practical application is hindered by complex synthetic procedures and limited comprehension of reaction mechanisms. A straightforward impregnation and pyrolysis method was devised to synthesize a zero-valent iron (ZVI) modified carbon-based catalyst which significantly boosts PMS activation to degradation of tetracycline hydrochloride (TCH), more importantly, it elucidated the correlation between the electronic structure and the production of non-radical reactive oxygen species (ROS). The optimized catalyst demonstrates exceptional performance, achieving 97 % removal of TCH within 30 min, with a remarkable apparent rate constant ( k obs ) of 0.1962 min −1 , outperforming the pristine carbon catalyst by 11-fold. Mechanistic investigations reveal that the incorporation of ZVI facilitates redox cycling with PMS, thereby boosting the generation of diverse ROS. Theoretical calculations reveal that both radical and non-radical pathways synergistically enhance catalytic activity. This work presents a cost-effective and scalable approach to designing high-performance carbon-based catalysts for PMS activation, providing valuable insights into the development of sustainable water purification technologies for emerging contaminants.
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