SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Guohui Liu,Qiongfang Wang,Lei Dong,Xin Zhang,Min Zhang,Pinhua Rao,Naiyun Gao,Wenjuan Zhang,Jing Deng
The activity of iron oxychloride (FeOCl) in advanced oxidation processes (AOPs) was limited by the redox cycle of Fe(III)/Fe(II). To resolve this problem, FeOCl loading on WS 2 (FW-X) was successfully synthesized with the different ratios of Fe/W (X = 0.5, 1, 2, 3) to active peroxymonosulfate (PMS). Among them, FW-3 displayed excellent catalytic performance which activated 0.5 mM PMS to degrade 97 % thiamphenicol (TAP) in 45 min. FW-3/PMS performed well in a wide pH range (3–10). Besides, the anions ( C l - , N O 3 - , H 2 P O 4 - , H P O 4 2 - and H C O 3 - ) and humic acid inhibited the oxidation of TAP in varying degrees. During the catalytic process, H 2 O and PMS were adsorbed on the surface of FW-3 with the formation of surface hydroxyl groups (Fe–OH) and Fe–HOOSO 3 . Surface hydroxyls as a bridge promoted the electron transfer between O–O bond and Fe sites. Then O–O bond broke to generate reactive oxygen species (ROS, H O · , S O 4 ∙ - , Fe(IV), O 2 ∙ - and 1 O 2 ), and S O 4 ∙ - was the dominant ROS for the degradation of TAP. Additionally, WS 2 as a co-catalyst broke the limitation of the iron redox cycle. Under the attack of these ROS, TAP produced eighteen intermediates through four possible degradation pathways. According to ecotoxicity assessment, toxicity of some intermediates produced from path of S-C bond breakage was less harmful than TAP. After three consecutive cycles, FW-3 maintained outstanding catalytic performance. Additionally, FW-3/PMS possessed a good non-selectivity that could remove different contaminants. In a word, this paper proved the potential of FW-3/PMS in practical wastewater remediation.
研究领域:
环境科学
·
催化化学
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高影响因子
APPLIED SURFACE SCIENCE
·
2026
·
IF 6.6
Jingzhao Lu,Yanfang Zhu,Zhen He,Jun Zhao,Bingxia Duan,Yanyan Lu,Zhiliang Li,Yapeng Zhou,Guizhu Wu
Antibiotic residues pose a serious threat to aquatic environment, underscoring the urgency of developing efficient and stable advanced oxidation technologies. While the activation process based on peroxymonosulfate (PMS) shows great promise, its efficacy is highly dependent on the performance of the catalyst. In this study, a novel Mn 3 O 4 -Mn 5 O 8 nanohybrid was successfully synthesized and its performance in activating PMS for the degradation of tetracycline (TC) was systematically evaluated. By constructing an electron-rich interface, the nanohybrid achieved optimized manganese valence distribution and efficient cycling, leading to significantly enhanced catalytic activity. In the PMS system, the Mn 3 O 4 -Mn 5 O 8 attained 99.4% TC removal within 30 min, with the reaction rate constant (0.150 min⁻ 1 ) significantly exceeding those of the Mn 3 O 4 (0.052 min⁻ 1 ) and Mn 5 O 8 (0.066 min⁻ 1 ) systems, while the manganese leaching rate (3.65%) was much lower than that of unstable Mn 3 O 4 (8.53%). Mechanistic investigations revealed that the outstanding performance originated from interface-driven manganese valence cycling and electron transfer, which synergistically regulated both radical (O 2 ⁻) and non-radical ( 1 O 2 ) pathways. Furthermore, the catalyst exhibited good anti-interference capability in complex water matrices and cycling stability. This work provided a novel design principle centered on interface engineering and valence state synergy for developing high-performance manganese-based catalysts in PMS-driven water purification.
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高影响因子
Journal of Water Process Engineering
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2026
·
IF 6.6
Lei Fang,Yuman Lv,Xinlei Liu,Shijie Wang,Miaomiao Ye
An iron–copper bimetallic biochar catalyst (Fe-Cu@BC) was synthesized to establish a heterogeneous peroxymonosulfate (PMS) activation system aimed at improving the removal of typical organic pollutants in drinking water sources. The physicochemical properties of the catalyst, the catalytic performance, reactive species generation, pollutant degradation pathways, and impacts on dissolved organic matter (DOM) transformation were systematically investigated. Under the optimized conditions, a humic acid (HA) removal efficiency of 66.28% was achieved, which was attributed to the cooperative redox behavior of Fe and Cu species. Radical quenching experiments and electron paramagnetic resonance (EPR) spectroscopy confirmed the simultaneous generation of OH, and 1 O 2 . A quantitative chemical probe-based kinetic analysis clarified the contributions of individual reactive species, and pollutant degradation proceeded through the combined action of OH/-driven radical oxidation and 1 O 2 -mediated selective oxidation. Advanced characterization using three-dimensional excitation-emission matrix (3D-EEM) fluorescence spectroscopy and Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR-MS) showed that the system altered the molecular composition of DOM in both conventionally treated and advanced-treated effluents, converting high-molecular-weight, reduced components into low-molecular-weight, more oxidized intermediates. This work provides an effective catalytic strategy for the deep treatment of organic-contaminated water using carbon-based bimetallic activators.
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高影响因子
Catalysts
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2025
·Vol. 15
·期 7
·610
·
IF 4
Wei Wang,Jiaqi Liu,Guang Shi,Shiqi Wu,Nan Zhang,Ruixia Yuan
Spherical Cu2O nanoparticles were obtained by reducing copper acetate in N,N-dimethylformamide (DMF) system using glucose as the reducing agent and polyvinylpyrrolidone (PVP) as the surfactant, with which spherical PdCu nanocatalysts were thus synthesized by disproportionation. The catalyst was used for the activation of peroxymonosulfate (PMS) and showed an excellent degradation effect on rhodamine B and methylene blue-contained printing and dyeing wastewater with good stability. Additionally, the surface morphology analysis of the catalyst was carried out by SEM and TEM. The structure was characterized by XRD and FT-IR. The valence state and composition of the catalyst were characterized by XPS. The catalytic performance of the prepared catalysts was investigated with methylene blue and rhodamine B used as target pollutants. The results showed that the catalytic reduction efficiency of PdCu nanocatalyst for the two pollutants could reach 99% at 20 °C, when catalyst concentration was 60 mg/L and PMS concentration was 1.0 g/L and 0.6 g/L, respectively. The degradation efficiency of the catalyst was significantly reduced when Cl−,HCO3−and HA were present in the water. The degradation efficiency was above 90% when the pH was in the range of 5–11. The excellent performance of the PdCu/PMS system in the treatment of RhB-contained wastewater was further confirmed by taking into account of the data of free radical quenching experiment and the results of electron paramagnetic resonance (EPR) experiment. After three cycles, the removal rate of MB and RhB could still be maintained at more than 90%, which proved its excellent recyclability due to its remarkable stability and efficiency.
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高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2025
·
IF 9
Bingyang Liu,Yu Wang,Qi Yang,Xiaojing Li
Atrazine (ATZ), a highly persistent triazine herbicide, poses significant environmental risks due to its endocrine-disrupting effects, necessitating efficient remediation technologies. To overcome the limitations of active site availability and electron transfer bottlenecks in single-metal iron-based MOFs (Fe-MIL-101) during peroxymonosulfate (PMS) activation, this study innovatively constructed bimetallic FeM-MIL-101 (M = Co, Zn, Ni, Cu) catalysts. Through hydrothermal synthesis and multi-scale characterization, FeCo-MIL-101 was shown to achieve complete ATZ degradation within 60 min ( k obs = 0.059 min −1 ), representing a 3.9-fold enhancement in degradation efficiency over the best-performing control. The catalyst maintained >95 % removal efficiency across a broad pH range and under interference from high concentrations of common anions (Cl − , NO 3 − , SO 4 2− , H 2 PO 4 − ), while exhibiting minimal inhibition by HCO 3 − (>82 % removal). Mechanistic studies revealed that Fe O Co bridging bonds induced oxygen vacancy (OV) generation, significantly accelerating the Fe 3+ /Co 3+ ↔ Fe 2+ /Co 2+ redox cycles and synergistically optimizing both radical and non-radical pathways. Sulfate radicals (SO 4 – ) served as the dominant reactive species (contributing 58.3 %), with singlet oxygen ( 1 O 2 ) and superoxide radicals (O 2 – ) playing a synergistic role (collectively 38 %). The catalyst retained >90 % activity over 6 consecutive cycles, with metal leaching below 14 μg/L, and the degradation products exhibited significantly reduced developmental toxicity. Bimetallic synergy and OV-mediated electron transfer were identified as the key factors enhancing PMS activation efficiency. By strengthening HSO 5 − adsorption energy and interfacial charge transfer, FeCo-MIL-101 overcomes the limitations of single-metal systems, providing an atomic-level design strategy for the efficient removal of persistent organic pollutants in complex aqueous environments.
研究领域:
环境化学
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材料科学
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催化化学
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水污染控制
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分子环境科学
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毒理学
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纳米催化
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高影响因子
CHEMICAL ENGINEERING JOURNAL
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2022
·
IF 16.744
Xin Yang,Lu Yao,Yu Wang,Xinran Zhang,Pengfei Ren
Algae blooms can clog filtration tank, release toxic cyanotoxin and produce undesirable disinfection byproducts (DBPs) in post-chlorination, which brings challenges to conventional water treatment processes. In this study, peroxymonosulfate (PMS) was tested for its ability to improve Fe(III) coagulation of Microcystis aeruginosa in water treatment. Compared with conventional Fe(III) coagulation, the presence of PMS resulted in the formation of larger floc and thus better algae and turbidity removal. The removal of algae by PMS-enhanced Fe(III) coagulation (PMS-Fe(III)) process reached 97.5% at 1 mM PMS, which was 1.5 times higher than that by Fe(III) coagulation alone. The oxidization of surface-adsorbed extracellular organic matter destabilized the algal cells and enhanced their coagulation without greatly damaging the cells’ integrity. Simultaneously, about 80% of Microcystin-LR, a cyanotoxin, was degraded in the enhanced process. Moreover, the formation of DBPs and their associated toxicity during the subsequent chlorination were decreased by 49.2% and 13.6%, respectively. The production of trihalomethanes, haloacetic acids and haloacetronitriles was particularly abated. SO 4 •- and HO • , which were formed from PMS activation through redox cycling of Fe mediated by the existing natural organic matter, were mainly responsible for algae removal. The results indicate that supplementing Fe(III) coagulation with PMS is a promising option for treating water during algal blooms.
研究领域:
环境科学
·
水处理工程
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高影响因子
Journal of Environmental Sciences
·
2026
·
IF 6.3
Lihui Zhao,Can Jin,He Liu,Zhaozhe Yang,Yupeng Liu
Bisphenol A (BPA), a widespread endocrine-disrupting compound, necessitates efficient activation of peroxymonosulfate (PMS) for its degradation. Conventional carbon-based catalysts frequently exhibit limited efficiency, poor stability, and potential environmental risks. Bamboo-derived porous carbon material (BCM) and bamboo-derived porous carbon material loaded with Fe (BCM-Fe) serve as effective catalysts for activating PMS to degrade BPA. The BCM/PMS system achieved a BPA removal efficiency of 94.44 % within 150 minutes, while the BCM-Fe/PMS system attained 97.8 %. Quenching experiments and electron paramagnetic resonance (EPR) analysis identified non-radical singlet oxygen (¹O₂) as the dominant reactive species. Density functional theory (DFT) calculations demonstrated that atomically dispersed Fe species on BCM-Fe significantly enhanced PMS adsorption energy and activation kinetics compared to BCM. Both catalysts exhibited excellent reusability, confirming their potential as practical and sustainable catalysts. This study provides fundamental insights for designing efficient, environmentally benign carbon-based catalysts for advanced oxidation processes.
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高影响因子
Journal of Environmental Chemical Engineering
·
2025
·
IF 7.2
Yonglei Xing,Huimin Ma,Jian Yi,Xiaoyong Jin,Yage Peng,Gang Ni
Antibiotic pollutants such as levofloxacin (LVF) pose serious threats to ecosystems and human health due to their persistence in aquatic environments, making their efficient removal a great challenge. In this study, a BiFeO 3 /BiVO 4 heterojunction photoanode was rationally designed for the photoelectrocatalytic (PEC) degradation of levofloxacin (LVF) in the presence of peroxymonosulfate (PMS). Under visible light irradiation and a 0.6 V bias, the BiFeO 3 /BiVO 4 photoanode coupled with PMS achieved 78 % LVF degradation, markedly surpassing bare BiVO 4 (≈44 %), with excellent mineralization and stability, retaining > 72 % efficiency after four cycles. Radical quenching experiments revealed the synergistic roles of SO 4 •− , ‧O 2 − , ‧ OH , and h + . To clarify the PMS activation pathway, a dual-chamber H-type reactor with a proton exchange membrane was employed, confirming that PMS activation originated from photogenerated electrons at the photoanode, while the cathode contribution was negligible. Photoelectrochemical analyses (OCP, DPV, EIS, i–t) further demonstrated the adsorption–activation–electron capture behavior of PMS. These findings highlight BiFeO 3 /BiVO 4 as a promising photoanode for PMS-assisted PEC degradation of antibiotics, offering an effective strategy for water purification.
研究领域:
环境科学
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材料化学
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光催化
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水处理技术
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DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2021
·
IF 6.707
Cong Wang,Jingyu Zhao,Congmei Chen,Ping Na
In this study, we compared the differences between bimetallic oxides FeCo 2 O 4 catalyzing the oxidation of phenol by peroxydisulfate (PS) and peroxymonosulfate (PMS) under near neutral and alkaline conditions. Phenol could be completely oxidized and removed in both PMS and PS systems. X-ray photoelectron spectroscopy (XPS) analysis and density functional theory (DFT) calculations showed that there was a synergistic mechanism between Co and Fe on the catalyst surface. Although the PMS-FeCo 2 O 4 system reached the fastest reaction rate of 1.5 × 10 −1 min −1 , it showed a higher oxidants consumption and more residual total organic carbon (TOC) (36%) in solutions after reactions. Quenching experiments and electron paramagnetic resonance (EPR) analysis showed that sulfate radical (SO 4 − ), hydroxyl radical ( OH) and singlet oxygen ( 1 O 2 ) played important roles in the oxidation of phenol in PMS system. While in the PS-FeCo 2 O 4 system, in addition to free radical reactions, the non-radical mechanisms between PS and the catalyst surface played a major role in phenol oxidation, and the soluble organic matter in the PS system could be completely removed. Thus, PS has a better application prospect in the treatment of phenol. This discovery has certain guiding significance for catalyst modification and doping to improve catalyst activity and the choice of oxidant.
研究领域:
环境科学
·
催化化学
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2019
·
IF 8.355
Bo Sheng,Fei Yang,Yihao Wang,Zhaohui Wang,Qian Li,Yaoguang Guo,Xiaoyi Lou,Jianshe Liu
Despite the success of Fe(II)/peroxymonsulfate (PMS) process in detoxifying organic pollutants, its intrinsic drawback of sluggish Fe(III) conversion to Fe(II) limits its large-scale practical application. Here we report that commercial MoS 2 , a common metal sulfide, can be used to unlock this kinetic constrain. Addition of MoS 2 greatly accelerates the reduction of Fe(III) to Fe(II), decomposition of PMS, and thus results in enhanced degradation efficiency of 2,4,6-trichlorophenol (TCP) (>95%) and other biorefractory halogenated organic compounds within 30 min. Mass spectroscopy data indicate that TCP can be destructed into low-molecular-weight organic acids, manifesting its powerful oxidation capacity of MoS 2 -assisted Fe(II)/PMS process. Once the Fe(III) in aqueous solution is stabilized by its organic or inorganic ligands, the boosting effects of MoS 2 are largely inhibited and less than 80% of TCP is degraded. Sulfate radicals and hydroxyl radicals are identified as the dominant reactive oxidants in the MoS 2 /Fe(II)/PMS process by radical scavenging tests. The unsaturated S on the fresh MoS 2 surface and the exposed Mo(IV) sites are supposed to react with PMS and Fe(III) in the aqueous solution, respectively. No iron oxides and Mo oxides are detected in X-ray photoelectron spectroscopy (XPS) and X-ray powder diffraction (XRD) measurement, indicating the accelerated Fe(II)/PMS process mainly occurs in the homogeneous solution. MoS 2 exhibits excellent recyclability and sustainable reactivity for the degradation of TCP after 5 consecutive runs. Overall, the present study provides a novel strategy to overcome the rate-limiting step of Fe(III)/Fe(II) that is commonly challenging Fe-based advanced oxidation processes (AOPs) and enable Fe(II)/PMS as efficient as typical Co(II)/PMS.
研究领域:
环境科学
·
催化化学
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高影响因子
ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2019
·Vol. 26
·期 36
·36410-36422
·
IF 2.914
Latif Abdul,Kai Sun,Si Youbin
This study demonstrated, for the first time, Fe(III)/peroximonosulphate (PMS) could be an efficient advanced oxidation process (AOP) for wastewater treatment. Bisphenol A (BPA) was chosen as a model pollutant in the present study. Fe(III)-activated PMS system proved very effective to eliminate 92.18% of BPA (20 mg/L) for 30-min reaction time at 0.50 mM PMS, 1.5 g/L Fe(III), pH 7.0. The maximum degradation of BPA occurred at neutral pH, while it was suppressed at both strongly acidic and alkaline conditions. Organic and inorganic ions can interfere with system efficiency either positively or negatively, so their interaction was thoroughly investigated. Furthermore, the presence of organic acids also affected BPA degradation rate, especially the addition of 10 mM citric acid decreased the degradation rate from 92.18 to 66.08%. Radical scavenging experiments showed that SO 4 •– was the dominant reactive species in Fe(III)/PMS system. A total of 5 BPA intermediates were found by using LC/MS. A possible degradation pathway was proposed which underwent through bridge cleavage and hydroxylation processes. Acute toxicity of the BPA degradation products was assessed using Escherichia coli growth inhibition test . These findings proved to be promising and economical to deal with wastewater using iron mineral for the elimination of organic pollutants.
Graphical abstract
研究领域:
环境科学
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化学工程
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水处理
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PubMed
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
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2021
·
IF 10.588
Qianyu Zhang,Xiaoqin Sun,Yuan Dang,Jun-Jie Zhu,Yuan Zhao,Xiaoxiang Xu,Yuanzhen Zhou
A novel electrochemically enhanced homogeneous-heterogeneous catalytic system was constructed by placing the prepared heterogeneous catalyst (CoFe 2 O 4 /NF) in parallel between the anode and the cathode for peroxymonosulfate (PMS) activation to remove levofloxacin (LVF) in this work. Over 90% of LVF could be effectively removed by the constructed system after 40 min's degradation. And the electrical energy consumption was only 2.51 kWh/m 3 , which was lower than 54.5% of the traditional electrochemical advanced oxidation process . Besides, the system broadened the response range of pH and overcame the inhibitory effect of alkaline conditions on degradation. These activities were mainly due to the high generation ability of free radical (SO 4 ·- , ·OH and O 2 ·- ) and non-radical ( 1 O 2 ). And the SO 4 ·- was found to be the main radical for LVF degradation. The high SO 4 ·- generation ability was demonstrated to be resulted from the dual effects of synergy of CoFe 2 O 4 /PMS and enhancement of electrochemistry in EC/CoFe 2 O 4 /PMS system. In detail, electrochemistry could effectively promote the continuous circulation of Co 2+ /Co 3+ and Fe 2+ /Fe 3+ redox cycles on the surface of CoFe 2 O 4 to enhance the activation of PMS , thereby generating SO 4 ·- . This work can provide a promising and cost-effective approach to construct highly efficient organic pollutant degradation system.
研究领域:
环境科学
·
化学工程
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DOI
PubMed
高影响因子