WATER SCIENCE AND TECHNOLOGY
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2024
·Vol. 89
·期 7
·1682-1700
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IF 2.5
Zhang Longbin,Gao Jianxiong,Liu Yulong,Zhou Zhengyuan,Sheng Xianxian,Li Dexiao,Chen Yuantian,Lyu Shuguang
View large Download slide View large Download slide Close modal In this research, ascorbic acid (AA) was used to enhance Fe(II)/Fe(III)-activated permonosulfate (PMS) systems for the degradation of fluoranthene (FLT). AA enhanced the production of ROS in both PMS/Fe(II) and PMS/Fe(III) systems through chelation and reduction and thus improved the degradation performance of FLT. The optimal molar ratio in PMS/Fe(II)/AA/FLT and PMS/Fe(III)/AA/FLT processes were 2/2/4/1 and 5/10/5/1, respectively. In addition, the experimental results on the effect of FLT degradation under different groundwater matrixes indicated that PMS/Fe(III)/AA system was more adaptable to different water quality conditions than the PMS/Fe(II)/AA system. was the major reactive oxygen species (ROS) responsible for FLT removal through the probe and scavenging tests in both systems. Furthermore, the degradation intermediates of FLT were analyzed using gas chromatograph-mass spectrometry (GC-MS), and the probable degradation pathways of FLT degradation were proposed. In addition, the removal of FLT was also tested in actual groundwater and the results showed that by increasing the dose and pre-adjusting the solution pH, 88.8 and 100% of the FLT was removed for PMS/Fe(II)/AA and PMS/Fe(III)/AA systems. The above experimental results demonstrated that PMS/Fe(II)/AA and PMS/Fe(III)/AA processes have a great perspective in practice for the rehabilitation of FLT-polluted groundwater. The effect of AA on the circulation between Fe(II) and Fe(III) in the PMS system was investigated. SO 4 •− was the primary ROS in PMS/Fe(II)/AA and PMS/Fe(III)/AA systems. The effect of actual groundwater matrixes on FLT removal was investigated. The possible degradation pathways of FLT were proposed. Effective degradation of FLT in actual groundwater was achieved.
研究领域:
环境科学
·
化学
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PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
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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International Journal of Environmental Research
·
2024
·Vol. 18
·期 6
·1-16
·
IF 2.6
Gao Yu-qiong,Ma Jia-xin,Rao Yan-yan,Chen Ju-xiang,Gao Nai-yun
Bezafibrate (BZF), an extensively used lipid-regulating agent, has been frequently detected in aqueous environments. In this work, we systematically investigated the Fe(II)/sulfite process for degrading BZF and its impact on disinfection byproducts (DBPs) during postchlorination. Degradation conditions were optimized by adjusting the pH, sulfite concentration, Fe(II), and BZF concentration. Under the conditions of pH = 4, [BZF] 0 = 5 μM, [Fe(II)] 0 = 25 μM, and [sulfite] 0 = 250 μM, the BZF removal efficiency reaches 97.9% in 15 min. Sulfate radicals (SO 4 ●– ) and singlet oxygen ( 1 O 2 ) are recognized as the main reactive agents, with Fe(IV) also contributing to the removal of BZF. Common anions (Cl − and HCO 3 − ) and humic acid generally impede the degradation process, except that trace amounts of Cl − can slightly accelerate BZF degradation. A total of ten products are recognized by ultra high performance liquid chromatography and quadrupole time-of-flight mass spectrometry, and four major degradation pathways are proposed: hydroxylation, cleavage of amino bonds, removal of fibrate chains, and dechlorination. Meanwhile, the toxicity assessment shows that the majority of products exhibit lower biological toxicity and less bioaccumulation potential than BZF itself. The Fe(II)/sulfite pretreatment alters the DBP formation potential, especially when Br − is present. The formation of trichloromethane (TCM) is diminished following pretreatment with the Fe(II)/sulfite process, whereas a noticeable increase in the formation of dichloroacetonitrile (DCAN) is found. Moreover, Fe(II)/sulfite pretreatment enhances the formation of brominated DBPs. Therefore, special consideration should be given to DBP formation when a Fe(II)/sulfite system is employed as a pretreatment for the removal of BZF in water. Graphical abstract
研究领域:
环境科学
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水处理工程
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毒理学
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高影响因子
Water
·
2025
·Vol. 17
·期 21
·3100
·
IF 3
Bingyang Wang,Xiaochen Wang,Shuang Liu,Zheng Wang,Fan Bai,Yujie Cheng,Dingkun Lu,Pengchao Xie
In this study, insoluble CaSO3was applied to replace soluble sulfite/bisulfite salt in the Fe(II)-activated sulfite/bisulfite [S(IV)] process for the efficient 2,4,6-tribromophenol (TBP) degradation. CaSO3serves as a low-cost and slow-release source of S(IV), significantly improving S(IV) utilization compared to conventional soluble Na2SO3. The Fe(II)/CaSO3system generated SO4•−and HO•through Fe(II)/Fe(III) redox cycling. Mechanistic studies confirmed SO4•−as the dominant reactive species, selectively attacking C-Br bonds and hydroxyl groups in TBP. Process optimization revealed effective performance under acidic conditions (pH 3.5–4.0) with minimal inhibition by common anions (Cl−, HCO3−). The reactive sites of TBP were identified through Fukui function calculations, and the degradation pathway was elucidated based on LC-MS analysis. Toxicity evaluation indicated reduced ecological risk of degradation intermediates due to debromination and benzene ring cleavage. This work provides a sustainable strategy for efficient TBP removal and detoxification in wastewater treatment with benefiting S(IV) utilization.
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BULLETIN OF THE CHEMICAL SOCIETY OF JAPAN
·
2018
·Vol. 91
·期 6
·998-1007
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IF 3.526
Zhang Xuezhi,Jia Shaoyi,Song Jia,Wu Songhai,Han Xu
Flocculation using Fe(II) instead of Fe(III) has been considered more efficient in the removal of As. However, excess Fe(II) used in the process always leaves substantial TFe [Fe(II)+Fe(III)] unutilized. We therefore developed three methods [the one-staged process (OS), the one-staged process with H2O2 (OSH) and the two-staged process (TS)] to remove As(III)/As(V) by Fe(II) (Fe:As = 2.0). Our results indicate that pH is an important factor that determines the utilization efficiency of TFe and the removal efficiency of As. In OS, the initial pH was adjusted before the reaction. At the optimal pHs of 10.0 and 11.0, the removal efficiencies of As(V) and TAs [As(III)+As(V)] could reach 84.0% and 66.7%, with only 61.9% and 80.2% TFe being utilized, respectively. In OSH, H2O2 was added after pH adjustment. After OS, pH was re-adjusted to the optimal values before the next 30 min reaction (TS). Compared with OS, the removal efficiencies of As could increase by more than 9% in OSH and TS at the optimal pHs. Besides, there is more than 10% improvement in the utilization efficiencies of TFe except at 12.0. Accelerating oxidation of Fe(II) or re-adjusting pH is therefore highly efficient for a more efficient removal of As from Fe(II)-rich groundwater.
研究领域:
环境科学
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水处理工程
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MINERALS ENGINEERING
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2024
·
IF 4.9
Qinbo Cao,Yan Yan,Heng Zou,Haiyu Zhang,Dianwen Liu,Shuming Wen,Yanjun Li
The separation of galena (PbS) from chalcopyrite (CuFeS 2 ) requires strong oxidants for the depression of PbS, due to the excellent hydrophobicity of PbS. In this work, an advanced oxidation process, i.e., S 2 O 8 2− /Fe 2+ treatment, was employed to selectively depress PbS. The parameters of the S 2 O 8 2− /Fe 2+ process were determined via flotation tests as follows: pH 3, 1:1 S 2 O 8 2− : Fe 2+ molar ratio, and 10 min reaction time. The S 2 O 8 2− /Fe 2+ treatment selectivity decreased the hydrophobicity of the PbS surface. UV–vis spectroscopy results revealed that SO 4 − (major species) and OH radicals were produced in solution by the activation of Fe 2+ . The SO 4 − / OH radicals reacted with the PbS surface, generating the SO 4 2− and PbSO 4 species. These species coated the PbS surface, forming a hydrophilic PbS surface and inhibiting the PbS flotation. By contrast, the S 2 O 8 2− /Fe 2+ treatment generated only a minimal amount of SO 4 2− (5.98 % of the total S species) on the CuFeS 2 surface. Therefore, the CuFeS 2 surface was hydrophobic and CuFeS 2 particles could still be floated into the foam phase. This study provides a promising method for the selective depression of PbS in the PbS-CuFeS 2 mixture.
研究领域:
矿物加工工程
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化学工程
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JOURNAL OF MEMBRANE SCIENCE
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2025
·
IF 9
Bing Zhang,Qiuhua Chen,Heli Tang,Rongqing Qi,Wenxin Shi
The persistent challenges of membrane fouling and insufficient removal of emerging pollutants remain significant barriers to the widespread adoption of ultrafiltration processes. Therefore, a pre-oxidation system combining Fe(II)-activated persulfate with micro-nano bubble enhancement (MBs/Fe(II)/PS) was developed to alleviate membrane fouling and efficiently remove acetochlor (AC). The results demonstrated that, under conditions where Fe(II) and persulfate (PS) were applied at concentrations of 15 μM and 30 μM respectively, the MBs/Fe(II)/PS pre-oxidation system outperformed the Fe(II)/PS pre-oxidation system in mitigating both reversible and irreversible membrane fouling caused by natural organic matter (NOM) mixture. The superior fouling mitigation capabilities of the MBs/Fe(II)/PS system can be primarily attributed to the coagulation effect of in-situ generated Fe(III) and the oxidation mechanisms involving free radicals. Furthermore, the MBs/Fe(II)/PS pre-oxidation process effectively reduced foulant accumulation on the membrane surface while decreasing interfacial free energy between foulants and the membrane. This transition facilitated a shift from cake filtration to complete blocking or intermediate blocking modes. Additionally, the MBs/Fe(II)/PS pre-oxidation system exhibited optimal performance in degrading NOM and AC due to the presence of SO 4 •– , •OH, and 1 O 2 . This study introduces a novel pre-oxidation strategy for mitigating membrane fouling and eliminating emerging pollutants, providing a theoretical basis for the practical application of MBs-based pre-oxidation technology.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2026
·
IF 19.7
Lei Wang,Jianpu Xing,Jianqiao Zhang,Weijun Chen,Mingyan Wang,Yan Li,Yongmin Cao,Wenjie Liu,Weibin Li,Yinghe Zhang,Lei Yang
Highly efficient synergistic catalysis is achieved by constructing a dual two-dimensional MoS 2 /ZnFe-layered double hydroxide composite (2D/2D MoS 2 @ZnFe-LDH) and coupling photocatalysis and Fenton-like process to address the drawbacks of the traditional Fenton-like system. The layered structure of ZnFe-LDH enables firm anchoring and uniform dispersion of Fe active sites within the layers without forming clusters, meanwhile enhancing mass transfer efficiency and accelerating both peroxymonosulfate (PMS) adsorption and reactive oxygen species desorption. The constructed 2D/2D heterojunction strengthens interfacial covalent bonding and compatibility, shortens the migration distance of photogenerated carriers, thereby significantly improving the charge separation efficiency, which accelerates the Fe(III)/Fe(II) cycle for sustainable catalysis across a broad pH range without Fe sludge aggregation. Comprehensive analysis of EPR, in-situ XPS, quenching and probe experiments, and DFT indicates that PMS is efficiently adsorbed onto Fe sites and reduced to generate SO 4 •- and •OH. Meanwhile, further characterization combining EPR, determination of surface Fe(II) concentration, in-situ photoelectrochemical and Raman measurements, XPS and DFT confirms that photogenerated electron can simultaneously reduce Fe(III) and promote radical desorption, thereby achieving sustainable catalysis. Hence, the system achieves complete phenol removal with a high synergistic index and figure of merit of 9.69 and 2.62 × 10 −10 mol·L −1 ·h −1 ·g −1 ·J −1 , respectively. It also operates efficiently in various complex water matrices and maintains stable operation over 24 h in the continuous-flow reactor, demonstrating strong anti-interference capability without any biological toxicity. In conclusion, this study proposes a new strategy to develop for developing high-performance and sustainable photo-Fenton-like dual-system.
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Water Supply
·
2016
·Vol. 17
·期 3
·665-673
·
IF 0.532
Zang Xueke,Gu Xiaogang,Lu Shuguang,Miao Zhouwei,Zhang Xiang,Fu Xiaori,Fu George Y.,Qiu Zhaofu,Sui Qian
Trichloroethene (TCE) degradation by Fe(II)-activated sodium percarbonate (SPC) in the presence of citric acid (CA) in aqueous solution was investigated. The results indicated that the presence of CA enhanced TCE degradation significantly by promoting HO• generation. The presence of Cl − , HCO 3 − and the initial solution pH appeared to be not negligible on the effect of TCE oxidation, while humic acid had no influence on TCE degradation. The generation of HO• and O 2 − • in the SPC/Fe(II)/CA system was confirmed with chemical probes, and the radical scavenging tests showed that TCE degradation was due to direct oxidation by HO•. Acidic pH condition was favorable for TCE degradation. In summary, this study provided detailed information for the application of the CA-enhanced Fe(II)-activated SPC technique for TCE-contaminated groundwater remediation.
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高影响因子
CHEMOSPHERE
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2020
·
IF 5.778
Haopeng Luo,Xin Zhou,Xiaojie Guo,Zhiyong Fang,Quanyuan Chen,Juan Zhou
The greatest constraint in the advanced oxidation processes involved Fe(II)/PMS was the low utilization of Fe(II) and PMS. In the present study, the co-catalytic effect of WS 2 on the Fe(II)/PMS system for the degradation of organics was investigated. In the presence of WS 2 , Fe(III) was reduced to Fe(II) during the reaction and resulted in improved decomposition of PMS as well as the degradation of 4-chloriphenol (4-CP). The decomposition rate of PMS and degradation efficiency of 4-CP were 10% and 25% in the Fe(II)/PMS process, while the efficiencies respectively increased to 99% and 100% in the WS 2 assisted Fe(II)/PMS system. The degradation of 4-CP was completed via the free radical pathway and SO 4 • - played a more important role than other active species. Low concentration of inorganic ions such as Cl − and HCO 3 − exhibited irrelevant effect while humic acid showed significant suppression on the WS 2 /Fe(II)/PMS system. Additionally, characterization and recycle results implied that WS 2 maintained a good stability during the co-catalytic processes.
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SCIENCE OF THE TOTAL ENVIRONMENT
·
2021
·
IF 7.963
Jiayi Luo,Yunqiang Yi,Guangguo Ying,Zhanqiang Fang,Yifeng Zhang
The content of active components in magnetic biochar, especially Fe(II), is closely related to its activation performance. Therefore, improving Fe(II) content in magnetic biochar is an ideal strategy to enhance the activation performance of magnetic biochar. In this study, the potassium-doped magnetic biochar was prepared and employed to activate persulfate for degradation of metronidazole. The degradation efficiency of metronidazole in potassium-doped magnetic biochar/persulfate system was 98.4%, which was 13.1 times higher than that in magnetic biochar/persulfate system. Free radicals quenching experiments and electron spin resonance analyses confirmed that surface-bound free radicals were responsible for metronidazole degradation followed the order of 1 O 2 > ·OH > SO 4 · - > O 2 · − . The doping of magnetic biochar with potassium increased its Fe(II) content, approximately 3.1 times higher than that of pristine magnetic biochar. The differences in Fe(II) content between potassium-doped magnetic biochar and magnetic biochar were the key reasons for the activation performance differences. Based on the ultra-high pressure liquid chromatography-quadrupole tandem time-of-flight mass spectrometer , the primary degradation intermediates of metronidazole were identified, and possible degrading pathways were proposed. Overall, this work provides an effective strategy to improve the activation performance of magnetic biochar.
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CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Chenying Zhou,Zixuan Zhang,Shuang Meng,Jian Zhang,Chuanshu He,Yang Liu,Yanbiao Shi,Gang Yao,Peng Zhou,Bo Lai
Phthalates are a class of widely used endocrine-disrupting chemicals, presenting substantial health hazards upon their release into aquatic environments. Herein, the catalytic potential of two-dimensional transition metal borides (MBenes, including Fe 2 B 2 , MnB, MoB, and Mo 1.33 B) as co-catalysts for activating diverse peroxides in Fenton/Fenton-like oxidation processes, with particular emphasis on optimizing the Fe(III)/Fe(II) cycling efficiency. Under optimized conditions, the Fe 2 B 2 /hydrogen peroxide (H 2 O 2 ) system demonstrated superior catalytic performance, achieving complete degradation of dimethyl phthalate (DMP) within 15 min. This system exhibited pseudo-first-order rate constants that were 5.7–154.3 times higher than those of other MBenes/Fe(III)/H 2 O 2 systems, highlighting its exceptional catalytic efficiency. Notably, Fe 2 B 2 exhibited exceptional stability through five consecutive cycles, maintaining DMP degradation rates (∼100 %) with minimal boron leaching (∼1.05 mg/L). Mechanistic studies revealed a dual activation pathway. Surface-bound Fe(II) species decompose H 2 O 2 directly to produce hydroxyl radicals. Meanwhile, B–Fe–B bridges facilitate Fe(II) regeneration by transferring electrons from iron atoms or B B bonds in Fe 2 B 2 to dissolved FeOH 2+ species. This synergistic interaction establishes a self-sustaining catalytic cycle that significantly enhances the Fenton reaction kinetics. These findings establish Fe 2 B 2 MBene as dual-functional material that serves as both a sustainable dual-function catalyst and an efficient iron source, providing new perspectives for designing MBene-based catalysts for environmental remediation applications.
研究领域:
环境科学
·
催化
·
纳米技术
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材料科学
·
化学工程
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高影响因子
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