SEPARATION AND PURIFICATION TECHNOLOGY
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2025
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IF 9
Nan Li,Haibo Liu,Bin Yang,Bo Xie,Yangtao Wu,Lingjun Bu,Shiqing Zhou
This study establishes a manganese-activated ferrate (Mn(II)/Fe(VI)) process for autonomous Microcystis aeruginosa removal, addressing the critical challenge of additive dependency and secondary pollution in conventional algal control strategies. System performance was critically governed by Mn/Fe stoichiometric ratios and total oxidant dosages, with near-complete algal elimination (>98 %) achieved at Mn/Fe = 1:1 (≥200 μM total dosage) while maintaining cell integrity. TOC analysis revealed dosage-dependent control over cellular lysis and intracellular organic matter (IOM) releasing. Spectroscopic characterization demonstrated process efficacy in degrading dissolved organics through decreased UV 254 absorbance (unsaturation reduction), declining SUVA (aromaticity loss), and elevated E2/E3 ratios (molecular weight reduction). Comparative analyses identified dissolved organic carbon as a more sensitive cellular stress indicator than K + release, attributed to MnO 2 adsorptive sequestration of released intracellular constituents. Mechanistic investigations revealed dual role of Mn(II) that rapid surface accumulation provided oxidative protection, while subsequent Fe(VI)-driven MnO x formation enabled floc growth through particle bridging. Water matrix effects followed valence-specific modulation, where divalent cations (Ca 2+ /Mg 2+ ) enhanced removal via charge screening, and excessive monovalent ions (Na + /NH 4 + ) impaired efficiency through ionic strength interference. This work pioneers a green oxidation-coagulation synergy that eliminates supplemental additives, offering a sustainable paradigm for mitigating cell rupture and IOM release in algae-laden water treatment.
研究领域:
环境科学
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水处理技术
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生态工程
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DOI
高影响因子
RSC Advances
·
2019
·Vol. 9
·期 70
·41022-41030
·
IF 3.049
Feilong Dong,Qiufeng Lin,Cong Li,Tuqiao Zhang
Blue-green algae commonly bloom in fresh water in summer, producing extra- and intra-cellular algal organic matters, which are important precursors for disinfection byproduct (DBP) formation. In this study, we evaluated the effect of pre-oxidation with ferrate(VI) (FeO42−, Fe(VI)) on the characterization of intracellular organic matter (IOM) and extracellular organic matter (EOM). The results indicated that soluble microbial-like products of EOM and IOM decreased and humic acid-like products of IOM increased, which would influence the DBP formation in the subsequent chlorination step. Therefore, in this study, the effect of Fe(VI) pre-oxidation on the DBP formation from IOM and EOM with subsequent chlorination was also investigated. For Chlorella sp., EOM presented no significant change, and IOM presented a reduction of THMs (8.2%) after Fe(VI) oxidation at a dosage of 16 mg L−1. For P. limnetica, EOM and IOM both exhibited reduction of trihalomethanes (THMs) and chloral hydrate (CH) after Fe(VI) oxidation. Besides, THMs had the lowest concentration at pH 8.0 in all four solutions. Haloacetonitriles (HANs) and haloketones (HKs) showed slight changes with increasing pH values. Due to the frequent detection of bromide (Br−) in surface water, the effect of bromide existence on THM formation was also investigated. The results indicated that all brominated DBPs increased, and chlorinated DBPs decreased with the increase in bromide concentration. In addition, the bromine substitution factor (BSF) of Chlorella sp. and P. limnetica both increased with the increase in Br− concentration.
研究领域:
环境科学
·
水处理工程
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DOI
PubMed
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
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2026
·
IF 10.6
Kunyu Chen,Jie Wang,Xiaoxiang Cheng,Weikang Zhang,Jingwei Huang,Congwei Luo,Xinsheng Luo,Peijie Li,Yan Jin,Daoji Wu,Ruimin Mu,Jinsuo Lu
The CaSO 3 /Fe(VI) system was demonstrated to efficiently degrade emerging contaminants under alkaline conditions. However, the integrated impacts of pH-driven mechanisms remain to be fully elucidated. The present study investigated the degradation of sulfonamide antibiotics (SAs) in both buffer solution (BS) and deionized water (DW) by conducting comparative experiments under varying pH conditions, evaluating the pH-driven degradation efficiency and mechanisms, and clarifying the integrated impacts of pH variations in the CaSO 3 /Fe(VI) system. The results indicated that pH significantly influenced the degradation performance and kinetics of the CaSO 3 /Fe(VI) system toward SAs, identifying neutral pH as the optimum condition. The dynamic increasing in pH in DW enhanced the oxidation capacity under acidic conditions. In neutral and alkaline conditions, Fe(V) was the primary active species, while alkaline conditions favored radical generation. Conversely, acidic conditions favored the formation of Fe(IV) as the predominant species. Furthermore, the active sites of SAs were identified, and degradation pathways were proposed, confirming that the process simultaneously achieves contaminant removal and toxicity reduction. In terms of engineering implications, the CaSO 3 /Fe(VI) system offers a highly competitive treatment cost of only 0.45 CNY/m 3 , while also reducing chemical dosage requirements in potential processes such as coagulation and disinfection. Moreover, the end products SO 4 2− and Fe(III) both promote coagulation, demonstrating broad application potential. Such findings underscore the significance of pH in the CaSO 3 /Fe(VI) system, elucidate the integrated impacts of pH-driven mechanisms, and provide data support for engineering applications.
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PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 13.2
Jia Zhao,Heng Zhang,Mengfan Luo,Hongyu Zhou,Zehua Wang,Jialong Yin,Chuanshu He,Peng Zhou,Jing Zhang,Bo Lai
Ferrate (Fe(VI)) activation by Mn(II) has been proven as a powerful technology due to the high catalytic activity of Mn(II) and the generation of multiple intermediates. However, the reactivity and stability of these intermediates greatly differ, thus necessitating the precise regulation of redox pathways towards the generation of the most desirable intermediates. In this study, we utilized ligand engineering to finely tune the redox pathways between Fe(VI) and Mn(II). Mn(II) complexing with ethylenediaminetetraacetic acid (EDTA) and nitrotriacetic acid (NTA) switched the redox pathways from generating Mn(IV) to more robust intermediates and enhanced the decontamination ability of Fe(VI). Ligand-to-metal charge transfer promoted the electron migration from Mn(II) complexes to Fe(VI), generating Fe(V) and Mn(III) intermediates. Then, complexing regulated the transformation of Mn(III) to generate different reactive species. Specifically, Mn(II)-EDTA activated Fe(VI) through Fe(IV)/Fe(V) and Mn(V), whereas the Fe(VI)-Mn(II)-NTA system relied on Mn(VII). Owing to the weaker chelating effect of NTA, unstable Mn(III)-NTA was successively oxidized via Mn(V) to Mn(VII). In contrast, the stronger stability of EDTA suppressed the excessive oxidation of Mn(V)-EDTA, boosting pollutant interception of reactive species. Accordingly, the Fe(VI)-Mn(II)-EDTA process delivered stronger activation and wider applicability, diminishing contaminant toxicity and resisting background interference. This study provides valuable insights into Fe(VI) activation induced by transition metal complexes and serves as a reference for selecting efficient strategies to avoid excessive consumption of oxidative capacity.
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高影响因子
WATER RESEARCH
·
2025
·
IF 12.4
Tianyi Luo,Xiaohu Dai,Yuting Zhang,Wei Wei,Bing-Jie Ni
Antibiotic resistance genes (ARGs) and antibiotic resistant bacteria (ARB) are emerging environmental contaminants that threaten public health, highlighting the urgent need for effective control strategies. Ferrate (Fe(VI)), a strong and eco-friendly oxidant, shows great potential for this purpose. This study systematically evaluated the efficacy of Fe(VI) in mitigating ARGs and ARB in anaerobically digested sludge, with a particular focus on elucidating the underlying mechanisms by which Fe(VI) effects ARGs dissemination through both vertical gene transfer (VGT) and horizontal gene transfer (HGT). Result shows that Fe(VI) doses of 20 and 60 mg/g-TS reduce ARGs by 9.75% and 19.12%, respectively, while inactivating up to 24.7% of ARB at the higher dose. Pathogenic ARB, such as Escherichia coli and Shigella sonnei, are preferentially removed, with abundances decrease by 63.7% and 28.0%. Mechanistically, the structural disruption of bacterial cells caused by Fe(VI) in anaerobically digested sludge, as indicated by a 29% reduction in extracellular polymeric substances and a 23.7% increase in cell membrane permeability. Subsequently, a marked release of intracellular ARGs into the extracellular environment is also observed, where they are likely subjected to degradation by Fe(VI). This oxidative killing accounts for the observed ARB decrease, thereby limiting the VGT of ARGs. In addition, Fe(VI) impairs the HGT of ARGs by diminishing their mobility potential, reflected in the reduced co-occurence with mobile genetic elements. Meanwhile, sludge bacterial competence for DNA uptake and recombination is markedly reduced, as evidenced by a 9.8% decline in the abundance of related functional genes. These findings demonstrate that Fe(VI) effectively inhibits the dissemination of ARGs by targeting both primary transmission pathways. It suppresses VGT, thereby reducing the inheritance of ARB within populations, and limits HGT, curbing the spread of mobile ARGs among competent species. By disrupting these two critical routes, Fe(VI) shows strong potential as an effective strategy for mitigating ARGs propagation in sludge systems.
研究领域:
环境微生物学
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分子生物学
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环境工程
·
抗性基因传播
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水处理技术
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DOI
PubMed
高影响因子
ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2021
·
IF 9.028
Shuchang Wang,Yang Deng,Binbin Shao,Jiahui Zhu,Zixin Hu,Xiaohong Guan
For the first time, this study showed that the apparent second-order rate constants (kapp) of six selected emerging organic contaminants (EOCs) oxidation by Fe(VI) increased, remained constant, or declined with time, depending on [EOC]0/[Fe(VI)]0, pH, and EOCs species. Employing excess caffeine as the quenching reagent for Fe(V) and Fe(IV), it was found that Fe(V)/Fe(IV) contributed to 20–30% of phenol and bisphenol F degradation by Fe(VI), and the contributions of Fe(V)/Fe(IV) remained nearly constant with time under all the tested conditions. However, the contributions of Fe(V)/Fe(IV) accounted for over 50% during the oxidation of sulfamethoxazole, bisphenol S, and iohexol by Fe(VI), and the variation trends of kapp of their degradation by Fe(VI) with time displayed three different patterns, which coincided with those of the contributions of Fe(V)/Fe(IV) to their decomposition with time. Results of the quenching experiments were validated by simulating the oxidation kinetic data of methyl phenyl sulfoxide by Fe(VI), which revealed that the variation trends of kapp with time were significantly determined by the change in the molar ratio of Fe(V) to Fe(VI) with time, highlighting the key role of Fe(V) in the oxidative process. This study provides comprehensive and insightful information on the roles of Fe(V)/Fe(IV) during EOC oxidation by Fe(VI).
研究领域:
环境科学
·
化学动力学
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DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Kunyu Chen,Zhanguo Cui,Zhiqiang Zhang,Heliang Pang,Jing Yang,Xiaojiang Huang,Jinsuo Lu
The present study developed a prolonged oxidizable sulfur(IV)/ferrate(VI) system for the generation of hydroxyl radical ( OH) and sulfate radical (SO 4 − ) within 120 min, and proposed a reaction mechanism. In the presence of H + in solution, the S(IV)/Fe(IV) system provided excellent oxidation performance of refractory organics O,O-dimethyl-S-methylcarbamoyl methyl phosphorothioate (dimethoate, a widely used organophosphorus pesticide) within 120 min. The degradation efficiency of dimethoate in the bisulfite/Fe(VI) system (e.g., 90.06% dimethoate) was higher than that in the sulfite/Fe(VI) system (e.g., 51.03% dimethoate), while Fe(VI) alone degraded 27.81% of dimethoate. In the S(IV)/Fe(VI) system, the active species consisted of Fe(VI) (including the highly-reactive iron-based intermediate species, i.e. Fe(V) and Fe(IV)), OH and SO 4 − , with OH being identified as the main active species, contributing more than half of the total. The degradation mechanism of dimethoate in the S(IV)/Fe(VI) system mainly included the cleavage of the S-P bond, C-S bond and the oxidation of the P = S bond. Two plausible degradation pathways were proposed based on the detected transformation products. Dimethoate could be efficiently degraded when the [bisulfite]/[Fe(VI)] molar ratio was 4:1 with a low Fe(VI) dosage (218 µM), the changes in HA and HCO 3 − concentrations affected the transformation of dimethoate, the presence of Cl − , SO 4 2− and NO 3 − had a negligible effect, and the S(IV)/Fe(VI) system performed well in real waters. The S(IV)/Fe(VI) system has excellent oxidation performance for the removal of organic pollutants in water, with a final pH (pH = 6.6) close to neutral and ultimate products of SO 4 2− and Fe(OH) 3 , which has great potential for engineering applications.
研究领域:
环境科学
·
水处理技术
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DOI
高影响因子
WATER RESEARCH
·
2025
·
IF 12.4
Xiao Luo,Yihan Li,Xiaoke Ma,Tapas Sen,Lin Zhao,Yongkui Yang,Peizhe Sun
The individual Fe(VI) as FeO 4 2- or peroxydisulfate (PDS) oxidation process faces challenges of limited oxidation efficiency, excessive dosage consumption, and a narrow pH range. Fe is an important component in both Fe(VI) oxidation and PDS activation. We propose linking Fe in the combined Fe(VI)/PDS process to address the challenges of their individual processes. The contribution of Fe species to reactive oxygen species (ROS) production in the Fe(VI)/PDS process and the regulatory effects of quinones on Fe species in the Fe(VI)/PDS-benzoquinone (BQ) process were investigated. The reactive oxidation species generated by the Fe(VI)/PDS process included high-valency iron species such as Fe(VI), Fe(V), and Fe(IV); hydroxy radicals (∙OH), singlet oxygen ( 1 O 2 ), and SO 4 ˙ˉ contributed differently at varying pH levels. PDS accelerated the conversion of Fe(VI) to Fe(V) and Fe(IV), which are more reactive, and facilitated their regeneration from Fe(III) and Fe(II). The Fe(II) concentration in the Fe(VI)/PDS process increased by 35.0% after BQ addition, which enhanced PDS activation and shifted the dominant oxidizer from high-valency iron to ROS. In the Fe(VI)/PDS-BQ process, norfloxacin underwent oxidative degradation via piperazinyl ring degradation, defluorination, and quinolone group degradation, as evidenced by degradation byproducts and further supported by density functional theory calculations. The Fe(VI)/PDS-BQ process significantly reduced the toxicity of norfloxacin. A novel Fe(VI)/PDS-BQ process was developed with the potential to eliminate antibiotics from water and to identify the Fe-involved oxidation mechanism regulated by BQ addition and pH.
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高影响因子
WATER RESEARCH
·
2023
·
IF 12.8
Bin Liu,Yin Jun,Changrong Zhao,Chu Zhou,Tingting Zhu,Senlin Shao
Ultrafiltration (UF) is a technology commonly used to treat secondary effluents in wastewater reuse; however, it faces two main challenges: 1) membrane fouling and 2) inadequate nitrogen (N), phosphorus (P), and organic micropollutants (OMPs) removal. To address these two issues, in this study, we applied peracetic acid (PAA), Fe(VI)/PAA, and Fe(II)/PAA as UF pretreatments. The results showed that the most effective pretreatment was Fe(II)/200 μM PAA, which reduced the total fouling resistance by 90.2%. In comparison, the reduction was only 29.7% with 200 μM PAA alone and 64.3% with Fe(VI)/200 μM PAA. Fe(II)/200 μM PAA could effectively remove fluorescent components and hydrophobic organics in effluent organic matter (EfOM), and enhance the repulsive force between foulants and membrane (according to XDLVO analysis), and consequently, mitigate pore blocking and delay cake layer formation. Regarding pollutant removal, Fe(II)/200 μM PAA effectively degraded OMPs (>85%) and improved P removal by 58.2% via in-situ Fe(Ⅲ) co-precipitation. The quencher and probe experiments indicated that Fe IV O 2+ , •OH, and CH 3 C(O)OO•/CH 3 C(O)O• all played important roles in micropollutant degradation with Fe(II)/PAA. Interestingly, PAA oxidation produced highly biodegradable products such as acetic acid, which significantly elevated the BOD 5 level and increased the BOD 5 /total nitrogen (BOD 5 /TN) ratio from 0.8 to 8.6, benefiting N removal with subsequent denitrification. Overall, the Fe(II)/PAA process exhibits great potential as a UF pretreatment to control membrane fouling and improve water quality during secondary effluent treatment.
研究领域:
环境科学
·
水处理工程
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DOI
PubMed
高影响因子
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