WATER RESEARCH
·
2026
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IF 12.4
Mengqiang He,Mingzhu Liu,Xiaolei Teng,Shengnan Zhang,Zunyao Wang,Xiaohong Guan,Ruijuan Qu
Phenolic pollutants, frequently detected in aquatic environments as trace-level mixtures, pose significant challenges for water treatment. In this study, we examined the removal of 35 trace phenol mixtures (0.1 μmol/L each) under Fe(VI) oxidation, revealing kinetic differences between single and mixed systems. Fast-reacting phenols with secondary reaction rate constant ( k app ) > 350 M −1 •s −1 experienced accelerated oxidation upon mixing, whereas slow-reacting ones ( k app ≤ 350 M −1 •s −1 ) exhibited decreased rates. The quantitative structure-activity relationship (QSAR) models were constructed to correlate the k app of these phenols with molecular descriptors, showing that higher E HOMO and lower E gap were conductive to increasing the reaction rate in the mixed system, while E LUMO had a minimal effect on the reaction. Employing molecular networking for non-targeted screening, we identified the prevalence of cross-polymerization within the mixed system, yielding various cross-polymer products. Reaction pathway analysis, TOC and COD measurements, and theoretical calculations collectively demonstrated that electrophilic attacks of Fe(VI) trigger electron loss in phenols, generating phenoxy radicals that drive cross-polymerization and accelerate reaction rates of fast-reacting phenols, aligning with QSAR model predictions. These findings can deepen our understanding of Fe(VI) oxidation mechanism on mixed trace phenols, offering valuable insights for the advancement of wastewater treatment technologies.
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PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Sheng Deng,Xu Han,Ningqing Lv,Xiaochun Yang,Qiyuan Liu,Yonghai Jiang,Yu Yang,Beidou Xi
Despite the widespread use of biochar as a heterogeneous catalyst in AOPs, there is still a need to clarify the activation mechanism of nitrogen-doped biochar on ferrate (Fe(VI)). The Fe(VI) activation was significantly enhanced by the nitrogen-doped biochar synthesized at 800 °C (BC N -800) in this research, resulting in improved degradation of carbamazepine. Characterizations showed that a honeycomb-like pore and channel structure was formed on the inner layer of modified biochar and the SSA and pore volume were increased five and two times respectively as the temperature raised to 800 °C. Numerous indications indicated that the main active oxidizers in the BC N -800/Fe(VI) system were the high Fe species, and subsequent examination unveiled that the incorporation of nitrogen resulted in decreased resistance to charge transfer and enhanced efficiency of electron transfer for the production of high Fe species. DFT calculation illustrated that the SET path in the BC N -800/Fe(VI) system was spontaneous and single-electron oxygen atom transfer was the primary path for generating more highly reactive Fe(V) species. Notably, the BC N -800 remains stable after the organic degradation reaction and the toxicity of the intermediates produced during degradation decreases. This research will not only establish a theoretical foundation for designing eco-friendly catalysts based on biochar but also boost the investigation of biochar's ecological impacts.
研究领域:
环境科学
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催化化学
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DOI
高影响因子
Journal of Environmental Sciences
·
2018
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IF 3.12
Tuqiao Zhang,Feilong Dong,Feng Luo,Cong Li
Sulfonamides are used in human therapy, animal husbandry and agriculture but are not easily biodegradable, and are often detected in surface water. Sulfamethazine (SMZ) and sulfadiazine (SDZ) are two widely used sulfonamide antibiotics that are used heavily in agriculture. In this study, they were degraded in an aqueous system by chlorination after pre-oxidation with ferrate(VI) (Fe VI O 4 2 − , Fe(VI)), an environmentally friendly oxidation technique that has been shown to be effective in degrading various organics. The kinetics of the degradation were determined as a function of Fe(VI) (0–1.5 mg/L), free chlorine (0–1.8 mg/L) and temperature (15–35°C). According to the experimental results, SMZ chlorination followed second-order kinetics with increasing Fe(VI) dosage, and the effect of the initial free chlorine concentration on the reaction kinetics with pre-oxidation by Fe(VI) fitted a pseudo-first order model. The rate constants of SDZ and SMZ chlorination at different temperatures were related to the Arrhenius equation. Fe(VI) could reduce the levels of THMs formed and the toxicity of the sulfonamide degradation systems with Fe(VI) doses of 0.5–1.5 mg/L, which provides a reference for ensuring water quality in drinking water systems.
研究领域:
环境科学
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水处理工程
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PubMed
高影响因子
JOURNAL OF MEMBRANE SCIENCE
·
2024
·
IF 8.4
Bin Liu,Danjing Lu,Tianliang Zhang,Yixun Shen,Zhen Qiu,Xin Mao,Ruoxi Wu
Landfill leachate, with its high concentrations of persistent organic pollutants, salts, heavy metals, and emerging contaminants, presents significant environmental challenges. This study investigated the combination of dielectric barrier discharge (DBD) and ferrate (Fe(VI)) pretreatment technology in landfill leachate treatment, focusing on its effectiveness in enhancing oxidation performance and mitigating membrane fouling. The results indicated that after DBD/Fe(VI) treatment, TOC and UV 254 removal efficiencies increased by 44 % and 67 %, respectively. Additionally, the DBD/Fe(VI) system excelled in removing fluorescent substances and high molecular weight organic compounds, thereby reducing the formation of the cake layer on the nanofiltration membrane. This system enhanced oxidation performance through the synergistic production of reactive intermediates, with Fe(V)/Fe(IV) and •OH being the main active species, O 2 •- , and 1 O 2 also contributing significantly. The degradation pathway of perfluorooctanoic acid was investigated by utilizing it as the representative pollutant. Compared to the raw landfill leachate system, the DBD/Fe(VI) increased membrane flux by 104 %, while reducing reversible and irreversible fouling resistances by 67 % and 75 %, respectively. Furthermore, the advantages and practical application potential of the DBD/Fe(VI) system were evaluated from energy consumption, economic cost, and carbon dioxide emissions. The study offers an innovative method for landfill leachate treatment and fouling mitigation.
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
Applied Sciences-Basel
·
2025
·Vol. 15
·期 11
·5945
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IF 2.5
Lia Wang,Xu He,Lan Liang,Yanshan Wang,Beibei Yan,Guanyi Chen,Ning Li,Li’an Hou
The conventional Fenton process generates large amounts of Fenton sludge during wastewater treatment. Achieving effective utilization of Fenton sludge and reducing its production remain pivotal challenges. In this study, Fenton sludge biochar catalysts (Cat) were prepared using Fenton sludge via pyrolysis. In addition, chemical oxygen demand (COD) from secondary effluent was removed by Fenton sludge biochar catalysts activated with H2O2/Fe(VI). Specifically, the removal efficiency of COD could reach 46.2% in the Cat−2/H2O2/Fe(VI) system under weakly alkaline conditions. The mechanistic analysis confirmed that high-valent iron,•OH, O2•−, and1O2all participate in the degradation process. Furthermore, a continuous-flow reactor was applied to treat secondary effluent, with COD decreasing from 65 mg/L to 36 mg/L. This study provides new insights into the resource utilization of Fenton sludge and the treatment of complex wastewater.
研究领域:
环境科学
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废水处理
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高影响因子
SCIENCE OF THE TOTAL ENVIRONMENT
·
2023
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IF 9.8
Feilong Dong,Chuyun Fu,Zhu Meng,Qiufeng Lin,Jinzhe Li,Tao Zeng,Da Wang,Juntao Tang,Shuang Song
Ferrate (Fe(VI)) has been extensively studied as a green oxidant to treat wastewater. But Fe(VI) oxidation still faces several challenges for application, such as the sensitivity of Fe(VI) to pH and the restrictions on the Fe(VI) utilization efficiency for pollutant elimination at low concentration levels. This study proposed a two-stage Fe(VI) oxidation process to enhance the bisphenol A (BPA) removal for potential applicability, consisting of the adsorption by CNTs of stage I and the degradation by Fe(VI) of stage II. The Fe(VI) utilization efficiency in the two-stage process (0.848) was higher than that in one-stage processes (0.727) and Fe(VI) alone system (0.504) at pH 9. In stage I, the adsorption process had good compliance with the Langmuir isotherm model and pseudo-second-order kinetic model. In stage II, the effective utilization of low-concentration Fe(VI) was 2.45 times more than Fe(VI) alone, and the reduction of reaction volume was beneficial to further enhance utilization. The probe experiments (sulfoxide) and the degradation experiments of other electron-donating/withdrawing pollutants (e.g., atrazine, benzoic acid) demonstrated that Fe(IV) and Fe(V) were major oxidizing species in the two-stage process. The regeneration experiments showed that CNTs still had acceptable adsorption and catalytic capabilities after five cycles. Finally, the intermediate products in the two-stage process were detected and four possible degradation pathways of BPA were proposed. These findings were meaningful for the practical application of Fe(VI) oxidation to overcome the conditional limitation and improve the utilization.
研究领域:
环境科学
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化学工程
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PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2024
·
IF 13.3
Muhan Sun,Xiaoxu Jiang,Rui Liu,Deqin Kong,Hao Wu,Zhao Wang,Gang Zheng,Chongmiao Zhang,Weihua Yu
Sewage effluent and reclaimed water usually contain elevated concentrations of bacteria-derived endotoxins, which may have serious public health implications upon exposure. Both conventional disinfection methods, such as chlorine, ultraviolet, and ozone disinfection, and the new potassium ferrate disinfection process have limited endotoxin removal capacity. Therefore, it is necessary to find new methods of removing endotoxins. In this study, we investigated the effects of ultraviolet/ferrate (UV/Fe(VI)) combination treatment on endotoxin elimination and inhalation hazard control. Our results indicate that UV or Fe(VI) alone cannot sufficiently eliminate endotoxins but can instead exacerbate endotoxin release during bacterial inactivation. However, the UV/Fe(VI) combination rapidly eliminated approximately 85.6 % of both pure and bacteria-derived endotoxins. The optimal conditions for this disinfection process were determined to be 10 mg/L of Fe(VI) and 160 μW/cm 2 of UV exposure for 15 min. Furthermore, the pH value, bicarbonate (HCO 3 – ), humic acid, and turbidity were determined as potential factors that may affect UV/Fe(VI)-mediated endotoxin removal in reclaimed water. The potential mechanism underlying UV/Fe(VI)-induced endotoxin degradation involves several strongly oxidizing species, among which Fe(IV)/Fe(V) is regarded as the primary contributor, followed by the superoxide anion ( • O 2 – ) and hydroxyl ( • OH) radicals. These active substances induce the breakdown of the endotoxin molecular structure into smaller, non-toxic fragments. Furthermore, pure endotoxins, Escherichia coli , and Pseudomonas aeruginosa were disinfected with UV/Fe(VI), and then these aerosolized samples were inhaled exposed to mice. Our results demonstrated that combined use of UV and Fe(VI), rather than administration alone, remarkably blunted bacterial- and endotoxin-induced lung injury. In conclusion, these results demonstrate that the UV/Fe(VI) approach successfully eliminates endotoxins and related inhalation hazards from reclaimed water.
研究领域:
环境科学
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公共卫生
·
微生物学
·
水处理
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高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2023
·
IF 13.6
Jia Zhao,Heng Zhang,Yang Shi,Mengfan Luo,Hongyu Zhou,Zhenjun Xie,Ye Du,Peng Zhou,Chuanshu He,Gang Yao,Bo Lai
Ferrate (Fe(VI)) has aroused great research interest in recent years due to its environmental benignancy and lower potential in disinfection by-product generation. However, the inevitable self-decomposition and lower reactivity under alkaline conditions severely restrict the utilization and decontamination efficiency of Fe(VI). Here, we discovered that Ru(III), a representative transition metal, could effectively activate Fe(VI) to degrade organic micropollutants, and its performance on Fe(VI) activation exceeded that of previously reported metal activators. The high-valent metal species (i.e., Fe(IV)/Fe(V) and high-valent Ru species) made a major contribution to SMX removal by Fe(VI)−Ru(III). Density functional theory calculations indicated the function of Ru(III) as a two-electron reductant, leading to the production of Ru(V) and Fe(IV) as the predominant active species. The characterization analyses proved that Ru species was deposited on ferric (hydr)oxides as Ru(III), indicating the possibility of Ru(III) as an electron shuttle with the rapid valence circulation between Ru(V) and Ru(III). This study not only develops an efficient way to activate Fe(VI) but also offers a thorough understanding of Fe(VI) activation induced by transition metals.
研究领域:
环境科学
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化学
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水处理
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PubMed
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2024
·
IF 12.2
Beibei Li,Ruijuan Qu,Ting Wang,Ruixue Guo,Jie Tian,Shuyi Li,Mostafa R. Abukhadra,Rehab Khaled Mahmoud,Zunyao Wang
In this investigation, we conducted a detailed analysis of the oxidation of 16 imidazole ionic liquid variants by Fe(VI) under uniform experimental setups, thereby securing a dataset of second-order reaction rate constants ( k obs ). This methodology ensures superior data consistency and comparability over traditional methods that amalgamate disparate data from varied studies. Utilizing 16 chemical structural parameters obtained via Density Functional Theory (DFT) as descriptors, we developed a Quantitative Structure Activity Relationship (QSAR) model. Through rigorous correlation analysis, Principal Component Analysis (PCA), Multiple Linear Regression (MLR), and Applicability Domain (AD) evaluation, we identified a pronounced negative correlation between the molecular orbital gap energy ( E gap) and k obs . MLR analysis further underscored E gap as a pivotal predictive variable, with its lower values indicating heightened oxidative reactivity towards Fe(VI) in the ionic liquids, leading the QSAR model to achieve a predictive accuracy of 0.95. Furthermore, we integrated an advanced machine learning approach - Random Forest Regression (RFR), which adeptly highlighted the critical factors influencing the oxidation efficiency of imidazole ionic liquids by Fe(VI) through elaborate decision trees , feature importance assessment, Recursive Feature Elimination (RFE), and cross-validation strategies. The RFR model demonstrated a remarkable predictive performance of 0.98. Both QSAR and RFR models pinpointed E gap as a key descriptor significantly affecting oxidation efficiency, with the RFR model presenting lower root mean square errors , establishing it as a more reliable predictive tool. The application of the RFR model in this study significantly improved the model's stability and the intuitive display of key influencing factors, introducing promising advanced analytical tools to the field of environmental chemistry .
研究领域:
环境化学
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计算化学
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PubMed
高影响因子
Desalination and Water Treatment
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2024
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IF 1
Debo Wu,Xingmin Gao,Shuiping Yang,Winston Duo Wu
Sequential removal of phenol and As(V) from co-contaminated water by ferrate (Fe(VI)) was investigated. The results showed that a neutral pH condition favored the sequential of phenol and As(V) by Fe(VI). Around 70% of phenol was removed at neutral pHs with a Fe(VI): phenol molar ratio of 10:1. While about 50% of As(V) was finally removed under similar conditions. The presence of a high concentration of Cl – (up to 0.2 M) showed 6% inhibitory effect on the final removal percentage of phenol compared to that without Cl – . Fourier transform infrared spectroscopy, X-ray powder diffraction, and X-ray photoelectron spectroscopy analyses suggested that As(V) was removed through adsorption by the precipitates (amorphous iron (oxy)hydroxide), while phenol was removed via degradation (89%) and adsorption (11%), respectively. Removal of As(V) occurred immediately when phenol degradation was initiated, indicating a rapid generation of Fe(III)- (oxy)hydroxide. Our study also revealed that an excessive amount of Fe(III) ions in the aqueous phase did not facilitate the degradation of phenol. On the other hand, improving the precipitation rate of Fe(III) could further improve the removal efficiency of phenol and As(V).
研究领域:
环境化学
·
水处理
·
污染物修复
·
氧化过程
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DOI
高影响因子
CHEMOSPHERE
·
2020
·
IF 5.778
Jinsuo Lu,Zhanguo Cui,Xiaoyong Deng,Zhijie Liang,Shouning Chai,Junyu Fan,Zhiqiang Zhang,Zhiwei Zhao
Ferrate (Fe(VI)) is usually effective for oxidizing a variety of organic pollutants within a few seconds, but some recalcitrant asorganophosphorus pesticides such as dimethoate require higher dose of Fe(VI) and inorganic phosphorus produced by mineralization is difficult to remove. In this study, acid-activated ferrate (Fe(VI)) was firstly used to degrade organophosphorus pesticides dimethoate and simultaneously remove total phosphorus (TP) from solution under simulated sunlight. At a Fe(VI):dimethoate molar radio of 15:1, dimethoate was almost completely removed within 20 min and 47% of TP in the solution was removed by the reduction product of Fe(VI) within 240 min. Electron paramagnetic resonance (EPR) and terephthalic acid (TA) fluorescence experiments showed that •OH radicals were continuously generated in the system, and •OH formation pathway was proposed. Importantly, the involvement of •OH in acid-activated Fe(VI) process was confirmed for the first time by EPR. In the acid-activated Fe(VI)/simulated sunlight system, the removal of dimethoate and TP gradually increased with the decrement of activation pH, whereas the increase of molar ratio of Fe(VI):dimethoate enhanced the removal of dimethoate and TP. The addition of inorganic anions (HCO 3 - and NO 2 - ) had obvious inhibitory effects on dimethoate and TP removal. Eight degradation products including O,O,S-trimethylphosphorothiate, omethoate and 2- S -methyl-(N-methyl) acetamide were determined by gas chromatography mass spectrometry (GC-MS) analysis, and two possible degradation pathways were proposed. The insights gained from this study open a new avenue to simultaneously degrade and remove organic contaminants .
研究领域:
环境科学
·
污染控制
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DOI
PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Zhengming He,Cong Li,Jingzhen Su,Kai Zhang,Jiaxue zhu,Ren Cai,Yunshu Zhang,Jieming Yuan,Xiaohong Guan
Iron-based catalysts are generally used to activate oxidizing species, such as hydrogen peroxide by increasing homogeneous active substances like free radicals, to promote the degradation of organic matter. However, less attention has been paid to the reactions on the surface or the generation of heterogeneous metal-oxo species. Herein, oxygen vacancies (Vo) were introduced into Fe oxides by a calcination-induced hetero-atom doping modification. The characteristic peak of the heterogeneous hypervalent iron-oxo [≡Fe IV =O] species in the UV–Vis spectrum at 371 nm was observed. In the context of electrochemical experiment, Vo-rich Mn-Fe 2 O 3 significantly enhanced the electron conduction of sulfamethoxazole and H 2 O 2 , while simultaneously inhibiting the self-decomposition of potassium ferrate (Fe(VI)). Regarding the H 2 O 2 generated during the self-decomposition process of Fe(VI), Vo-rich Mn-Fe 2 O 3 can accelerate the degradation of sulfamethoxazole, increasing the reaction rate to 0.1081 min −1 (with a 30.05 % improvement in removal efficiency). Density functional theory calculations indicate that Vo leads to an enhanced capture of O atoms by the low-coordinated Fe atoms, promoting the anchoring of H 2 O 2 and the formation of the active ≡Fe IV =O with a higher spin state. This work proposes heterogeneous reactive species on the surface of metal oxidase, constructing Vo as the O atom capture sites in iron-based oxides to facilitate the formation of ≡Fe IV =O and the degradation of organic compounds.
研究领域:
环境化学
·
催化科学
·
材料化学
·
环境污染与控制
·
物理化学
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高影响因子
危险品化学品经营许可证（带存储）