ENVIRONMENTAL SCIENCE & TECHNOLOGY
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2018
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IF 6.653
Jing Chen,Nannan Wu,Xinxin Xu,Ruijuan Qu,Chenguang Li,Xiaoxue Pan,Zhongbo Wei,Zunyao Wang
Potassium ferrate [Fe(VI)] is a promising oxidant widely used in water treatment for the elimination of organic pollutants. In this work, the reaction kinetics, products, and mechanisms of the antimicrobial agent chlorophene (CP) undergoing Fe(VI) oxidation in aqueous solutions were investigated. CP is very readily degraded by Fe(VI), with the apparent second-order rate constant, k, being 423.2 M–1 s–1 at pH 8.0. A total of 22 oxidation products were identified using liquid chromatography–quadrupole time-of-flight–mass spectrometry , and their structures were further elucidated using tandem mass spectrometry. According to the extracted peak areas in mass spectra, the main reaction products were the coupling products (dimers, trimers, and tetramers) that formed via single-electron coupling. Theoretical calculations demonstrated that hydrogen abstraction should easily occur at the hydroxyl group to produce reactive CP· radicals for subsequent polymerization. Cleavage of the C–C bridge bond, electrophilic substitution, hydroxylation, ring opening, and decarboxylation were also observed during the Fe(VI) oxidation process. In addition, the degradation of CP by Fe(VI) was also effective in real waters, which provides a basis for potential applications.
研究领域:
环境科学
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化学
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产品关联
DOI
PubMed
高影响因子
ENVIRONMENTAL POLLUTION
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2019
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IF 5.714
Afzal Ahmed Dar,Jing Chen,Asam Shad,Xiaoxue Pan,Jiayi Yao,May Bin-Jumah,Ahmed A. Allam,Zongli Huo,Feng Zhu,Zunyao Wang
In this study, the degradation of eight bromophenols (BPs), including monobromophenols (2-BP, 3-BP, and 4-BP), dibromophenols (2,4-DBP, 2,6-DBP, and 3,5-DBP), a tribromophenol (2,4,6-TBP) and a pentabromophenol (PBP), by a Fe(VI) reaction process at a pH of 8.0 was systematically studied. It was concluded that their degradation rates increased with increasing Fe(VI) concentrations in solution. The removal of 2,4,6-TBP, 2-BP, and 2,6-DBP was faster than that of the other five BPs, which could be attributed to the position of the substituting Br atom. Moreover, the direct oxidation and coupling reactions greatly influenced the reactivity of the bromophenols with Fe(VI). The electron paramagnetic resonance (EPR) analysis confirmed the presence of hydroxyl radicals in present system. The oxidation reaction products of PBP and 2-BP were recognized by an electrospray time-of-flight mass spectrometer ; hydroxylation, hydroxyl substitution, the cleavage of the C–C bond, direct oxidation and polymerization via an end linking mechanism were noticeably found in the reaction process, resulting in the formation of polymerization products and causing hydroxylation to occur. Theoretical calculations further determined the possible oxidation sites of 2-BP and PBP. This study may provide comprehensive and important information on the remediation of BPs by Fe(VI).
研究领域:
环境科学
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化学
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DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Xiaoxue Pan,Fengtao Sun,Min Wang,Hong Sun,Rui Zhang,Mingbao Feng,Xuesheng Zhang
Synthetic phenolic antioxidants (SPAs) have been commonly used in industrial and domestic products to prevent the adverse effects of oxidants such as oxygen. However, attention to the removal of SPAs is scarcely attracted. In this paper, the removal kinetics, influencing factors, transformation mechanisms and toxicity in Fe(VI) oxidation of 18 SPA congeners were investigated in detail. Results showed that propyl gallate (PG), butylated hydroxyanisole (BHA), and tert -butylhydroquinone (TBHQ) had the highest reactivities with Fe(VI), while the reaction rate constant ( k app ) value of 2,4-di- tert -butylphenyl 3,5-di- tert -butyl-4-hydroxybenzoate (UV120) was the lowest (221.3 M −1 s −1 ). A robust quantitative structure–activity relationship (QSAR) model between k app and molecular structural descriptors of SPAs was established. The energy gap between the lowest unoccupied molecular orbital ( E LUMO ) and the highest occupied molecular orbital ( E HOMO ) was a vital parameter to determine the removal efficiencies of the SPA congeners. Furthermore, the numbers of oxygen atoms and alkyl groups in SPA structures also determined their reactivities with Fe(VI) to some extent. In addition, aqueous 2,6-di- tert -butyl-4-methylphenol (BHT, a representative of SPAs) could be efficiently removed with the increased amount of oxidant, and decreased substrate concentration and slightly alkaline conditions. Seventeen intermediates were identified, and oxidation routes including H-abstraction, single- and double-oxygen(s) transfer, and coupling were deduced. However, H-abstraction inevitably led to the generation of BHT-Q with higher toxicity than parent. These findings provide novel insights into the production and removal of SPA analogs.
研究领域:
环境科学
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化学
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毒理学
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DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
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2023
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IF 13.6
Jinzhe Li,Chuyun Fu,Qiufeng Lin,Tao Zeng,Da Wang,Xinwen Huang,Shuang Song,Cong Li,Feilong Dong
Ferrate (Fe(VI), FeO 4 2- ) has been widely used in the degradation of micropollutants with the advantages of high redox potential , no secondary pollution and inhibition of disinfection byproducts . However, the low transformation of Fe(V) and/or Fe(IV) by Fe(VI) and incomplete mineralization of pollutants limit their application. In this work, we designed a photo electric cell with TiO 2 nanotubes (TNTs) and Pt serving as the anode and cathode to enhance the utilization of Fe(VI) (Fe(VI)-TNTs system). TNTs accelerated the generation of •OH via h VB + oxidation of OH - and photogenerated electrons at Pt boosted the transformation of Fe(VI) to Fe(V) and/or Fe(IV), resulting in a 22.2 % enhancement of chloroquine (CLQ) removal compared to Fe(VI) alone. The results from EPR and quenching tests showed that Fe(VI), Fe(V), Fe(IV), •OH, O 2 •- and h VB + coexisted in the Fe(VI)-TNTs system, among which Fe(V) and Fe(IV) were testified as the primary reactive substances accounting for 59 % of CLQ removal. The performance tests and recycling tests demonstrated that the Fe(VI)-TNTs system maintained excellent performance in an authentic water environment. The plausible degradation pathway of CLQ oxidized in the Fe(VI)-TNTs system was proposed with nine identified oxidation products via N-C cleavage, electrophilic addition and carboxylation processes. Based on the ECOSAR calculation, the constructed reaction system allowed a decrease in acute and chronic toxicity. Our findings provide a highly efficient and cost-effective strategy to enhance Fe(VI) application for micropollutant degradation in the future.
研究领域:
环境科学
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化学工程
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材料科学
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产品关联
DOI
PubMed
高影响因子
Journal of Water Process Engineering
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2025
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IF 6.7
Yang Song,Shibin Zhang,Haoxin Shen,Wen Qin,Jin Jiang,Jun Ma
In this study, calcium hypochlorite (Ca(ClO) 2 ) combined with potassium ferrate (Fe(VI)) (Ca(ClO) 2 /Fe(VI)) oxidation system was developed to enhance the stability of Fe(VI) and removal efficacy of emerging contaminants. For the removal of micropollutants with various moieties, carbamazepine (CBZ) and phenol removals (50 % and 35 %) in the initial stage were enhanced by Ca(ClO) 2 /Fe(VI) oxidation system, which were primarily attributed to the Ca(ClO) 2 enhanced micropollutant removal by stabilizing Fe(VI) through H 2 O 2 scavenging in the Ca(ClO) 2 /Fe(VI) system, increasing Fe(VI) exposure to boost direct degradation efficiency for Fe(VI)-reactive contaminants (CBZ or phenol), but showed limited efficacy for ClO − reactive pollutants (SMX), because the reaction of Ca(ClO) 2 with SMX was more favorable than that of Fe(VI) with SMX. The microplastics (MPs) removal achieved by the Ca(ClO) 2 /Fe(VI) oxidation system (86 %) was also higher than the sum values (65.69 %) achieved by each individual reactant, indicating the synergy of Ca(ClO) 2 and Fe(VI) could enhance coagulation and improve the removal efficiency of microplastics. Moreover, the UV 254 , electron-donating capacity (EDC), and turbidity removals by Ca(ClO) 2 /Fe(VI) oxidation system from simulated source water (36 %, 53 % and 32 %) and real source water (48 %, 86 % and 53 %) were higher than those by Fe(VI) alone (26 %, 43 % and 21 %). This study provided novel insights into optimizing Fe(VI)-based systems applied for pre-oxidation process in drinking water treatment.
研究领域:
环境科学
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水处理技术
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化学工程
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环境工程
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产品关联
DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
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2019
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IF 7.65
Binbin Shao,Hongyu Dong,Liying Feng,Junlian Qiao,Xiaohong Guan
Although several groups have made efforts to study micropollutants degradation by Fe(VI)/sulfite process, the mechanism is far from clear and warrants further investigation. Herein, the degradation kinetics and mechanism of selected micropollutants by sulfite (SO 3 2− )-activated Fe(VI) oxidation were systematically investigated. The oxidation rates of enrofloxacin (ENR) and phenol in Fe(VI)/sulfite process ranged from 0.151 s −1 to 6.18 s −1 at pH 6.5 and 8.0. Sulfite applied in multiple-addition mode improved the degradation efficiency of micropollutants with electron-rich moieties compared to the single-addition mode. Based on results of the quenching experiments and kinetic simulation, Fe(V) was identified as the predominant active oxidant at [SO 3 2− ]/[Fe(VI)] molar ratio of 0.1 to 0.3. However, both Fe(V) and SO 4 − / OH contributed to micropollutants oxidation at [SO 3 2− ]/[Fe(VI)] molar ratio ≥ 0.4 and their contributions were strongly dependent on the properties of micropollutants. The different degradation products of ENR in Fe(VI)/sulfite process at different sulfite dosages further supported the contribution of different active oxidants at different [SO 3 2− ]/[Fe(VI)] molar ratios. The toxicity of the reaction products of ENR towards Vibrio qinghaiensis sp.-Q67 decreased dramatically after Fe(VI)/sulfite treatment. The results of this work may promote the application of sulfite-activated Fe(VI) oxidation in water treatment.
研究领域:
环境科学
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化学工程
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
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2024
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IF 12.2
Xiaoyu Fu,Jingfeng Gao,Qian Wang,Hao Chen,Ying Liu,Liqin Zeng,Yukun Yuan,Hongxin Xu
The existence of antibiotic resistant bacteria (ARB) and antibiotic resistance genes (ARGs) has been a global public environment and health issue. Due to the different cell structures, gram-positive/negative ARB exhibit various inactivation mechanisms in water disinfection. In this study, a gram-negative ARB Escherichia coli DH5α ( E. coli DH5α) was used as a horizontal gene transfer (HGT) donor, while a gram-positive ARB Bacillus as a recipient. To develop an efficient and engineering applicable method in water disinfection, ARB and ARGs removal efficiency of Fe(VI) coupled peroxydisulfate (PDS) or peroxymonosulfate (PMS) was compared, wherein hydroxylamine (HA) was added as a reducing agent. The results indicated that Fe(VI)/PMS/HA showed higher disinfection efficiency than Fe(VI)/PDS/HA. When the concentration of each Fe(VI), PMS, HA was 0.48 mM, 5.15 log E. coli DH5α and 3.57 log Bacillus lost cultivability, while the proportion of recovered cells was 0.0017 % and 0.0566 %, respectively, and HGT was blocked. Intracellular tetA was reduced by 2.49 log. Fe(IV) and/or Fe(V) were proved to be the decisive reactive species. Due to the superiority of low cost as well as high efficiency and practicality, Fe(VI)/PMS/HA has significant application potential in ARB, ARGs removal and HGT inhibition, offering a new insight for wastewater treatment.
研究领域:
环境科学
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微生物学
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产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Jianchao Wang,Chunhui Wang,Zikun Cheng,Chenshuo Wang,Dongbei Yue,Hui Wang,Hongru Jiang,Bo Jiang,Lingyue Zhang
Plastic recycling is a promising technology, as it can both contribute to circular economy goals and reducing plastic pollution; however, it faces significant challenges due to the lack of effective separation methods. Herein, we studied the flotation separation of polycarbonate (PC), a major component of plastic waste, from multi-plastic mixtures after hydrophilization by Fe(VI). First, the effect of Fe(VI) treatment on the surface properties of the plastics was studied. Fe(VI) induced hydrophilization of PC, with a decreased contact angle of about 19°; this was attributed to the introduction of hydrophilic moieties by surface oxidation and hydrolysis reactions. Then, the effect of operating conditions in both hydrophilization and flotation on the flotability of plastics was investigated. In both binary and multi-plastic mixtures, hydrophilization selectively suppressed the flotability of PC from 100% to about 0.0%. Numerical simulation was performed using the population balance model of computational fluid dynamics to determine the gas-liquid flows during flotation. It was found that the flow rate affected flotation of plastics via bubble formation rather than flow fields. Finally, the optimization of hydrophilization was performed using the Box Behnken design of response surface methodology. The results showed that PC was separated from multi-plastic mixtures with recovery and purity of 100.0% under the optimum conditions. These results would greatly facilitate the development of plastic recycling.
研究领域:
环境科学
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材料科学
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产品关联
DOI
高影响因子
Biomed Research International
·
2015
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IF 1.579
Yan Ma,Kejia Zhang,Cong Li,Tuqiao Zhang,Naiyun Gao
The photocatalytic degradation of sulfonamides in aqueous TiO2 suspension under UV irradiation has been investigated using potassium ferrate as electron acceptors. The results showed that the stability of Fe(VI) is dependent on pH significantly, and the stability reduces obviously in the presence of UV-TiO2. The experiments indicated that Fe(VI) could effectively scavenge the conduction band electrons from the surface of TiO2. The photocatalytic oxidation of sulfonamides with Fe(VI) was found to be much faster than that without Fe(VI). The SD, SM, and SMX concentration was greatly reduced by 89.2%, 83.4%, and 82.0%, respectively, after 10 min with UV-TiO2-Fe(VI), comparing to 65.2%, 66.0%, and 71.9%, respectively, with Fe(VI) only in the dark and 71.3%, 72.7%, and 76.0%, respectively, with UV-TiO2. The pH value of solution significantly influenced the sulfonamides degradation in UV-TiO2-Fe(VI) system. The degradation amount of sulfonamides after 10 min was a maximum at pH 7. The intermediate products of sulfonamides oxidation by UV-TiO2-Fe(VI) were analysed by LC-HESI-MS-MS and the results suggested that a majority of sulfonamides turned into large-molecule products without complete mineralization.
研究领域:
环境科学
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化学
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产品关联
DOI
PubMed
高影响因子
ACS ES&T Water
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2023
·
IF 5.3
Shangying Li,Renji Zheng,Yuanhao Zhou,Shimao Deng,Siyuan Luo,Ranhao Wang,Xuezhen Feng,Hong Chen
Heavy metal–organic complexes widely distributed in wastewater are hazardous and urgently need to be removed and recycled. Herein, copper glycinate (CuGly) was employed as a model complex and removed with the environmentally friendly oxidant ferrate(VI) (Fe(VI)). We found that Fe(VI) can be used to effectively remove CuGly and recycle Cu via a decomplexation–degradation–immobilization coupled pathway, i.e., decomplexing CuGly, degrading organic ligands, and immobilizing the released Cu ions. Theoretical calculation results revealed that CuGly was favored to be oxidized by Fe(VI), and the CuGly decomplexation and organic ligand degradation could spontaneously thermodynamically proceed at room temperature. Although different active oxidation species, including Fe(V), Fe(IV), H2O2, and •OH, are present during the Fe(VI) decomposition process, control experiments suggested that Fe(VI), Fe(V), and Fe(IV), rather than H2O2 and •OH, played critical roles in CuGly removal. The resultant Fe and Cu precipitate could be further converted to a magnetic composite material, which could be used as a catalyst for antibiotic degradation. This study presents an effective strategy and the comprehensive underlying mechanisms of synergistic heavy metal–organic complex removal and metal resource recycling using ferrate, which could be extended to green chemical treatment of heavy metal–organic complexes in various wastewater bodies.
研究领域:
环境科学
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化学工程
·
水处理
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产品关联
DOI
高影响因子
ACS Omega
·
2019
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IF 2.584
Jinjuan Xue,Zhengrong Zhu,Yuqing Zong,Chengjuan Huang,Mingxin Wang
This study investigates the degradation of dimethyl phthalate (DMP) with hydrogen peroxide and ferrate (Fe(VI)) under various reaction conditions. The results showed that the optimum conditions for dimethyl phthalate removal from water were as follows: (a) pH 7.0 and (b) the original molar ratio of [Fe(VI)]/[H2O2]/[DMP] equal to 10:2:1. Under the optimum conditions, the degradation rate of DMP can reach 89.7% in 360 min. Furthermore, 2,5-dihydroxybenzaldehyde, isophthalic acid, 2-ethylhexanol, oxalic acid, 2,6-dihydroxybenzoic acid, 2,6-dihydroxybenzaldehyde, 2,5-dihydroxybenzoic acid, and monomethyl phthalate were identified as the degradation intermediates, and degradation pathways were proposed.
研究领域:
环境化学
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水处理
·
高级氧化过程
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DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2026
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IF 9.1
Xiaoyuan Zhang,Rui Zeng,Zhenbei Wang,Fei Qi,Chen Li,Yatao Liu,Fan Li,Ziteng Chen,Yujia Yuan,Zhuoran Bai,Yongshun Yu,Jun Nan,Amir Ikhlaq,Shengnan Li
The potential of Fe(VI) enhanced coagulation-ultrafiltration (C-UF) for the simultaneous enhancement of ibuprofen (IBP) removal and membrane alleviation was investigated by comparing Fe(VI)-UF, FeCl 3 -UF, AlCl 3 -UF, Fe(VI)-FeCl 3 -UF, and Fe(VI)-AlCl 3 -UF. The results showed that Fe(VI)-FeCl 3 -UF and Fe(VI)-AlCl 3 -UF achieved IBP removal efficiencies of 66.6% and 76.9%, respectively, which were significantly higher than those obtained with Fe(VI)-UF, FeCl 3 -UF, AlCl 3 -UF. This confirmed that Fe(VI) enhanced C-UF could effectively improve IBP removal compared to individual Fe(VI)-UF or conventional C-UF. This improvement was attributed to additional highly reactive Fe(V)/Fe(IV) intermediates generated by adding metal coagulants to instantaneously activate residual Fe(VI) during the Fe(VI) enhanced C-UF process. In addition, Fe(VI)-FeCl 3 -UF and Fe(VI)-AlCl 3 -UF further alleviated total membrane fouling compared to FeCl 3 -UF and AlCl 3 -UF, with a significant shift of membrane fouling toward reversible fouling. Floc properties, NOM characteristics, and membrane surface characterization were comprehensively analyzed to reveal membrane fouling alleviation mechanisms in Fe(VI) enhanced C-UF. Simultaneous cleavage into smaller molecules and polymerization into larger fractions of NOM by Fe(VI) could reduce the affinity of foulants for membrane surface adsorption and consequently lower irreversible fouling. While Fe(VI) reduction would produce iron-based hydroxides to participate in the growth process of flocs, leading to the formation of flocs with higher density. These flocs would accumulate on membrane surface to form a denser cake layer, which contributed to severe membrane fouling.
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产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）