WATER AIR AND SOIL POLLUTION
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2022
·Vol. 233
·期 6
·1-10
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IF 2.984
Xu Ying,Zhou Zhengwei,Xue Yingang,Wu Jun
Synthetic musks (SMs), as a group of pharmaceutical and personal care products (PPCPs), have been widely detected in the environment at ng L −1 ~ μg L −1 levels and require our serious attention regarding their presence, toxicity and treatment technologies. In this study, ferrate (Fe 2 O 4 2− , Fe(VI)) was employed to treat two typical SMs, galaxolide (HHCB) and tonalide (AHTN), in water solutions. The treatment efficiencies of trace level HHCB and AHTN compounds (16 μg L −1 each) in individual and mixed solutions by Fe(VI) (0–45 mg L −1 as Fe) at pH 5.5–8.5 were assessed, and oxidation products of both compounds were also investigated by means of solid phase extraction coupled with gas chromatography-mass spectrometry (SPE-GC–MS). Results demonstrated that Fe(VI) was more suitable to remove HHCB than AHTN from test solutions. Specifically, when solution pH was 6.5 and Fe(VI) dose was 15–18 mg L −1 as Fe, the removal efficiencies of HHCB and AHTN in individual test solutions were up to 60% and 40%, respectively. Comparatively, much higher Fe(VI) doses were required (up to 38 mg L −1 as Fe) in order to achieve considerable removal efficiencies of both compounds in mixed test solutions. Solution pH played an important role and neutral conditions would benefit the removal of both compounds. In addition, several oxidation products (OPs) of both HHCB and AHTN were identified, and degradation pathways were then tentatively proposed. Finally, engineering aspects of Fe(VI) technology in full-scale water treatment applications were also discussed.
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
JOURNAL OF HAZARDOUS MATERIALS
·
2023
·
IF 13.6
Wen-Yuan Fan,Xin Zhang,Pu-Can Guo,Guo-Ping Sheng
Phosphonates, as a kind of important organic phosphorus in wastewater, should be removed in terms of their environmental risks. Unfortunately, traditional biological treatments fail to remove phosphonates effectively due to their biological inertness. The reported advanced oxidation processes (AOPs) usually require pH adjustment or coupling with other technologies to achieve high removal efficiency. Thus, a simple and efficient method for phosphonate removal is urgently needed. Herein, ferrate was found to remove phosphonates effectively in one-step under near-neutral circumstances by coupling oxidation and in-situ coagulation. Nitrilotrimethyl-phosphonic acid (NTMP), a typical phosphonate, could be efficiently oxidized by ferrate to release phosphate. The fraction of phosphate release increased with increasing ferrate dosage and reached 43.1% when 0.15 mM ferrate was added. Fe(VI) was responsible for NTMP oxidation, while Fe(V), Fe(IV) and ⋅OH played a minor role. Ferrate-induced phosphate release facilitated total phosphorus (TP) removal, because the phosphate is more easily removed via ferrate-resultant Fe(III) coagulation than the phosphonates. The coagulation removal of TP could reach up to 90% within 10 min. Furthermore, ferrate exerted high removal efficiencies for other commonly used phosphonates with approximately or up to 90% TP removal. This work provides a one-step efficient method to treat phosphonate-containing wastewaters.
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
SCIENCE OF THE TOTAL ENVIRONMENT
·
2023
·
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
JOURNAL OF HAZARDOUS MATERIALS
·
2022
·
IF 14.224
Mengfan Luo,Heng Zhang,Peng Zhou,Jiali Peng,Ye Du,Zhaokun Xiong,Bo Lai
The sluggish oxidation kinetics of ferrate (Fe(VI)) at neutral and slightly alkaline pH impedes its rapid abatement of micropollutants in practical application. This work discovers that graphite (GP), a metal-free carbonaceous material , can be a promising material to improve the reactivity of Fe(VI) in the pH range of 7.0 − 9.0. The performance of the GP/Fe(VI) process for sulfamethoxazole (SMX) removal was further evaluated via altering the dosages of Fe(VI), GP, and SMX. Probe analysis and quenching experiments identified Fe(IV) and Fe(V) as the primary active species responsible for the removal of organic compounds in the GP/Fe(VI) system. The detailed activation mechanism of GP is discussed via analyzing the surface chemical changes of GP exposed to Fe(VI). It is found that the carbonyl groups on GP surface execute a critical role in Fe(VI) activation. The GP/Fe(VI) system shows powerful anti-interference ability to environmental background substances. Therefore, the new oxidation process proposed in this work holds a great application prospect for contamination remediation. Finally, we discuss the underlying degradation pathways of SMX by the GP/Fe(VI) system. This study not only develops a promising system for the removal of micropollutants but also provides an in-depth insight into the activation mechanism of metal-free carbonaceous material in Fe(VI) oxidation process.
研究领域:
环境科学
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化学
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2017
·
IF 6.216
Yulei Liu,Lu Wang,Zhuangsong Huang,Xianshi Wang,Xiaodan Zhao,Yuanyuan Ren,Shaofang Sun,Mang Xue,Jingyao Qi,Jun Ma
Indole is a typical fecal odor compound and has negative impact on water quality at low concentrations. Here, the oxidation of indole by ferrate [Fe(VI)] was investigated, in terms of the reaction kinetics, the oxidation products, and the variation of assimilable organic carbon (AOC). The oxidation of indole was pH-dependent (6.0–9.5), and the pH-dependent profile could be well explained by the acid-base equilibrium of Fe(VI). The apparent second-order rate constants (k app ) for indole oxidation with Fe(VI) ranged from 692 ± 26 M −1 s −1 at pH 6.0 to 3.08 ± 0.15 M −1 s −1 at pH 9.5. The results of experiments conducted under real source water background showed that indole could be effectively removed by Fe(VI) from actual polluted waters. After analyzing the reaction pathway, it was found that the initial steps in the oxidation of indole were the hydroxylation of indole to 2,3-dihydroxyindole, followed by the cleavage of N-heterocyclic ring. Formanilide was a major oxidation product in this process, and it is less reactive with Fe(VI) than that of indole. High concentrations of Fe(VI) could effectively oxidize indole in the water and has little impact on the microbiological stability of the treated water. Based on the results, Fe(VI) can be an effective agent for the control of indole in water treatment.
研究领域:
环境科学
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化学工程
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高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2017
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IF 3.359
Junfeng Zhao,Yiqing Liu,Qun Wang,Yongsheng Fu,Xiaohui Lu,Xiaofeng Bai
In this study, the effect of phosphate, Fe(III), Fe(II), and reductive substances (i.e., Mn 2+ and SO 3 2− ) on diclofenac (DCF) oxidation and its degradation mechanism by Ferrate (Fe(VI)) were investigated. The removal rate of DCF in reaction solution at pH 9.0 adjusted by NaOH (67.36%) was higher than that by phosphate buffer (14.87%) because of the complexation of phosphate with Fe(III) and/or Fe(II) restraining the self-catalysis of Fe(VI). Fe(III) or Fe(II) could significantly catalyze Fe(VI) to generate more intermediates (i.e., Fe(V) and Fe(IV)), whose oxidation capacity was magnitude stronger than that of Fe(VI), leading to the improvement of DCF degradation, besides, the presence of reductive substances, e.g., Mn 2+ and SO 3 2− , could also increase the self-catalysis of Fe(VI), enhancing the removal of DCF, which will be further verified in follow-up studies. Seven oxidation products (OPs) were detected using a quadrupole-time of flight-mass spectrometer coupled with an ultra performance liquid chromatograph (LC-QTOF/MS). Based on these identified OPs, the potential degradation mechanism of DCF by Fe(VI) was proposed showing six reaction pathways, including hydroxylation, decarboxylation, C N bond cleavage, dehydrogenation, formylation, and dechlorination-hydroxylation. This study suggests that Fe(VI) can effectively oxidize and degrade DCF.
研究领域:
环境科学
·
化学
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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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PubMed
高影响因子
SCIENCE OF THE TOTAL ENVIRONMENT
·
2021
·
IF 7.963
Kanming Wang,Ji Shu,Virender K. Sharma,Cong Liu,Xiping Xu,Nasri Nesnas,Hongyu Wang
Imidacloprid (IMI), an emerging pollutant, has high toxicity to non-target organisms. This paper presents the kinetics of IMI removal by ferrate(VI) at different pH (6.0–9.0), molar ratios ([ferrate(VI)]:[IMI]) and added Fe(III) ions. The apparent second-order rate constant ( k app ) decreased with increase in pH from pH 6.0 to 9.0 (i.e., (1.2 ± 0.1) × 10 2 M −1 s −1 to (8.3 ± 0.3) M −1 s −1 ). The species-specific rate constants were obtained as k (HFeO 4 − ) = 1.3 × 10 2 M −1 s −1 and k (FeO 4 2− ) = 6.9 M −1 s −1 . The decreases in the concentration of HFeO 4 − with increase in pH caused the observed pH dependence in k app . At pH 7.0, the removal of IMI increased with the molar ratio from 1.0 to 10.0 with complete removal at the highest ratio. The variation in pH from 6.0 to 9.0 had no obvious effect on removal of IMI. Experiments indicate that IMI removal is mainly by ferrate(VI) oxidation and to a lesser extent by Fe(III) adsorption. Mineralization of IMI was also observed (20–26%). The addition of Fe(III) ions to ferrate(VI)-IMI at pH 7.0 and 8.0 resulted in enhanced removal of IMI, but the presence of Ca 2+ , SO 4 2− , HCO 3 − , and humic acid (HA) has negative effects. The presence of coexisting substances in river water slightly decreased IMI removal by ferrate(VI) by less than 10%. Identification of products and frontier electron density (FED) calculations demonstrated involvement of opening of the five-membered heterocyclic moiety of IMI by ferrate(VI). Toxicity assessment with NIH 3T3 fibroblasts and ECOSAR analysis indicated lower toxicity of oxidized products than parent IMI.
研究领域:
环境科学
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化学
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PubMed
高影响因子
ENVIRONMENTAL TECHNOLOGY
·
2019
·
IF 1.918
Jing Deng,Huadan Wu,Sujuan Wang,Yibing Liu,Hongyu Wang
The removal of sulfapyridine (SPY) by ferrate(VI) in aqueous solutions under a broad range of reaction conditions, including ferrate(VI) dosage, solution pH, natural organic matter and coexisting inorganic ions, was systematically investigated and the oxidation pathway of SPY by ferrate(VI) was deeply explored. Results showed that 500 µg/L of SPY was efficiently decomposed (86%) within 1 min by 5 mg/L ferrate(VI) at pH 5.6. The increment in ferrate(VI) dosage was surely favorable for SPY removal. The best SPY degradation was achieved at pH 5.6, under or above which the removal decreased. The introduction of inorganic ions in solutions retarded SPY removal. Ten oxidation intermediates were identified and the cleavages of C–S and S–N bonds might be the primary ways of SPY oxidation by ferrate(VI).
研究领域:
环境科学
·
化学
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PubMed
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
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2019
·
IF 7.65
K.M. Wang,J. Shu,S.J. Wang,T.Y. Hong,X.P. Xu,H.Y. Wang
Anode passivation is still a main challenge for the electrochemical generation of ferrate(VI, Fe(VI)), leading to the reduction of Fe(VI) production efficiency. In this study, cyclic voltammetry, scanning electronic microscopy, and electrochemical impedance spectroscopy were used to select better anode electrode configurations (iron wire, iron gauze, and iron coil). The results indicate that iron coil had the least degree of passivation. Different imposed current waveforms during the electrochemical generation of Fe(VI) were also investigated, and the iron coil imposed with square alternating current (AC) wave can mitigate the anode passivation, resulting in higher Fe(VI) production efficiency. The optimum conditions for the electrochemical generation of Fe(VI) were evaluated and the optimum temperature (40 ℃), current density (10 mA/cm 2 ), AC cycle period (15 s) and electrolyte concentrations (14 M NaOH) were identified. As a result, 0.12 mol/L Fe(VI) concentration and over 50% of current efficiency can be achieved after 3 h electrolysis. The generated Fe(VI) solution was further applied to oxidize doxycycline(DOX) and sulfadiazine(SDZ) as typical antibiotics. Over 80% of DOX can be removed at a Fe(VI) to DOX molar ratio of 5:1 (pH = 4–9), whilst a higher Fe(VI) to SDZ molar ratio of 20:1 (pH = 7) was needed to obtain 75% SDZ removal.
研究领域:
环境科学
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电化学工程
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PubMed
高影响因子
Journal of Environmental Sciences
·
2018
·
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
CHEMOSPHERE
·
2019
·
IF 5.108
Xueyin Wu,Aixi Tang,Xiaochao Bi,Thanh H. Nguyen,Baoling Yuan
Surface water contaminated with algae and with enteric viruses is a global problem. When surface water is used as a drinking water source, it is important to know the influence of algal organic matter on the disinfection of viruses. In this work, we studied the disinfection efficacy of ferrate and the influence of algal organic matter on the disinfection. We determined the MS2 inactivation kinetics by ferrate under three pH conditions (7, 8, and 8.7). The experimental results and pH-dependent calculation suggest that H 2 FeO 4 and HFeO 4 − are 1935 and 8 times as effective as FeO 4 2− in MS2 inactivation. We also found that intracellular algal organic matter (IAOM) had a stronger effect on MS2 inactivation kinetics than extracellular algal organic matter (EAOM) suggesting that IAOM led to higher consumption of Fe(VI) compared to EAOM. At pH 8.7, while significant consumption of FeO 4 2− by as low as 8 mg C/L of EAOM and 2 mg C/L of IAOM was detected, MS2 inactivation was negatively influenced only when 13 mg C/L of IAOM present. This study showed that it is important to control pH and to determine the concentration of algal organic matter if ferrate is used for disinfection of surface water contaminated with algae.
研究领域:
环境科学
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水处理工程
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病毒学
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PubMed
高影响因子
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