CHEMOSPHERE
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2019
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IF 5.108
Xiaobing Wang,Yueyao Wang,Na Chen,Yanbiao Shi,Lizhi Zhang
Persulfate (PS) is widely used for environmental remediation, but its organic contaminant removal performance strongly depends on its activation. In this study, we demonstrate that pyrite (FeS 2 ) can more effectively activate PS than the commonly used FeSO 4 for atrazine degradation. When 3.0 mM of PS and 4.2 mM of iron salts were used, the atrazine degradation efficiency of FeS 2 /PS was 1.4 times that of FeSO 4 /PS, while the amount of consumed PS in case of FeS 2 was only 53% of that by FeSO 4 . The better PS activation performance of FeS 2 could be attributed to its slow and sustainable release of dissolved Fe(II), inhibiting the quenching reaction between •SO 4 − /•OH and Fe(II) ions, and thus producing more reactive oxygen species for the atrazine degradation. More importantly, the surface bound Fe(II) of FeS 2 could activate molecular oxygen to generate superoxide radical (•O 2 − ), which could further promote the effective decomposition of PS by accelerating the Fe(III)/Fe(II) redox cycle. This study unravels the roles of dissolved Fe(II) and surface bound Fe(II) on the persulfate activation, and provides a promising heterogeneous persulfate activator for pollutant control and environmental remediation.
研究领域:
环境科学
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化学工程
✓ 已验证
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Junchuan Zhang,Yuan Yan,Andac Armutlulu,Kexin Wei,Jian Wu,Bo Lai,Ruzhen Xie
Heterojunctions present a promising avenue for improving charge separation in photocatalytic water purification processes. However, the multicomponent heterojunction interfaces often act as recombination centers for photogenerated carriers. Herein, a Ti-based homologous-like heterojunction was fabricated by in-situ growth of controllable CaTiO 3 on sulfur-doped TiO 2 (STCTO). This heterojunction exhibits outstanding performance in photocatalytic water decontamination when assisted by peroxymonosulfate (PMS). The well-matched interfaces within the heterojunction generate internal electric fields that facilitate efficient electron migration from ST to CTO by minimizing the energy barrier. PMS serves as a dual function as an electron-acceptor to enhance carriers separation efficiency, and as a precursor for sulfate radical generation, thereby promoting the production of reactive species. Consequently, the homologous-like heterojunction STCTO enables complete Atrazine removal without any deterioration even after 8th recycle. These findings underscore the synergistic effects of photo-energized and PMS-intensified homologous heterojunctions, providing insights into a novel approach for the removal of refractory hazardous organic contaminants using solar energy.
研究领域:
环境科学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
CHEMOSPHERE
·
2020
·
IF 5.778
Nan Yang,Yanping Liu,Jia Zhu,Zhongqiang Wang,Jinwei Li
In order to improve the catalytic activity and recycling performance of heterogeneous Fenton catalyst, a heterogeneous Fenton catalyst Fe/TiO 2 based on TiO 2 supported visible light response was prepared by a simple method using TiO 2 synthesized by sol-gel method as carrier and ferric nitrate as Fe source. It was characterized by SEM , EDX , XRD, UV–vis instruments. The influencing factors of catalytic degradation of atrazine by visible light heterogeneous Fenton of Fe/TiO 2 were studied and the reaction kinetics were fitted. The mineralization degree of atrazine was reflected by the removal rate of TOC. The intermediate products by the degradation of the catalytic system was analyzed and the reaction mechanism of Fe/TiO 2 –H 2 O 2 visible light system was discussed. The XRD results showed that Fe was highly dispersed on the surface of TiO 2 in the form of α-Fe 2 O 3 . The Fe/TiO 2 catalyst with heterogeneous Fenton and visible light photocatalytic activity was successfully optimized, forbidden bandwidth of Fe/TiO 2 after Fe supported was narrower, the scope of light absorption red-shifted, the electron-hole pairs were more generated, and there was a significant synergistic effect between the carrier TiO 2 and the supported Fe, which exhibited good oxidation capacity for degradation of 10 mg L −1 atrazine in pH of 3, the concentration of H 2 O 2 was 1.6 mM, and the catalyst was added at 1 g L −1 , achieving over 95% removal efficiency within 30 min, and, in the range of pH 3–7, the degradation rate of the reaction for 30 min can be maintained above 75%, which greatly broadened the range of pH application and had good recycling performance. The degradation process conformed to the quasi-first-order kinetic model . Through LC-MS analyzed, 12 intermediate products were formed during the degradation of atrazine, the final products were all cyanuric acid, and then the triazine ring was mineralized into inorganic substances such as CO 2 , H 2 O and NO 3 − by oxidation of ·OH, and the possible degradation pathways were inferred.
研究领域:
环境科学
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催化化学
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2016
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IF 5.31
Shiqing Zhou,Lingjun Bu,Zhou Shi,Chen Bi,Qihang Yi
In this work, iron electrode was employed to enhance the reactivity of ozone (EC/O 3 ) in atrazine degradation. Compared to ozonation and Fe 2+ -catalyzed ozonation, the elimination rate of atrazine by the EC/O 3 process increased significantly with increasing applied currents. The simultaneous formation of hydroxyl radical (OH ) and ferryl ion (Fe(IV)) from the reaction between ozone and in-situ formed Fe 2+ was proposed and experimentally confirmed. The second order rate constant for atrazine reacting with Fe(IV) was estimated to be 125 M −1 s −1 using a relative rate method. The individual roles of the reactive species (OH , Fe(IV), and O 3 ) in atrazine degradation were modeled using a kinetic model and OH was the predominant reactive species in the EC/O 3 system. Furthermore, the effects of water quality parameters, such as initial pH and natural organic matters (NOM), on the performance of EC/O 3 process were also evaluated. The results demonstrated that higher initial pH is favorable for ozone consumption and atrazine degradation. The presence of NOM appreciably inhibited the degradation of atrazine, which may be attributed to the competition of NOM for OH . This study provides a new approach to enhance ozonation, and broadens the knowledge of ozonation in removing organic contaminants from water.
研究领域:
环境科学
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水处理技术
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产品关联
DOI
高影响因子
Journal of Water Process Engineering
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2025
·
IF 6.7
Kang Zhichao,Wang Tianye,Nannan Li,Han Xuerong,Wang Chenxu,Yang Xiutao,Jing Yue,Yu Hongwen
The leaching of atrazine wastes from agricultural areas presents a considerable risk to the ecosystem. This work aims to create microorganism-material systems employing the atrazine-degrading strain Paenarthrobacter sp. KN0901 and C 3 N 5 -based materials to efficiently eliminate atrazine residues from aquatic environments at low temperatures. The synthesized C 3 N 5 and O-C 3 N 5 markedly improved the growth and atrazine degradation of KN0901. The degradation rate of atrazine in the KN0901-C 3 N 5 and KN0901-O-C 3 N 5 systems rose by 7.3 % and 15.1 %, respectively, in comparison to biodegradation systems. The elevated NADH/NAD+ and GSH/GSSG ratios indicated a greater availability of electrons to KN0901 when associated with C3N5-based materials, implying that these materials contributed electrons to KN0901. Nitazoxanide and methyl viologen inhibited the electron transfer route, leading to a significant decrease in the breakdown rate of KN0901-C 3 N 5 systems. Glucose and sodium citrate, functioning as electron donors, markedly accelerated the degradation rate of atrazine in the KN0901-C 3 N 5 systems. This work demonstrated that C 3 N 5 -based materials may donate electrons to KN0901, hence improving the efficiency of atrazine breakdown at low temperatures. This work successfully developed microorganism-material systems that effectively eliminate atrazine in aquatic settings, especially in cold climates.
研究领域:
环境生物学
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微生物学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2019
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IF 14.229
Hongwei Sun,Guihong Xie,Di He,Lizhi Zhang
In this study we constructed a heterogeneous Fenton system with ascorbic acid (AA), magnetite (Fe 3 O 4 ) and H 2 O 2 for the alachlor degradation, aiming to clarify the heterogeneous Fenton mechanism. The addition of AA could significantly accelerate the Fenton reaction by promoting the surface Fe(III)/Fe(II) redox cycle (iron cycle) of Fe 3 O 4 . A kinetic model was successfully developed to quantitatively describe the complicated reactions in the Fe 3 O 4 /AA/H 2 O 2 system. We thus employed this model to identify the individual contributions of surface and homogeneous Fenton reactions to the overall alachlor degradation in the Fe 3 O 4 /AA/H 2 O 2 system, and found the surface Fenton reaction was mainly responsible for the alachlor degradation with more than 62.6% of contribution. This work offers a new strategy to improve the heterogeneous Fenton activity via promoting surface Fenton reaction, and sheds light on the possibility to quantitatively describe and predict the heterogeneous Fenton processes with first principle kinetic models.
研究领域:
环境科学
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
Journal of Environmental Sciences
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2017
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IF 2.865
Xiangjuan Yuan,Xuan Yan,Haiming Xu,Dongya Li,Lei Sun,Gang Cao,Dongsheng Xia
Enhanced ozonation degradation of atrazine (ATZ) with nano-ZnO (nZnO) as catalyst and the influences of the operational parameters have been investigated through semi-continuous experiments in this study. The results demonstrated that the combination of ozone (O 3 ) and nZnO showed an obvious synergetic effect and the ATZ degradation conformed to pseudo-first-order kinetics. An improvement of ATZ degradation efficiency by 41.8% and pseudo-first-order rate constant by more than a factor of four was obtained in the O 3 /nZnO process after 5 min of reaction compared to O 3 alone. Meanwhile, the degradation efficiency of ATZ was gradually enhanced with increasing nZnO dosage and initial pH in the range from 3.0 to 8.0, and a higher amount of ATZ was degraded when the initial concentration of ATZ rose from 0.5 to 5 mg/L. Additionally, sulfate ion, chloride ion, nitrate ion and low concentrations of humic acid substances led to enhancement of the ATZ degradation. The notable decrease of ATZ removal efficiency observed in the presence of radical scavengers and the results of free radical tests indicated that OH is the dominant active radical species. The mechanism investigation demonstrated that the enhancement effect could be attributed to the introduction of nZnO, which could promote the utilization of O 3 , enhance the formation of superoxide radical, and further accelerate the production of hydrogen peroxide and the generation of OH/O 2 − .
研究领域:
环境科学
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化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
WATER RESEARCH
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2017
·
IF 6.942
Xiaoxiang Cheng,Heng Liang,An Ding,Xiaobin Tang,Bin Liu,Xuewu Zhu,Zhendong Gan,Daoji Wu,Guibai Li
Ferrous iron/peroxymonosulfate (Fe(II)/PMS) oxidation was employed as a pretreatment method for ultrafiltration process to control membrane fouling caused by natural organic matter, including humic acid (HA), sodium alginate (SA), bovine serum albumin (BSA), and their mixture (HA-SA-BSA). To evaluate the mechanism of fouling mitigation, the effects of Fe(II)/PMS pretreatment on the characteristics of feed water were examined. The degradation of atrazine (ATZ) was also investigated and the species of generated radicals were preliminarily determined. Under the test exposure (15 and 50 μM), Fe(II)/PMS pretreatment effectively mitigated membrane fouling caused by HA, SA and HA-SA-BSA mixture, and the performance improved with the increase of Fe(II) or PMS dose; whereas aggravated BSA fouling at lower doses and fouling alleviation was observed only at a higher dose (50/50 μΜ). The fouling mitigation was mainly attributed to the effective reduction of organic loadings by coagulation with in-situ formed Fe(III). Its performance was comparable or even slightly higher than single coagulation with Fe(III), most likely due to the oxidation by Fe(II)/PMS process. Fe(II)/PMS oxidation showed better performance in reducing DOC and UV 254 , fluorescence intensities of fluorescent components and UV-absorbing compounds than single coagulation. In addition, Fe(II)/PMS pretreatment was efficient in ATZ degradation due to the generation of sulfate and hydroxyl radicals , whereas coagulation was ineffective to remove it.
研究领域:
环境科学
·
水处理技术
✓ 已验证
产品关联
DOI
PubMed
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2021
·
IF 19.503
Rongdi Tang,Daoxin Gong,Yaoyu Zhou,Yaocheng Deng,Chengyang Feng,Sheng Xiong,Ying Huang,Guanwei Peng,Ling Li
Herein, a g-C 3 N 4 /PDI-g-C 3 N 4 homojunction has been fabricated for piezo-photocatalytic atrazine removal and exhibited better performance than individual photocatalysis or piezocatalysis. The introduction of PDI induces the π-π interaction facilitating electrons migration, and twists the g-C 3 N 4 plane into a more polar porous structure with enhanced piezoelectricity. The homojunction facilitates the photoelectron transfer at the g-C 3 N 4 /PDI-g-C 3 N 4 interfaces. The photoelectricity and the piezoelectricity of g-C 3 N 4 /PDI-g-C 3 N 4 were assessed. The finite element simulation showed that the porous structure of the g-C 3 N 4 /PDI-g-C 3 N 4 is essential to the enhanced piezoelectricity. Astonishingly, the piezo-photocatalytic atrazine degradation rate under an optimized condition (pH=2.97) reached 94% within 60 min. Moreover, the g-C 3 N 4 /PDI-g-C 3 N 4 homojunction produced 625.54 μM H 2 O 2 during the one-hour piezo-photocatalysis. Given the quenching experiments, reactive species detection and the electronic band of g-C 3 N 4 /PDI-g-C 3 N 4 , the piezo-photocatalytic mechanism has been proposed. In addition, the degradation pathways and the reduced intermediates toxicity intermediates of atrazine have been investigated.
研究领域:
环境科学
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材料科学
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催化化学
✓ 已验证
产品关联
DOI
高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2021
·
IF 4.539
Qiangbin Yang,Jibin An,Zhonghao Xu,Shuting Liang,Honghong Wang
Due to the carcinogenicity of atrazine, the effective removal of atrazine in water and soil has become the focus of attention. In the paper, the advanced oxidation technology based on sulfate radicals ( S O 4 · - ), which the visible light catalysis and nanocatalyst Co 3 O 4 /g-C 3 N 4 synergistically catalyzed to yield S O 4 · - , was constructed to efficiently degrade and remove atrazine. The Co 3 O 4 /g-C 3 N 4 was prepared through a simple solvothermal method, and its microstructure and composition were characterized by SEM and XRD. A series of experiments were carried out to degrade atrazine by Co 3 O 4 /g-C 3 N 4 activation of peroxymonosulfate under visible light, which revealed that the degradation efficiency reached to 78.5 percent in 35 min, CO 3 2− had a significant inhibitory effect on the degradation of atrazine in coexisting ions of NO 3 -, SO 4 2− , Cl- and CO 3 2− , the e -, ⋅OH, and S O 4 · - were mainly active species. Combined with density function theory calculations of Co 3 O 4 /g-C 3 N 4 , the high-efficiency degradation of atrazine was due to the synergetic enhancement between photocatalysis and Co 3 O 4 /g-C 3 N 4 catalyst in the constructed catalytic system.
研究领域:
环境科学
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化学工程
✓ 已验证
DOI
高影响因子
Journal of Environmental Sciences
·
2025
·
IF 6.3
Qingkong Chen,Jieyu Xia,Fengjun Liu,Jianping Fan,Peng Yan,Mika Sillanpää
This study developed a novel heterogeneous Vis-Photo+Fenton-like system by integrating visible-light-responsive Co 3 O 4 /TiO 2 photocatalysis with peroxymonosulfate (PMS) activation for efficient atrazine (ATZ) degradation. The synergistic process achieved complete ATZ removal within 60 min under near-neutral pH (6.9), outperforming individual Fenton-like (39 %) and photocatalytic (24 %) processes. Key factors influencing the degradation efficiency included light sources (UV > visible), pH (optimal at 6.9), catalyst dosage (0.01 g Co 3 O 4 /TiO 2 ), and PMS:ATZ molar ratio (1:2). The system exhibited a synergistic coefficient of 5.03 (degradation) and 1.97 (mineralization), attributed to enhanced radical generation and accelerated Co 3+ /Co 2+ redox cycling through photoinduced electron transfer. Intermediate analysis revealed dealkylation, dechlorination, and oxidation pathways, with reduced toxicity of by-products (e.g., CEAT, CIAT) confirmed by ecotoxicity assessments. The mineralization efficiency (Vis-Photo+Fenton-like) reached 83.1 %, significantly higher than that of standalone processes (Fenton-like: 43.2 %; photocatalysis: 30.5 %). The catalyst demonstrated excellent stability (nearly 90 % recovery, < 1 μg/L Co leaching) and practical applicability. This study provides an efficient, sludge-free, and solar-compatible strategy for eliminating persistent herbicides in water treatment.
研究领域:
环境科学
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化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Jawad Ali,Dan Li,Ajmal Shahzad,Muhammad Wajid Ullah,Jerosha Ifthikar,Muhammed Asif,Chen Yanan,Xie Lei,Zhuqi Chen,Songlin Wang
The Fe-based materials were considered very attractive for the treatment of wastewater using peroxymonosulfate (PMS) activation. However, the difficulties to restore the active Fe 2+ oxidation state restrict them to attained sustainable efficiency. In this work, a new strategy was introduced to accelerate the regeneration of Fe 2+ state through constructing an electron-rich MoS 4 2− centre in the inter-layers of FeMgAl layered double hydroxide (MoS 4 -LDH) catalyst. The dual centre MoS 4 -LDH catalyst was found more efficient as clear from the observed atrazine (ATZ) degradation rate of 0.117 min −1 , 100 times higher than the Fe 3+ /PMS or 25–50 times higher than the Fe based single centre NO 3 -LDH/PMS, CO 3 -LDH/PMS or S 2 O 4 -LDH/PMS systems, respectively. This boosted efficiency was related to the electron-rich MoS 4 2− centre which allows the constant electron transfer to reduce the electron-deficient Fe 3+ center at MoS 4 -LDH surface and thereby accelerating the Fe 2+ /Fe 3+ redox cycle during reaction. Furthermore, the MoS 4 -LDH/PMS system exhibited a broader effective pH (3.0–9.0), good stability and minimum influence of background electrolyte or organic matter. The degradation pathway of ATZ based on free radical (SO 4 – and OH), involving the redox cycles of Fe 3+ /Fe 2+ and Mo 6+ /Mo 4+ was proposed for the activation of PMS . This work highlighted the essential role of MoS 4 2− moiety, to accelerate the Fe 3+ reduction at the surface of the LDH catalyst through the continuous feeding of electrons.
研究领域:
环境科学
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子