APPLIED CATALYSIS B-ENVIRONMENTAL
·
2021
·
IF 19.503
Leiduo Lai,Peng Zhou,Hongyu Zhou,Minglu Sun,Yue Yuan,Yang Liu,Gang Yao,Bo Lai
Coupling dithionite (DNT) with FeVO 4 induced PMS activation (FeVO 4 /PMS/DNT) effectuates fast heterogeneous Fe(III) reduction to generate multitudinous reactive oxygen species (ROS) for fast degradation of carbamazepine (2.5 mg/L, >90 % degradation efficiency within 300 s) in batch mode. The Fe(III)/Fe(II) circulation propelled by DNT and reduced V species experiences two stages. DNT induces SO 2 − generation, which is a highly active species with strong reducibility for Fe and V reduction. The reduced V species donate electrons to ≡Fe(III) via Fe-O-V bond rather than directly react with PMS, implying introducing polyvalent V to modulate Fe-based materials intensifies DNT utilization and alleviates ROS quenching effects. Moreover, FeVO 4 crystalline form regains after reaction, and FeVO 4 /PMS/DNT system has an excellent reutilization and strong resistance to natural waters. Our discovery sheds new light on acceleration of heterogenous Fe(III)/Fe(II) circulation to promote Fenton-like oxidation , it may be a long-lasting strategy for water remediation.
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高影响因子
JOURNAL OF ENVIRONMENTAL MANAGEMENT
·
2026
·
IF 9.2
Lu Zeng,Xuexia Guo,Jiahao Sun,Wenbin Huang,Huinan Zhao,Lingling Hu,Shuanghong Tian,Chun He
In Fenton-like processes, achieving rapid and efficient redox cycling of metal active centers remains a challenge. This study presents an innovative strategy that harnesses the mechanical energy of water flow to drive the redox cycling of metal active centers. Herein, Fe 3 O 4 /MoS 2 heterojunction with interfacial Mo-S-Fe bridge bonds was constructed via a one-step hydrothermal method. Under the stimulation induced by water-flow mechanical, the piezoelectric effect of MoS 2 generates charge carriers, which are rapidly directed to Fe active sites through the Mo-S-Fe bonds. This process significantly accelerates the Fe(III)/Fe(II) cycle and enhances H 2 O 2 activation, achieving 93.8% removal of sulfamethoxazole (SMX) within 60 min under water flow stimulation. The composite exhibits robust performance across a broad pH range (3.0-10.7) and in the presence of humic acid (HA) and coexisting anions, demonstrating its strong environmental adaptability. Spectroscopic evidence confirmed the formation of Mo-S-Fe bonds at the heterojunction interface. Mechanistic studies further revealed that the structure improves charge separation, promotes rapid electron transfer from MoS 2 to Fe sites, and strengthens H 2 O 2 adsorption, thereby synergistically boosting reactive oxygen species (ROSs) generation and the overall catalytic efficiency. This study proposes an innovative strategy that exploits mechanical forces generated by water flow to drive rapid redox cycling of active metal centers in Fenton-like reactions.
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CHEMICAL GEOLOGY
·
2026
·
IF 3.6
Yuan Qiu,Lisong Ma,Biao Wan,Xinran Liang,Shuai Lan,Guanjie Jiang,Yang Li,Qin Zhang,Yupeng Yan
Poorly crystalline iron hydroxides, such as ferrihydrite (Fh) and its aluminum-substituted counterpart (Al-substituted ferrihydrite, Al-Fh), are ubiquitous in surficial geochemical environments and undergo strong interfacial interactions with organic phosphorus (e.g., myo -inositol hexakisphosphate, phytate, IHP). However, how these interactions regulate the Fe(II)-catalyzed dissolution–recrystallization of Fh and Al-Fh into secondary Fe minerals and consequently influence phosphorus geochemical mobility and sequestration remains unclear. This study systematically investigated the Fe(II)-catalyzed transformation of phytate-preadsorbed Al-Fh via batch experiments and multiple characterizations to elucidate the regulatory role of phytate in governing Fe(II)-catalyzed Al-Fh transformation and phytate repartitioning. Results showed that isomorphous Al substitution inhibited goethite (Gt) nucleation in Fe(II)-catalyzed Al-Fh transformation by decreasing Al-Fh crystallinity and disrupting the periodic Fe–O–Fe crystal lattice arrangement. Fe(II) drove mineral dissolution and secondary phase nucleation via interfacial electron transfer (IET), with catalytic efficiency positively correlated with its concentration. Phytate exerted a concentration-dependent effect: at low concentration (0.5 mM), it impeded the further transformation of lepidocrocite (Lp) to Gt through strong inner-sphere surface complexation of phytate on reactive Fe sites, thereby favoring Lp mineral accumulation. At higher concentrations (≥1.0 mM), it greatly inhibited Al-Fh transformation via a combination of surface complexation, IET inhibition, reactive Fe(II) depletion, and the occupation of mineral dissolution sites, resulting in metastable Lp or amorphous products. Mechanistically, phytate formed stable complexes on Al-Fh surfaces, hindering electron transfer. Concurrently, phytate and Fe(II) generated ternary complexes (≡Fe–IHP–Fe(II)) or surface iron phytate precipitates on minerals, thereby depleting the reactive Fe(II) pool. Throughout transformation, phytate remained strongly sequestered in the solid phase rather than being released into solution due to its strong geochemical interactions with Fe/Al hydroxides. This work elucidates the synergistic regulatory mechanisms of Al and phytate in Al-Fh transformation, offering key theoretical insights into organic phosphorus–iron hydroxide interactions and long-term phosphorus immobilization in Al-rich soils.
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高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Zhengyuan Zhou,Mudassir Habib,Zhiqiang Xu,Guilu Zeng,Rumin Yang,Qian Sui,Shuguang Lyu
In this research, greigite (Fe 3 S 4 ) was innovatively applied for the enhancement of PDS/Fe(II) system. From XRD and SEM analyses, Fe 3 S 4 was successfully synthesized and appeared uniform sphere-like particles with a petal-like structure. Trichloroethylene (TCE), as the target, was significantly degraded from 28.5 % to 92.8 % in PDS/Fe(II)/Fe 3 S 4 system. The enhanced mechanisms, differences, and superiority of Fe 3 S 4 against the other three iron sulfides were elucidated as follows: (1) on account of the abundant reduction sites on its surface, Fe 3 S 4 could not only directly release Fe(II) and accelerate Fe(II) regeneration by sulfur substances, but also participate in the process of O 2 − • generation, and (2) the reaction mainly took place on Fe 3 S 4 surface, in which the surface-bound reactive species (RSs) were of great importance for TCE degradation. Through EPR, quantification, and scavenging tests of RSs, HO•, SO 4 − •, and O 2 − • were all the dominant RSs responsible for TCE removal. Besides, these enhanced systems had high tolerance on complex water conditions and could remediate various contaminants in actual groundwater. Three TCE degradation pathways were deduced in four iron sulfide-enhanced systems and the toxicities of intermediates were evaluated, recommending that Fe 3 S 4 -enhanced system was of the least toxicity and most favorable for application in practice.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2020
·
IF 7.489
Feng Cheng,Peng Zhou,Xiaowei Huo,Yang Liu,Yunxin Liu,Yongli Zhang
The photocatalytic behavior of the graphene oxide (GO) modified Fe(III)/peroxymonosulfate (Fe/PMS) system for bisphenol A (BPA) degradation was investigated. With the addition of GO, a dramatic enhancement of BPA degradation was obtained at pH 3.0 under visible light irradiation. According to ESR analysis and quenching tests, both SO 4 - and OH are responsible for BPA degradation. The characterization analysis demonstrates that Fe(III) can chelate with the oxygenic functional groups on the surface of GO forming a stable GO-Fe(III) complex. The detections of different kinds of Fe species reveal that Fe(III) can be reduced to Fe(II) by GO via intramolecular electron transfer in the GO-Fe(III) complex, and visible light could enhance this process. The Fe(III)/Fe(II) cycle not only occurs on the surface of GO, but also in aqueous solution via homogeneous reactions. In addition, the degradation pathway of BPA was proposed based on the identification of the intermediates using GC–MS and LC-MS techniques.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2020
·
IF 5.774
Fangke Yu,Yi Wang,Hongrui Ma,Minghua Zhou
In this study, we demonstrated that hydrothermal synthesized FeS 2 was highly efficient to catalyze the H 2 O 2 decomposition for diclofenac sodium (DCF) degradation in a wide range of initial pH (3–9) by heterogeneous electro-Fenton (EF) process, and this “Pyrite-EF” showed a better performance for the mineralization of DCF in comparison with the classic EF process. Effect of pyrite content on the hydroxyl radicals generation and iron dissolution produced by the decomposition of hydrogen peroxide (H 2 O 2 ), and applied current density on the degradation kinetics and mineralization efficiency were studied. Moreover, toxicity assessment by means of microtox method showed the solution toxicity was removed after treatment. Experimental results revealed that the enhancement of DCF degradation rate in the Pyrite-EF process was attributed to the molecular oxygen activation induced by more surface bound ferrous ions on FeS 2 , generating superoxide anions to accelerate the Fe(II)/Fe(III) cycle on the FeS 2 surface, which favored the H 2 O 2 decomposition to generate more hydroxyl radicals for the DCF degradation via a heterogeneous EF-like process. These findings could provide some new insights into the molecular oxygen activation induced by FeS 2 and the subsequent heterogeneous Pyrite-EF degradation of organic pollutants from wastewater.
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高影响因子
Journal of Environmental Sciences
·
2020
·
IF 4.302
Xiaoyang Fan,Yili Wang,Daxin Zhang,Yajie Guo,Shihui Gao,Enrui Li,Huaili Zheng
The effects of four conditioning approaches: Acid, Acid-zero-valent iron (ZVI)/peroxydisulfate (PMS), Fe(II)/PMS and ZVI/PMS, on wastewater activated sludge (WAS) dewatering and organics distribution in supernatant and extracellular polymeric substances (EPS) layers were investigated. The highest reduction in bound water and the most WAS destruction was achieved by Acid-ZVI/PMS, and the optimum conditions were pH 3, ZVI dosage 0.15 g/g dry solid (DS), oxone dosage 0.07 g/g DS and reaction time 10.6 min with the reductions in capillary suction time (CST) and water content (Wc) as 19.67% and 8.49%, respectively. Four conditioning approaches could result in TOC increase in EPS layers and supernatant, and protein (PN) content in tightly bound EPS (TB-EPS). After conditioning, organics in EPS layers could migrate to supernatant. Polysaccharide (PS) was easier to migrate to supernatant than PN. In addition, Acid, Acid-ZVI/PMS or Fe(II)/PMS conditioning promoted the release of some polysaccharides containing ring vibrations v P O, v C-O-C, v C-O-P functional groups from TB-EPS. ESR spectra proved that both radicals of SO 4 - · and ·OH contributed to dewatering and organics transformation and migration. CST value of WAS positively correlated with the ratios of PN/PS in LB-EPS and total EPS, while it negatively correlated with TOC, PN content and PS content in TB-EPS, as well as PS content in supernatant and LB-EPS. BWC negatively correlated to zeta potential and TOC value, PN content, and HA content in supernatant.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2019
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IF 5.107
Ping Tang,Wenchao Jiang,Shuguang Lyu,Yizhou Wu,Zhaofu Qiu,Qian Sui
In this study, we examined the effects of chelators on reductive degradation of carbon tetrachloride (CT) in Fe(II) activated CaO 2 system in the presence of methanol (MeOH). The results suggested that glutamate (Glu) could significantly enhance CT degradation percent with around 25.9% increase in 20 min at the initial CaO 2 /Fe(II)/MeOH/Glu/CT molar ratios of 20/20/10/10/1. In the system, MeOH and Glu acted through different mechanisms, in which MeOH was used to directly stimulate the reductants formation and its reactivity, whereas Glu was acted to keep relatively high soluble iron and thus promote Fenton reaction. The results of scavenging tests suggested that O 2 − was one of the reductive radicals for CT depletion and the mechanism of CT degradation was significantly distinguished from trichloroethene (TCE) degradation which was primarily through oxidation by OH . CH 2 Cl 2 , C 2 Cl 4 , and C 2 Cl 6 were detected as the intermediates accompanied by CT destruction, and a reduction mechanism for CT degradation by the CaO 2 /Fe(II)/MeOH/Glu process was proposed accordingly. Finally, the simultaneous removal of CT and TCE was achieved in the CaO 2 /Fe(II)/MeOH/Glu system, indicating a potential technique for complex contaminated sites remediation.
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2018
·Vol. 25
·期 26
·26394-26404
·
IF 2.8
Liu Yong,Lang Jie,Wang Ting,Jawad Ali,Wang Haibin,Khan Aimal,Chen Zhulei,Chen Zhuqi
Phenylurea herbicide residuals in soil may continuously contaminate surface water and groundwater due to unregulated and improper use. Herein, we reported a stable and active oxidation system including heterogeneous Fe-based layered double hydroxide materials as persulfate (PS) activators. Under mild conditions, 1% LDH in weight and 70 mM PS can completely degrade 500 mg/kg isoproturon in soil within 10 h, during which less than 0.1 ppm heavy metal leaching was detected. This remarkable performance was consistent in a broad pH range (3~11) and was resistant to various inorganic anions (Cl − , Br − , NO 3 − , HCO 3 − ) and humic acid. Mechanism studies from scavenging tests, EPR, and fluorescence spectra collectively proved that besides •OH and •SO 4 − , singlet oxygen ( 1 O 2 ) and superoxide (•O 2 − ) were also generated and were accounted for the oxidative degradation. This unique mechanism of generating diverse radicals was clearly distinguished from classic Fe(II)/PS system, significantly reduced the influence of varying parameters in water and soil matrix, and was suggestive to chemical oxidation system in soil remediation to avoid scavenging effects by background electrolytes or other components in water/soil matrix.
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ACS Applied Materials & Interfaces
·
2025
·
IF 8.2
Jiangnan Xu,Xiu Luo,Weiwei Su,Guorong Jia,Huawei Cai,Danni Li,Rou Li,Xiangdong Wang,Yefa Yang,Tao Wang,Changjing Zuo
Transarterial radioembolization (TARE) is a primary palliative treatment for advanced liver cancer. Nonetheless, its therapeutic efficacy is frequently hindered by resistance to tumor cell apoptosis induced by inter-radiotherapy. Induction of multiple cell death modalities provides a potential solution to this challenge. Ferroptosis, a distinct form of cell death from apoptosis, is dependent on the intracellular Fe2+-mediated Fenton reaction for the production of hydroxyl radicals (·OH) and is gaining recognition as a promising approach for cancer treatment. In this study, we synthesized a therapeutic radionuclide iodine-131 (131I)-based TARE agent by combining 131I-labeled iron-based MIL-88B(Fe) nanoparticles (NPs) (abbreviated as 131I-MIL-88B(Fe)) with Lipiodol to achieve a combined apoptosis–ferroptosis tumor therapy. Specifically, a mixture of Lipiodol and 131I-MIL-88B(Fe) NPs was injected into the liver tumors through the hepatic artery. Lipiodol blocks the arterial blood supply of the tumor, causing tumor tissue necrosis, whereas 131I inter-radiotherapy damages deoxyribonucleic acid (DNA) through direct action or indirectly via the production of ·OH through H2O radiolysis, leading to tumor cell apoptosis. Importantly, hydrated electrons (eaq–), a byproduct of H2O radiolysis, promoted the conversion of Fe3+ to Fe2+ in MIL-88B(Fe) NPs, enhancing the efficacy of the Fenton reaction and triggering ferroptosis. In vitro experiments demonstrated that compared to 131I alone, 131I-MIL-88B(Fe) NPs significantly enhanced ferroptosis-mediated tumor cell death due to 131I-induced Fe2+ production, which increased catalytic activity in the Fenton reaction. In a rat model bearing orthotopic N1S1 liver tumors, TARE with Lipiodol and 131I-MIL-88B(Fe) NPs induced tumor cell necrosis, apoptosis, and ferroptosis, resulting in improved therapeutic outcomes. This study leverages eaq– to facilitate Fe3+/Fe2+ conversion for efficient ferroptosis, turning waste into a valuable resource. This demonstrated the innovative integration of multiple treatment strategies to augment the efficacy of TARE in liver cancer therapy.
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WATER RESEARCH
·
2022
·
IF 13.4
Feng Wang,Wenyi Dong,Zilong Zhao,Hongjie Wang,Wenting Li,Liang Zhang,Heng Ouyang,Xiao Huang,Ji Li
Polycyclic aromatic hydrocarbons (PAHs) are found ubiquitously in contaminated aquatic sediments. They are difficult to degrade, particularly the high-molecular-weight PAHs (e.g., benzo[a]pyrene, BaP). In this study, CaO 2 assisted with ferrous ion (Fe(II)) - citric acid (CA) was applied for the first time in BaP degradation in aquatic sediment. Among the treatment processes we studied, CaO 2 /Fe(Ⅱ)/CA could effectively degrade BaP at circumneutral pH (7.0 ± 0.3), reaching a maximum of nearly 80% under optimal conditions (0.84 mM CaO 2 , 0.21 mM Fe(Ⅱ), and 0.35 mM CA in per gram of dry sediment). Contrary to some external environmental factors such as temperature, common metal ions, and natural organic matters, a certain amount of moisture content and inorganic anions (Cl − , SO 4 2− ) exhibited a positive effect on BaP degradation, which can probably be contributed to the improved mass transfer rate in the non-homogeneous sediment-water mixture and a higher level of free radicals. The degradation kinetic dominated by hydroxyl radicals included three main stages contribution ∼29.4%, ∼43.1%, and ∼2.4% to BaP degradation, respectively. Based on the theoretical calculations of density functional theory, a pathway for BaP degradation was proposed. For the treatment of actual contaminated sediment, the CaO 2 /Fe(II)/CA process could realize the elimination of black-odor and effective removal of PAHs from the sediment, as well as negligible ecotoxicity on benthic organisms. This study provides a reference and guidance for the use of CaO 2 based Fenton-like systems in treating PAH-contaminated black-odor river sediments.
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JOURNAL OF HAZARDOUS MATERIALS
·
2022
·
IF 14.224
Shiwei Xie,Chang Li,Hui Zhan,Wei Shao,Yuanxin Zhao,Peng Liu,Peng Liao
Fe-based replacement and precipitation are promising methods for removal of copper ethylenediaminetetraacetic acid (Cu(II)-EDTA) but are limited by the necessity of controlling pH and dissolved oxygen. The details of the decomplexation mechanism also remain unclear. The present work investigated an anoxic iron electrocoagulation process capable of automatically modulating anoxic conditions and solution pH during exposure to air and thus promoting the rapid and thorough decomplexation of Cu(II)-EDTA. Dissolved Fe (II), rather than Fe(II)-bearing minerals, was found to be primarily responsible for the reduction of Cu(II)-EDTA to Cu(I)-EDTA and for the subsequent replacement reaction to generate free Cu(I) ions within the initial pH range of 2–7. The Cu(I) was primarily precipitated as Cu 2 O on the surface of green rust and magnetite as the pH was increased. The aeration of these Fe-containing precipitates released free Cu(I) ions instead of chelated Cu into solution, allowing for recycling of the Cu. This release of Cu(I) was likely induced by the pH decrease during aeration. This study provides important insights regarding the reductive decomplexation of chelated Cu(II) and the recovery of Cu via anoxic iron electrocoagulation, which is a promising green approach to recycling Cu from wastewater.
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