SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Huaimin Wang,Shuang Meng,Zixuan Zhang,Chenying Zhou,Heng Zhang,Yang Liu,Chuan-shu He,Peng Zhou,Bo Lai
It has been reported that the ultrasonic agitation coupled system (US/A) has higher oxidation efficiency than the pure ultrasonic system (US), and the atomic hydrogen ( H) and hydroxyl radicals ( OH) produced by H 2 O cracking and in situ hydrogen peroxide (H 2 O 2 ) can be significantly detected. In order to utilize the residual H 2 O 2 and explore the role and fate of H, US/A/Fe(III) as an in situ Fenton oxidation system, was constructed in this study. The experimental results proved that the system can generate H 2 O 2 in situ , and adding Fe(III) could significantly promote the oxidation of refractory organic pollutants. Quenching tests, probes experiments and EPR test were performed to successfully monitor the existence of OH. The contribution of H to Fe(III) reduction was speculated and confirmed. In addition, the kinetic model showed the decomposition rate of water molecule and the reduction rate of Fe(III) by H under different ultrasonic power. The effects of the factors (pH, coexisting substance, and actual water environment) on degrading organic pollutants were evaluated. Therefore, this work provides new strategy and mechanistic insight into in situ Fenton technique by coupling ultrasonic agitation and Fe(III) without external oxidants.
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高影响因子
Pharmaceutics
·
2025
·Vol. 17
·期 10
·1257
·
IF 5.5
Jialing Li,Ning Han,Mingyue Ruan,Hongmei Wei,Yunan Dong,Haitong Zhang,Zishuo Guo,Shouying Du,Pengyue Li
Background/Objectives:Triple-negative breast cancer (TNBC) exhibits pronounced biological heterogeneity, aggressive behavior, and a high risk of recurrence and metastasis. The conventional treatments for TNBC have notable limitations: surgical resection may leave residual tumor cells; chemotherapy (CT) frequently induces systemic toxicity and drug resistance; and radiotherapy damages surrounding organs and compromises the patients’ immune function.Methods: Herein, we designed a carrier-free nanodrug delivery system composed of self-assembled Curcumin nanoparticles (NPs) coated with a tannic acid (TA)/Fe(III) network (denoted as CUR@TA-Fe(III) NPs). We systematically evaluated the in vitro cytotoxicity and photothermal–ferroptosis synergistic therapeutic efficacy of CUR@TA-Fe(III) NPs in 4T1 breast cancer cells, as well as the in vivo antitumor activity using 4T1 tumor-bearing mouse models.Results:CUR@TA-Fe(III) NPs had high drug loading efficiency (LE) of 27.99%, good dispersion stability, and photothermal properties. Curcumin could inhibit the growth of 4T1 cancer cells, while TA-Fe(III) efficiently converted light energy into heat upon exposure to near-infrared (NIR) light, leading to direct thermal ablation of 4T1 cells. Additionally, TA-Fe(III) could supply Fe(II) via TA, increase intracellular Fe(II) content, and generate reactive oxygen species (ROS) through the Fenton reaction, in turn inducing lipid peroxidation (LPO), a decrease in mitochondrial membrane potential (MMP), and glutathione depletion, eventually triggering ferroptosis.Conclusions:This treatment strategy, which integrates CT, PTT, and ferroptosis, is expected to overcome the limitations of traditional single-treatment methods and provide a more effective method for the treatment of TNBC.
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PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Haonan Chen,Shiqi Tian,Zheng-Qian Liu,Jun Ma,Gang Wen
Iron oxides are widely utilized in catalytic ozonation, but their effectiveness is often limited by the slow Fe(II)/Fe(III) redox cycle. In this study, a series of metal sulfide–iron oxide composites were synthesized, all of which exhibited enhanced catalytic performance, with MoS 2 @Fe 3 O 4 showing outstanding efficiency. The catalytic system decomposes ozone (O 3 ) into hydroxyl radicals (·OH) and singlet oxygen ( 1 O 2 ), with ·OH predominantly contributing to the oxidation process. The catalytic process was significantly enhanced through three key pathways: (i) metal sulfides themselves demonstrate superior ozonation catalytic performance compared to iron oxides; (ii) the presence of Mo(IV) effectively promotes the Fe(II)/Fe(III) redox cycle; and (iii) the transient superoxide radical (·O 2 − ), a crucial intermediate in ozone chain decomposition, rapidly reduces high-valence Mo(VI) to Mo(IV), thereby reinforcing the Mo redox cycle, further strengthening the Fe redox cycle, and leading to the accumulation of 1 O 2 . Notably, the efficient utilization of ·O 2 − represents a unique mechanism in the catalytic ozonation system. These findings emphasize the critical role of the Mo redox cycle in enhancing Fe redox activity to promote catalytic ozonation, providing valuable insights for the development of advanced metal sulfide–iron oxide catalysts for environmental applications.
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高影响因子
SCIENCE OF THE TOTAL ENVIRONMENT
·
2018
·
IF 4.61
Rong Chen,Hui Liu,Man Tong,Lei Zhao,Peng Zhang,Deng Liu,Songhu Yuan
The interplay of Fe(II) oxidation and Fe(III) bio-reduction occurs widely in both natural and engineered redox-dynamic systems. This study aimed to unravel the impact of Fe(II) oxidation by O 2 in the presence of iron-reducing bacteria on subsequent Fe(III) bio-reduction. Mixed solutions of Fe 2+ (0.1–0.5 mM) and Shewanella oneidensis strain MR-1 (MR-1, 2.0 × 10 7 CFU/mL) at neutral pH were first exposed to laboratory air for Fe(II) oxidation and bacterial inactivation, and then the resultant Fe(III) suspensions were switched to anoxic conditions for bio-reduction by the surviving bacteria. In the oxidation step, the coexisting MR-1 was inactivated by 0.8–1.71 orders of magnitude within 60 min. In the subsequent bio-reduction step, the resultant Fe(III) was bio-reduced by the surviving MR-1. Bio-reduction of the resultant Fe(III) by the surviving MR-1 was 1.8–2.5 times faster than that of the Fe(III) that was produced from Fe 2+ oxidation without MR-1 by fresh MR-1 cells at 2.0 × 10 7 CFU/mL. Although MR-1 inactivation during Fe(II) oxidation may inhibit Fe(III) bio-reduction, the increase in bio-availability of the resultant Fe(III) and the residual reactivity of dead cells led to net enhancement of bio-reduction under the tested conditions. Lepidocrocite was the sole Fe(III) mineral that was produced from Fe 2+ oxidation without MR-1, while 19% ferrihydrite was produced from Fe 2+ oxidation in the presence of MR-1. The formation of low-crystallinity ferrihydrite accounts for the increase in bio-availability of the Fe(III) minerals. The findings of this study highlight an important but overlooked impact underlying the interplay of Fe(II) oxidation and Fe(III) bio-reduction.
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PubMed
高影响因子
FUEL
·
2021
·
IF 6.609
Xinyue Zhang,Bo Zhang,Yanjun Chen,Lei Li,Houxiang Sun,Xuandong Liu,Rong Guo,Bo Meng,Peng Liu,Weiyu Song,Qiaoxia Guo,Baojian Shen
Electronic structure tuning is an effective strategy to activate transition metals. In this study, silica-promoted γ-Al 2 O 3 -supported Fe-based hydrodesulfurization catalysts of Fe species with electron loss were successfully prepared by transferring electrons from Fe to Si. The characterization results showed that the Fe-based hydrodesulfurization catalyst with the addition of silica modulated the structure and properties of the active metal, which not only improved the degree of sulfidation of the active metal but also promoted the generation of Fe(III)-S. The hydrodesulfurization rate of dibenzothiophene showed a remarkable rise from 38.4 to 83.2% at 673 K. Importantly, the formation of Fe(III)-S greatly stretched the bond length of Fe-S bonds, exhibiting an increase of approximately 21%, this facilitating the generation of coordinatively unsaturated active site. Finally, the HDS reaction performance of the Fe-based hydrodesulfurization catalysts was mainly influenced by the Fe(III)-S/Fe(II)-S ratio, with the most significant enhancement in the direct desulfurization reaction path. The results of this study provide a promising approach for the design and development of environmentally friendly and economical Fe-based catalysts in the field of clean fuels.
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高影响因子
SOIL BIOLOGY & BIOCHEMISTRY
·
2022
·
IF 8.546
Jinzhi Yao,Shuping Qin,Ting Liu,Tim J. Clough,Nicole Wrage-Mönnig,Jiafa Luo,Chunsheng Hu,Tida Ge,Shungui Zhou
Poorly crystalline iron (Fe) oxides are commonly deposited on the surface of rice roots, forming an Fe plaque. This Fe plaque is an important area for Fe redox reactions because the poorly crystalline Fe is available for microbial transformations. However, it remains unclear what the mechanisms are that cause the root Fe plaque to affect CO 2 emissions from paddy soils . Thus, this study investigated the effects of Fe plaque on paddy soil CO 2 emissions and the associated mechanisms. Paddy soil with rice plant roots containing an Fe plaque-coating had 1.5-fold larger CO 2 emissions and higher expression levels of genes involved in soil carbon (C) degradation than Fe plaque-free roots, indicating that Fe plaque stimulated paddy soil derived CO 2 emissions. Fe plaque-coated rice roots, immersed in a 13 C-labeled glucose solution, emitted more CO 2 , with a higher abundance of 13 CO 2 , than the Fe plaque-free roots. These differences were not observed when the surfaces of the rice roots were sterilized. These results indicate that the Fe plaque-stimulated CO 2 emissions were due to soil microbial respiration , not autotrophic root respiration . Chelating the dissolved Fe on the root surface eliminated Fe plaque stimulation of CO 2 emissions, while Fe(III) supplementation correlated with enhanced CO 2 emissions. The stoichiometric mole ratio of the enhanced CO 2 emissions to the Fe(II) generated was comparable to the theoretical ratio of Fe(III) when used as an electron acceptor for organic C decomposition. These results showed that the Fe plaque enhancement of CO 2 emissions was coupled to Fe(III) reduction. Limiting the stimulating effects of Fe plaque on CO 2 emissions may be a potentially useful approach for mitigating organic C loss from paddy soils.
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高影响因子
Water
·
2026
·Vol. 18
·期 20
·2536
·
IF 3.5
Hanlin Wang,Tianhu Chen,Mengxue Li,Chang Liu,Guoqing Xu,Zijun Xiao,Ruoqing Fan,Zhengwei Pan,Lanbao Zhu
Fe(III) is widely present in non-stoichiometric pyrrhotite (Fe1−xS, 0 < x < 0.125); however, its role in determining the catalytic activity of Fe1−xS remains unclear. Herein, Fe1−xS with varying Fe(III) were prepared via the sulfidation of goethite and the pyrolysis of pyrite at different temperatures, respectively, and subsequently employed to activate peroxydisulfate (PDS) for tetracycline (TC) removal. A combination of characterization and chemical analysis revealed that the Fe(III) content in sulfurized Fe1−xS and pyrolytic Fe1−xS decreased linearly with increasing sulfidation temperature (R2= 0.9875) and calcination temperature (R2= 0.9665), respectively. Electrochemical and zeta potential measurements showed that both the electron-transfer capability and surface electronegativity of Fe1−xS increased with increasing Fe(III) content. Importantly, in the Fe1−xS/PDS system, the Fe(III) content in sulfurized Fe1−xS and pyrolytic Fe1−xS was positively correlated with the second-order reaction rate constant (k2, R2= 0.9276) and first-order reaction rate constant (k1, R2= 0.9741) for TC removal, respectively, suggesting a clear structure-activity relationship between Fe(III) content and catalytic activity. Meanwhile, Fe release, reactive oxygen species (ROSs) generation, and PDS consumption increased with increasing Fe(III) content in Fe1−xS. In addition, sulfurized Fe1−xS and pyrolytic Fe1−xS show a wide pH operating range and moderate reusability. These findings provide valuable insights into the rational design of Fe1−xS-based catalysts for advanced oxidation processes to remove refractory organic pollutants.
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高影响因子
FUEL
·
2025
·
IF 7.5
Hugang Li,Hongxu Chen,Yongfei Gao,Yuhong Qin,Shuai Niu,Hui Zhou,Yuanhui Zhang
Crystallization of vivianite-phosphorus is a promising method to recover phosphate as a vital resource from sewage sludge hydrothermal carbonization (HTC) products. This study reveals the in-situ recrystallization mechanism of vivianite-phosphorus (Fe 3 (PO 4 ) 2 ·8H 2 O) regulated by FeCl 3 -assisted HTC in depth. The key finding includes the decipherment that phosphorus is mainly enriched in hydrochar (72.7 ± 2.9 %wt ∼ 84.4 ± 3.31 %wt). Further identified by HRTEM and XRD, dominant phosphorus is profiled as vivianite (Fe 3 (PO 4 ) 2 ·8H 2 O) with very few calcium phosphate crystals (Ca 3 (PO 4 ) 2 ) formation in hydrochar at near-neutral condition. Under acidic conditions, HMF oxidation triggers reductive dissolution of surface-bound Fe(III)-phosphate complexes, releasing Fe 2+ , HPO 4 2− , and PO 4 3− . The anoxic, reducing conditions at circumneutral pH created by HTC, combining with favorable Fe: P ratio (1.72) and lower calcium concentration (532 mg L −1 ), comprehensively drives the crystallization of Fe 3 (PO 4 ) 2 ·8H 2 O. This demonstration-of-practice study provides deep insights into dual organic waste resource and energy valorization.
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高影响因子
JOURNAL OF APPLIED POLYMER SCIENCE
·
2025
·
IF 2.8
Ke Liu,Qisong Liu,Rui Fan,Hongfa Huang,Hua Yi,Chao Hu
Mixed matrix membranes (MMMs) incorporating metal–organic frameworks (MOFs) as fillers show attractive selectivity and permeability for gas separation. However, the performance improvement is restricted by undesirable interfacial interaction and inhomogeneous dispersion of MOFs in the membrane matrix. In this paper, amino-functionalized UIO-66 (U6N) with high porosity was employed as a filler and further regulated by a controlled plant polyphenol-induced surface modification strategy. The process involved the formation of tannic acid-iron(III) complex (TA-Fe(III)) on the U6N surface, which improved interfacial compatibility with the polyimide matrix while introducing abundant hydroxyl groups to enhance gas transport properties. Accordingly, the modified MMMs containing 30 wt.% U6N@TA-Fe(III) achieved optimized gas separation performance. Specifically, the CO 2 permeability increased to about 2495.9 Barrer with a CO 2 /CH 4 selectivity of 19.32, which exceeded the 2008 Robeson upper limit and showed an increase of 22.1% and 25.6%, respectively, compared to the MMMs embedded with unmodified U6N. Moreover, the improved dispersion of the U6N@TA-Fe(III) within the membrane structure is conducive to improving separation performance for CO 2 /N 2 and O 2 /N 2 . Therefore, this work provides a novel insight into the rational design of the MMMs via a facile modification strategy, which can further improve the gas separation performance of the MMMs.
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高影响因子
ACS ES&T Water
·
2025
·
IF 4.3
Neng Tao,Longjian Guo,Xiu Wu,Di Fang,Lixiang Zhou
To address the technical bottlenecks of the classic Fenton oxidation for anaerobically digested sludge (ADS) dewatering (e.g., high doses of Fe2+/H2O2/acid usage and slow reduction of Fe3+), we employed biodegradable tannin compounds as iron chelating and reducing agents to improve the Fenton reaction. Compared with the classic Fenton (pH 3.0), tannic acid (TA)-assisted Fenton enhanced the degree and rate of ADS dewatering (pH 5.2) with reductions of 99% in specific resistance filtration, 96% in capillary suction time, and 97% in filtration–compression time. Besides, this modification reduced the consumption of Fe2+/H2O2 by 50%. Mechanistically, TA could chelate Fe3+ to generate iron complexes while facilitating the reduction of Fe3+ to Fe2+. This phenomenon avoided Fe3+ precipitation and accelerated Fe3+/Fe2+ cycling to produce more hydroxyl radical (•OH).•OH oxidation disintegrated CHOP-, CHONS-, and CHONSP-containing protein-/lipid-like substances within tightly bound extracellular polymeric substances. Bioflocs were dispersed into an irregular block-shaped structure with smaller particle sizes. Employing low-cost and readily accessible tannin-rich plant crude extracts derived fromAcacia mangiumas an alternative to purified TA in Fenton conditioning of ADS exhibited comparable enhancements in dewaterability characteristics. These findings demonstrated that the synergy between tannin compounds and Fenton oxidation could facilitate the cost-effective dewatering of ADS.
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高影响因子
WATER RESEARCH
·
2022
·
IF 13.4
Zhengyuan Zhou,Jingyao Huang,Guilu Zeng,Rumin Yang,Zhiqiang Xu,Zhikang Zhou,Shuguang Lyu
S(IV)-based advanced oxidation process has been applied for contaminants remediation. However, as a traditional source of sulfite (SO 3 2− ), Na 2 SO 3 is extremely soluble in water, resulting in a high concentration of SO 3 2− to quench the generated reactive oxygen species (ROS). In this work, CaSO 3 was introduced instead of Na 2 SO 3 for its slow-released SO 3 2− ability and Fe(III)/CaSO 3 system was established for the removal of trichloroethylene (TCE) and other organic contaminants. The degradation efficiency of TCE reached 94.0% and TCE could be completely dechlorinated and mineralized, while the removal of other contaminants was all over 85.0% at the optimal tested conditions. Through EPR detection, ROS scavenging and probe tests, and quantification of ROS amounts, it was concluded that the dominant ROS in Fe(III)/CaSO 3 system were SO 4 − · and 1 O 2 , of which the transformation mechanism of SO 4 − · to 1 O 2 was revealed and demonstrated comprehensively. The synergistic contaminants degradation performance in different sulfur-iron-containing systems and in the presence of oxidants was evaluated. The effects of various solution conditions were assessed and Fe(III)/CaSO 3 system was of higher resistance on complex solution matrixes, suggesting the broad-spectrum and application perspective for the remediation of complex contaminants in actual water.
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高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2019
·
IF 7.65
Suding Yan,Xinping Zhang,Hui Zhang
The combination of persulfate (PS) activation by iron ions with electrochemical process (electro/Fe 3+ /PS) is a promising advanced oxidation process. However, almost all these systems were performed in an unbuffered solution and actually under acidic pH condition, with the electricity being frequently supplied by external power. Considering the high buffering capacity of wastewater and energy saving, peroxydisulfate (PDS) activation by Fe(III) species with bioelectricity provided by microbial fuel cell (MFC) for bisphenol A (BPA) oxidation was investigated at fixed near-neutral pH as well as acidic pH. The results indicate that 90.8% of BPA could be removed at pH 2.5. Though the iron existed in the form of precipitate, BPA could still be efficiently removed at pH 6.0. The precipitate formed in the system at pH 6.0 was identified as the amorphous iron oxyhydroxides. Sulfate radicals in the bulk solution and that adsorbed on the precipitate were the dominant reactive species responsible for the oxidation of BPA in the homogeneous and heterogeneous MFC/Fe(III)/PDS processes, respectively. The mechanisms of BPA degradation at both pH values were proposed via EPR and quenching tests as well as XPS analysis. The effects of operating parameters, the mineralization, the mineralization current efficiency and energy consumption were also explored.
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高影响因子
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