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芬顿化学
Catalysts · 2023 ·Vol. 13 ·期 7 ·1057 · IF 3.9

Oxygen-Vacancy-Rich Fe@Fe3O4 Boosting Fenton Chemistry

Rongwei Zheng,Ruifan Tan,Yali Lv,Xiaoling Mou,Junqiao Qian,Ronghe Lin,Ping Fang,Weidong Kan

Iron-based materials are widely applied in Fenton chemistry, and they have promising prospects in the processing of wastewater. The composition complexity and rich chemistry of iron and/or oxides, however, hamper the precise understanding of the active sites and the working mechanism, which still remain highly controversial. Herein, iron oxides of four different model systems are designed through a conventional precipitation method plus H2reduction treatment. These systems feature Fe@Fe3O4with abundant oxygen vacancy, Fe0and Fe3O4particles with interface structures, and Fe3O4-dominated nanoparticles of different sizes. These materials are applied in the decomposition of methyl orange as a model reaction to assess the Fenton chemistry. The Fe@Fe3O4with core–shell structures exhibits significantly higher decomposition activity than the other Fe3O4-rich nanoparticles. A thin Fe3O4layer formed by auto-oxidation of iron particles when exposed to air can boost the activity as compared with the Fe0and Fe3O4particles with interface structures but poor oxygen vacancy. The unique hetero-structure with the co-existence of both metallic iron and oxygen vacancy displays excellent redox propensity, which might account for the superior Fenton activity. This finding provides a new perspective to understand and design highly efficient iron-based Fenton catalysts.

研究领域: 环境科学 · 材料科学
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WATER RESEARCH · 2025 · IF 12.4

Silico-oxygen bonding integrated with nano-size pore enrichment enables sustainable low-oxidant-consumption Fenton-like chemistry

Qingbai Tian,Xin Zhang,Jiale Chang,Dongdong Chen,Siyuan You,Xiaoming Peng,Baoyu Gao,Yanan Shang,Bo Wei,Qian Li,Zhen Hu,Yue Gao,Xing Xu

Key bottlenecks of the persulfate-based advanced oxidation processes (AOPs) are the high dosage of persulfate and the secondary pollution of sulfate ion. In this work, a sustainable strategy involving the transformation of diatomite into a water purification catalyst consisting of nano-size pore enrichment and silico-oxygen bonding (Si/C@BD) was proposed. Results indicated that the pollutants with electron-donating groups can be quickly degraded by the Si/C@BD via amplified electron transfer process (ETP) under very low peroxymonosulfate (PMS) usage. Such “low-oxidant-consumption” Fenton-like chemistry can be also applied to other catalytic systems derived from a series of silicon-based materials. In addition, a pilot-scale device (54 L) based on ETP pathway was constructed, which provided a universal strategy to prevent direct contact of treated wastewater with oxidation additives, thereby solving the bottleneck of secondary pollution caused by sulfate dissolution associated with PMS oxidation systems. In addition, the Si/C@BD/PMS system exhibited the superior environmental significance and feasibility based on the quantitative analysis via the life cycle assessment (LCA). This work will be a significant contribution to the persulfate-based Fenton-like chemistry, emphasizing the low-persulfate-consumption and free-secondary-pollution characteristics with significant application value.

研究领域: 环境科学 · 材料科学
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SENSORS AND ACTUATORS B-CHEMICAL · 2016 · IF 4.758

A colorimetric biosensor using Fe3O4 nanoparticles for highly sensitive and selective detection of tetracyclines

Yilin Wang,Yujing Sun,Haichao Dai,Pengjuan Ni,Shu Jiang,Wangdong Lu,Zhen Li,Zhuang Li

A novel colorimetric biosensor for the determination of tetracyclines (TCs) based on the Fe 3 O 4 magnetic nanoparticles (Fe 3 O 4 MNPs) is presented in this paper. TCs are known to have a strong tendency to complex with metal ions such as Fe(II) and Fe(III) on the surface of Fe 3 O 4 MNPs. Experiments results show that the complexation of Fe 3 O 4 MNPs and TCs could lead to the accelerated catalysing H 2 O 2 -mediated oxidation of 3,3′,5,5′-tetramethylbenzidine (TMB) by Fenton chemistry. The reaction starts with oxidation of Fe 3 O 4 MNPs-TCs complex by dissolved oxygen to generate reactive oxygen species (ROS), primarily ·OH, leading to deepen the color of the solution. Analysis results can be seen with the naked eye and monitored by UV–vis spectra. Under the optimal conditions, the detection limits are 26   nM for oxytetracycline (OTC), 45   nM for tetracycline (TC) and 48   nM for doxycycline (DOX). Moreover, this method has been applied for the determination of OTC content in drugs with satisfactory results. The proposed colorimetric biosensor is advantageous over other conventional methods in terms of convenient operation without any complicated chemical synthesis, modification, or tedious experimental procedures and its simple signal generation and detection by the naked eye. To the best of our knowledge, this is the first report on the enhancement effect of TCs on Fe 3 O 4 MNPs-TMB-H 2 O 2 reaction and its application in colorimetric TCs analysis. The designed colorimetric strategy may provide a promising alternative detection for TCs in clinical samples.

研究领域: 分析化学 · 生物传感器 · 环境科学 · 药物分析
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Biomaterials Advances · 2024 · IF 5.5

Iron-based magnetic nanocomplexes for combined chemodynamic and photothermal cancer therapy through enhanced ferroptosis

Wenying Wei,Haifei Kang,Chenxi Lian,Jiawei Liu,Jinwei Lin,Junwei Yang,Zhangmancang Xu,Ziqi Wang,Meizhen Yin,Honglian Dai

Chemodynamic therapy (CDT) guided by Fenton chemistry and iron-containing materials can induce ferroptosis as a prospective cancer treatment method, but the inefficient Fe 3+ /Fe 2+ conversion restricts the monotherapeutic performances. Here, an iron-based nanoplatform (Fe 3 O 4 -SRF@FeTA) including a magnetic core and a reductive film is developed for combined CDT and photothermal therapy (PTT) through ferroptosis augmentation. The inner iron oxide core serves as a photothermal transducer, a magnet-responsive module, and an iron reservoir for CDT. The coated Fe 3+ -tannic acid film (FeTA) provides extra iron and reductants for Fe 3+ /Fe 2+ conversion acceleration, and functions as a door keeper for the pH- and light-responsive release of the embedded ferroptosis inducer sorafenib (SRF). The in vitro results demonstrate that the iron-based nanocomplexes promote the production of lipid peroxide through the amplified Fenton activity, and downregulate glutathione involved in lipid peroxide repair system through the responsively released SRF. Upon accumulation in tumor by magnetic targeting and sequential laser irradiation locoregionally, Fe 3 O 4 -SRF@FeTA nanocomplexes present prominent in vivo anticancer efficacy by leveraging PTT and CDT-enhanced ferroptosis.

研究领域: 纳米技术 · 癌症治疗 · 材料科学 · 生物医学工程
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CHEMICAL ENGINEERING JOURNAL · 2024 · IF 13.3

Fenton chemistry activation in metal-organic frameworks for synergistic bacteria eradication

Jiayi Qin,Jia Su,Hong Li,Ling Zhang,Ling Zhang,Ke Jiang

The development of novel antibacterial strategies as alternatives to antibiotics is of great significance but remains considerable challenges due to the lack of safe, effective, and broad-spectrum agents. Here, we explored the potential of a biocompatible metal–organic framework Fe-MIL-53-NH 2 (FM) for reactive oxygen species (ROS)-based antibacterial applications. However, FM was found to be catalytically inert due to the very weak reducibility of Fe 3+ toward H 2 O 2 . To address this challenge, we incorporated a small amount of Co 2+ (0.98 %) into FM (CFM), successfully activating Fenton chemistry and achieving a notable 5.5-fold improvement in Fenton activity. Density functional theory (DFT) calculations revealed that a very small amount of Co 2+ doping significantly reduces the energy barrier of the Fenton reaction by shifting the d-band center to the Fermi level and optimizing the charge density of active Co atoms. We further enhanced the antibacterial properties of CFM by modifying it with the photothermal agent polydopamine (PDA), resulting in CFMP. Through the synergistic effects of ROS and photothermal properties, CFMP exhibited remarkable antibacterial activity, with bacterial eradication rates exceeding 99 % against both E. coli and S. aureus . Moreover, in vivo experiments demonstrated the exceptional efficacy of CFMP in sterilizing S. aureus -infected wounds, while causing negligible damage to other major organs. This study not only highlights the role of atom engineering in activating Fenton reaction, but also provides rational designs for a synergistic antibacterial strategy via powerful MOFs chemistry.

CAS / MDL: 10312-55-7
研究领域: 材料科学 · 纳米技术 · 生物医学工程 · 化学 · 微生物学
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SENSORS AND ACTUATORS B-CHEMICAL · 2022 · IF 9.221

Zn-doped carbon dots-based versatile bioanalytical probe for precise estimation of antioxidant activity index of multiple samples via fenton chemistry

Muhammad Sohail,Bin Xie,Bingzhi Li,He Huang

The significance of antioxidant activity determination in health sciences and food technology has become a hot research area as it is directly related to oxidative stress which is affiliated with several diseases and food deterioration. Herein, we fabricated a Zn-CDs-based (Zn-doped carbon dots-based) bioanalytical probe for the estimation of antioxidant activity index (AAI) to cope with the truncated robustness, high interference effect in complex samples, photo-bleaching, and low stability of the traditional techniques. Besides, the novel AAI standardized the presentation of the results by considering the transducer, Zn-CDs, concentration as reported results vary diversely for the same sample. In principle, free radicals quenched the fluorescence of the probe via inner filter effect and dynamic quenching. The presence of antioxidants hindered the fluorescence quenching by sequestering the free radicals from the reaction. The designed nanoreagent was validated for its applications using ascorbic acid , human serum, topical cosmetic formulation, and tomato juice samples. The bioanalytical probe demonstrated precise linearity, high robustness, low interference effect, and analytical equivalence when compared to the DPPH free radical assay. Hence, it can be used for the diagnosis and follow-up of oxidative stress-related ailments, developing and characterizing cosmeceuticals, analysis of antioxidant-containing formulations, and assessing and controlling the quality of food products. It is the first report to explore the antioxidant feature of Zn-CDs and its advantage for the estimation of AAI.

CAS / MDL: 50-81-7 6119-70-6
研究领域: 分析化学 · 生物化学 · 生物技术 · 食品科学 · 健康科学
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Nano Today · 2023 · IF 17.4

Engineering a self-fueling and self-reported theranostic nanocatalyst for amplified cancer imaging and chemodynamic therapy

Hong Chen,Pingyu Wu,Zhenzhen Xiao,Ting Li,Minjuan Zhong,Yuqi Xie,Yanlan Liu

Chemodynamic therapy (CDT) has sparked increasing interest in selective cancer treatment. However, it remains a challenge to achieve an efficient and sustained therapeutic effect due to the restricted Fenton chemistry and deficient catalytic substrates within the tumor microenvironment (TME). Meanwhile, the lack of strategies to timely monitor the delivery and execution of CDT agents increases the risks of unwanted side effects. Here, we present that integration of TME-triggered cascade catalysis with tumor metabolism reprogramming to engineer activatable theranostic nanocatalysts is an effective way to tackle these challenges. A self-fueling and self-reported theranostic nanocatalyst is reported in this study by modifying multi-enzyme mimic MnO 2 nanosturctures with antisense oligonucleotides (ASO). This catalyst can produce free radicals through logic multi-enzymatic catalysis to induce oxidative damage to cancer cells, yet keeping inert in normal cells. Furthermore, the loaded ASO can silence MCT4 that overexpresses in tumor cells, resulting in efflux blockage of intracellular lactate and decrease of intracellular pH , which remarkably facilitates the cascade catalysis for amplified CDT. Meanwhile, such acidification triggers an MRI enhancement for reporting gene silencing. Results from in vivo testing further support the potential of our design for more effective CDT. This study offers different insights into the design and construction of advanced platforms for noninvasive imaging-guided treatment of a wide range of cancers.

CAS / MDL: 112-80-1 7722-64-7
研究领域: 癌症治疗 · 纳米技术 · 生物医学工程 · 分子生物学 · 医学成像
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Advanced Healthcare Materials · 2024 · IF 10

Cascade nanoreactor employs mitochondrial-directed chemodynamic and δ-ALA-mediated photodynamic synergy for deep-seated oral cancer therapy

Qiqi Yin,Yanli Yao,Handan Zhang,Jie Zhang,Jiaming Gao,Lin Weng,Tao Liu,Shuyang Sun,Xin Chen

The management of oral squamous cell carcinoma (OSCC) poses significant challenges, leading to organ impairment and ineffective treatment of deep-seated tumors, adversely affecting patient prognosis. We introduced a cascade nanoreactor that integrates photodynamic therapy (PDT) and chemodynamic therapy (CDT) for comprehensive multimodal OSCC treatment. Utilizing iron oxide nanoparticles and mesoporous silica, we developed the FMMSH drug delivery system, encapsulating the photosensitizer prodrug δ-aminolevulinic acid (δ-ALA). Triphenylphosphine (TPP) modification facilitated mitochondrial targeting, while tumor cell membrane (TCM) coating provided homotypic targeting. The dual-targeting δ-ALA@FMMSH-TPP-TCM nanoparticles demonstrated efficacy in eradicating both superficial and deep tumors through synergistic PDT/CDT. Esterase overexpression in OSCC cells triggered δ-ALA release, and excessive hydrogen peroxide in tumor mitochondria underwent Fenton chemistry for CDT. The synergistic interaction of PDT and CDT mechanisms increased cytotoxic ROS levels, intensifying oxidative stress and enhancing apoptotic and damage mechanisms, ultimately leading to enhanced tumor cell death. PDT/CDT-induced apoptosis generated δ-ALA-containing apoptotic bodies, enhancing anti-tumor efficacy in deep tumor cells. The advantageous anatomical accessibility of oral cancer emphasizes the potential of intratumoral injection for precise and localized treatment delivery, ensuring focused therapeutic agent delivery to maximize efficacy while minimizing systemic side effects. Thus, δ-ALA@FMMSH-TPP-TCM, tailored for intratumoral injection, emerges as a transformative modality in OSCC treatment. This article is protected by copyright. All rights reserved

CAS / MDL: 1830-78-0 110-18-9
研究领域: 纳米技术 · 肿瘤学 · 治疗学 · 生物医学工程 · 药学
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