Theranostics
·
2020
·
IF 8.579
Qingqing Tian,Lu An,Qiwei Tian,Jiaomin Lin,Shiping Yang
Rationale : Chemodynamic therapy (CDT) based on the Fe(II)-mediated Fenton reaction is an emerging tumor treatment strategy. However, the catalytic efficiency in tumors is crucially limited by Fe(II). Herein, an endogenous hydrogen sulfide (H 2 S) accelerated Fe(III)/Fe(II) transformation and photothermal synergistically enhanced CDT strategy based on ellagic acid-Fe-bovine serum albumin (EA-Fe@BSA) nanoparticles (NPs) was developed for colon tumor inhibition. On the one hand, the Fe(III) with low catalytic activity in the EA-Fe@BSA NPs could be rapidly reduced to the highly active Fe(II) by the abundant H 2 S in colon cancer tissues. Thus, a rapid Fe(III)/Fe(II) conversion system was established, wherein highly active Fe(II) ions were continuously regenerated to improve the CDT efficiency. On the other hand, the photothermal effect of EA-Fe@BSA NPs also accelerated the production of hydroxyl radicals (•OH), thereby synergistically enhancing the CDT performance and improving the therapeutic efficacy. Methods : The endogenous H 2 S accelerated Fe(III)/Fe(II) conversion and PTT enhanced CDT were investigated by characterization of the Fe valence state and detection of •OH. T 1 -weighted magnetic resonance imaging (MRI) was tested both in vitro and in vivo . The biocompatibility of NPs were examined via MTT assay, hemolysis analysis and routine blood measurements. The enhanced CDT was investigated in HCT116 colon cancer cells by Calcein-AM/PI staining and MTT assay, and tumor inhibition was demonstrated in HCT116 tumor bearing mice. Results : In this work, EA-Fe@BSA NPs were constructed as a CDT theranostic reagent. The H 2 S accelerated Fe(III)/Fe(II) conversion was confirmed, more degradation of MB and generation of •OH demonstrated the enhanced CDT in vitro . EA-Fe@BSA NPs exhibited good T 1 -weighted MRI performance. More importantly, it displayed strong near-infrared (NIR) absorption and excellent photothermal efficiency, further promotes the production of •OH. Hence, the efficacy of CDT was enhanced, and the tumor growth was inhibited efficiently. Conclusion : All results demonstrate that this strategy based on endogenous H 2 S promoted Fe(III)/Fe(II) transformation together with PTT acceleration permits efficient Fenton-reaction- mediated CDT both in vitro and in vivo , which holds great potential for effective colon cancer theranostics.
研究领域:
生物医学工程
·
肿瘤治疗
·
纳米医学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2021
·
IF 10.588
Heng Zhang,Mengfan Luo,Peng Zhou,Yang Liu,Ye Du,Chuanshu He,Gang Yao,Bo Lai
Recently, the enhancing role of hydrogen peroxide (H 2 O 2 ), a self-decay product of ferrate (Fe(VI)), on Fe(VI) reactivity has received increasing attention. In this study, we found that calcium peroxide (CaO 2 ) as a slow-releasing reagent of H 2 O 2 could also enhance the Fe(VI) performance for removing sulfamethoxazole (SMX). Compared with sole Fe(VI), sole CaO 2 and Fe(VI)-H 2 O 2 systems, the Fe(VI)-CaO 2 system showed higher reactivity to remove SMX. The radical scavenger and chemical probe test results indicated that the better oxidation performance of Fe(VI)-CaO 2 system than Fe(VI) alone was ascribed to the generation of Fe(Ⅳ) and Fe(Ⅴ) rather than • OH. In addition, the performance of Fe(VI)-CaO 2 system for degradation of contaminants was also superior to Fe(VI)-Na 2 SO 3 , Fe(VI)-NaHSO 3 and Fe(VI)-Na 2 S 2 O 3 systems under the same experimental conditions. Moreover, the effects of critical operating parameters, inorganic anions, inorganic cations, and humic acid on the degradation of SMX by Fe(VI)-CaO 2 system were revealed. The Fe(VI)-CaO 2 system exhibited good applicability in authentic water. Finally, the underlying degradation intermediates of SMX by Fe(VI)-CaO 2 system and their toxicity were confirmed. In conclusion, this study provides a new strategy for enhancing the oxidation capacity of Fe(VI) and comprehensively reveals the oxidation mechanism.
研究领域:
环境科学
·
水处理技术
✓ 已验证
DOI
PubMed
高影响因子
Frontiers in Chemistry
·
2025
·
IF 4.2
Xianbing Zhang,Yuheng Liu,Jiajia Yuan
Metal-organic frameworks (MOFs) are recognized as important Fenton-like materials for environmental remediation. However, their applications are often hindered by slow cycling between Fe (III) and Fe (II). This study aimed to address the slow Fe (III)/Fe (II) cycling limitation of Fe-MOFs through dual modification strategy: bimetallic modification and amino functionalization. A series of NH2-MOF(Fe, Co) catalysts with varying Fe/Co ratios were synthesized via a hydrothermal method and evaluated for sulfamethoxazole (SMX) degradation. The optimized NH2-MOF(Fe, Co) catalyst (Fe/Co ratio = 7:3) exhibited substantially enhanced catalytic performance, with SMX removal rate and rate constant in the H2O2 system being 3.2 and 43.5 times higher than those of the Fe-MOF/H2O2 system, respectively. The catalyst demonstrated robust performance across a wide pH range (3.05–7.00), addressing a common limitation of Fenton-like systems. Physicochemical characterization revealed that the enhanced performance was attributed to two key factors: the synergistic effect between Co and Fe in the bimetallic active center, and improved electron transfer to the central metal due to -NH2 functionalization. These modifications effectively addressed the Fe (III)/Fe (II) redox cycling limitation. The proposed reaction mechanism provides insights into SMX degradation pathways in the NH2-MOF(Fe, Co)/H2O2 system. This study presents an efficient and stable MOF-based Fenton-like catalyst with potential applications in wastewater treatment and environmental remediation.
研究领域:
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF ELECTROANALYTICAL CHEMISTRY
·
2024
·
IF 4.1
Yining Dong,Ping Song,Ce Han,Weilin Xu
In this paper, Pt-Fe alloy with low-content of Pt (2 %) was distributed uniformly over the porous Fe/NC substrate treated by nitric acid etching, with small amount of metallic Fe and Pt nanoparticles. The optimized Pt-Fe alloy on Fe/NC substrate showed higher ORR performance with the E 1/2 of around 0.83 V vs. RHE as well as faster catalytic kinetics. In addition, the catalytic activity has not been decayed through an accelerated durability test after 5000 cycles CVs, indicating better catalytic stability for the alloying catalyst. The introduction of Pt elements into Fe/NC substrate increased the numbers and species of ORR active sites, invoking higher ORR activity comparing with isolated Fe/NC catalyst. The acid etching provided more defects for the substrate to anchor the active sites stably. Moreover, the synergistic effect originated from the alloying of Pt and Fe modulated the electronic structure of Pt, increasing the ORR activity with low yield of H 2 O 2 . This decreasing H 2 O 2 yield can weaken the Fenton reaction to prevent the dissolution of Fe in the acid solution, which can improve the stability of the catalysts to meet the commercial needs for PEMFC.
研究领域:
材料科学
·
电化学
·
燃料电池研究
✓ 已验证
产品关联
DOI
高影响因子
Journal of Materials Chemistry A
·
2015
·Vol. 3
·期 7
·3988-3994
·
IF 7.443
Xiang Li,Fangyuan Gai,Buyuan Guan,Ye Zhang,Yunling Liu,Qisheng Huo
Fe@C core–shell particles were successfully synthesized by coating Fe2O3 particles with resorcinol–formaldehyde resins (RFs) and then calcining to make the RFs carbonize, and at the same time to reduce the core to Fe. Furthermore, we designed and synthesized Fe@C yolk–shell particles to increase the number of active sites on the Fe surface. Compared with pure Fe material, the Fe in these particles possesses a high surface area without serious aggregation. Tests to remove 4-chlorophenol suggest that both these kinds of particles can degrade chlorophenol rapidly and thoroughly based on a Fenton-like reaction. Using Fe@C yolk–shell particles, the chlorophenol can be degraded to a concentration below the HPLC detection limit (<0.5 mg l−1) within 12 minutes. The magnetic properties and good stability of Fe@C endow it with promising potential for water treatment.
研究领域:
材料科学
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
ENVIRONMENTAL RESEARCH
·
2025
·
IF 7.7
Ning Liu,Ti-Bo Fang,Ling-Xi Zhao,Na Li,Xiang-Feng Chen,Ru-Song Zhao
Naphthalene acetic acid (NAA) is an auxin plant growth regulator (PGR) and widely used to regulate the growth process of plants. As excessive NAA enter the environment, it damages the ecological environment and endangers human life and health. Layered bimetallic hydroxides (LDHs) are widely used for the adsorption of pollutants due to their large surface area and excellent structural properties. Based on the classical Fe 3 O 4 @MgAl-LDH material, Fe 3 O 4 @FeMgAl-LDHs were synthesized by adding different contents of Fe element to adsorb NAA in water. The morphology and properties of Fe 3 O 4 @FeMgAl-LDHs and the effect of Fe on adsorption efficiency were studied. The adsorption process and adsorption mechanism of NAA were analyzed. The results indicated that the content of Fe element will affect the adsorption effect of NAA by influencing the specific surface area and adsorption sites of Fe 3 O 4 @FeMgAl-LDHs. The maximum adsorption capacity for NAA can reach 330.1 mg/g when the proportion of Fe is 0.50. Exploring the adsorption mechanism, Fe 3 O 4 @FeMgAl-LDHs achieved efficient removal of NAA through hydrogen bonding, van der Waals forces, anion exchange, and electrostatic interactions. The adsorption efficiency of various PGRs were deeply explored. Fe 3 O 4 @FeMgAl-LDH (Fe-0.50) has good adsorption and regeneration ability for various PGRs. Therefore, by exploring the influence of different Fe ratios on the adsorption efficiency of the Fe 3 O 4 @FeMgAl-LDH, the adsorption performance of the material can be improved, making it have greater application advantages in wastewater treatment containing drugs.
研究领域:
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Journal of Environmental Sciences
·
2024
·
IF 5.9
Zheng Qi,Zaihui Huang,Chunguang Liu
Advanced oxidation processes (AOPs) exhibit significant potential for water disinfection due to their generation of large quantities of highly oxidizing free radicals. However, the neglect of viable but nonculturable (VBNC) cells obscures their true disinfection efficacy and potential environmental health risks. Therefore, the study evaluated the disinfection effectiveness and mechanisms of typical AOPs, including Fe/H 2 O 2 , Fe/persulfate (PS), and O 3 , from the perspective of the production of VBNC bacteria. The results indicate that Fe/PS exhibits the strongest bacterial inactivation rate (99.94%), and the cells lose their ability to reactivate. Fe/H 2 O 2 and O 3 induce more cells to enter the VBNC state compared to Fe/PS. Moreover, different AOPs result in varying levels of free radical production and utilization efficiency, with SO 4 •− and O 3 exhibiting greater selectivity in deactivating bacteria compared to HO • . The inhibition of VBNC bacteria production by Fe/PS treatment may be attributed to the combined action of HO • and SO 4 •− on microorganisms, leading to oxidative stress and metabolic disruption in bacteria through the inhibition of biofilm formation and aminoacyl-tRNA biosynthesis ( p < 0.05), thereby causing direct bacterial death rather than entry into the VBNC state. In contrast, Fe/H 2 O 2 and O 3 result in the upregulation of the metabolism of alanine, aspartate, and glutamate, as well as styrene degradation capacity by the bacteria, leading to the production of more VBNC bacteria. Overall, the study offers insights into mitigating potential biological risks in water disinfection and developing environmentally friendly and efficient disinfection technologies.
研究领域:
环境科学
·
微生物学
✓ 已验证
DOI
PubMed
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.
研究领域:
微生物学
·
环境科学
✓ 已验证
DOI
PubMed
高影响因子
Journal of Environmental Chemical Engineering
·
2021
·
IF 5.909
Qin He,Yangjie Fu,Xueying Ge,Abdullah M. Al-Enizi,Ayman Nafady,Qi Wang,Shengqian Ma
Novel Fe-BDC/Fe-2MI heterojunction (H 2 BDC: terephthalic acid, 2MI: 2-methylimidazole) was prepared via a one-pot solvothermal method. Herein, mixed ligands (H 2 BDC and 2MI) was applied to form complex with Fe(III). Interestingly, the presence of 2MI can regulate the structure of Fe-BDC. Spindle-like MIL-88B(Fe) was observed in Fe-BDC/Fe-2MI composite, while MIL-53(Fe) was identified in naked Fe-BDC. By employing photoelectrochemical characterizations, Fe-BDC/Fe-2MI was optimized at an initial molar ratio of 1:0.5:10 for Fe(III):H 2 BDC:2MI, which exhibited the highest photocurrent response, lowest charge transfer resistance, and fastest surface reaction kinetics as compared to the individual Fe-BDC and Fe-2MI. Due to the formation of the heterojunction which lead to beneficial photoelectrochemical properties, the as-prepared samples exhibited boosted photocatalytic activity for Cr(VI) reduction. The calculated pseudo-first-order rate constant ( k ) was 0.046 min −1 for Fe-BDC/Fe-2MI, which was 15.3 and 6.6 times that of Fe-BDC (0.003 min −1 ) and Fe-2MI (0.007 min −1 ), respectively. Moreover, the optimized Fe-BDC/Fe-2MI demonstrated superior performance with negligible loss in activity after 4 cyclic runs.
研究领域:
材料科学
·
环境科学
·
化学
✓ 已验证
产品关联
DOI
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.
研究领域:
催化
·
化学工程
·
材料科学
·
环境化学
✓ 已验证
DOI
高影响因子
JOURNAL OF PHOTOCHEMISTRY AND PHOTOBIOLOGY A-CHEMISTRY
·
2023
·
IF 4.3
Yunxin Shi,Liying Wang,Xin Miao,Zhenzhu Cao,Yongfeng Zhang,Lin Cheng,Jucai Yang
A series of donut-like nanostructured heterojunction materials are first synthesized via one-step solvothermal method to improve the photocatalytic efficiency for the environmental pollutants. The unique donut-like Fe-doped-BiOCl@Fe-MOF heterojunction with uniform size guarantees suitable surface area and many active sites for the model pollutant. The optimal photocatalytic efficiency is shown in degradation of RhB (99.0 %, 90 min) and TC (90.4 %, 90 min) solution, which had higher photocatalytic efficiency than a variety of similar materials previously reported. The result revealed that the enhancing photocatalytic activity is mainly depended on the synergistic effect of Fe-MOF and Fe-doped BiOCl. The possible mechanism is further studied, which shown h + and O 2 − are the primary active species in the degradation process of RhB and TC solution. Meantime, Fe-doped BiOCl@Fe-MOF with the excellent reusability and stability. After the fourth cycle, the degradation rate of RhB solution can still be as high as 86.4 %. In this work, we provide a higher efficiency heterojunction photocatalytic material by varying the organic ligand content.
研究领域:
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2021
·Vol. 46
·期 2
·739-746
·
IF 3.591
Tao Wang,Xiqing Liu,Mei Liu,Runhua Liao,Hongquan Zhan,Xiaoxue Qi,Yongqing Wang,Yanju Huang
Black TiO2 and metal–organic frameworks (MOF) are great materials with light-harvesting ability, redox power and consequently catalytic activity. Here, the integration of MIL-100(Fe) with TiO2(B) composite was designed for photocatalytic application, which greatly promoted light-harvesting and charge transfer. As expected, the integrated TiO2(B)/MIL-100(Fe) composite showed high photocatalytic activity due to unique Fe–O–Ti bonds that were constructed, which acted as an electronic tunnel to reduce electronic transfer resistance between MIL-100(Fe) and TiO2(B). In addition, the presence of Fe–O clusters in MIL-100(Fe) can also promote the charge dissociation and improve catalytic activity via the Fe3+/Fe2+ redox cycle. This achievement would help us to understand and design charge transfer pathways in the integration of MOF/semiconductor photocatalysts.
研究领域:
材料科学
·
光催化
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）