Sustainable Materials and Technologies
·
2024
·
IF 8.6
Yijun Chen,Meina Cheng,Hailiang Yang,Sanjian Ma,Long Jin,Zixia Lin,Xin Liu
The traditional Fenton process has two issues that hinder its further application and promotion. One is the generation of large amounts of iron sludge. The other is the safe storage and transport of explosive H 2 O 2 . The problems could be solved by accelerating to regenerate Fe(II) and realizing to self-generate H 2 O 2 . The key to the solution lies in the use of reducing active hydrogen [H] to supply electrons. The effect of different loading methods of Pd 0 nanoparticles (NPs), active centres for [H] generation, on the catalytic performance is unknown. Herein, the Pd/UiO-66(Zr) (Pd 0 NPs loaded on the surface of UiO-66(Zr)) and Pd@UiO-66(Zr) (Pd 0 NPs confined into the pores of UiO-66(Zr)) were synthesized. It confirmed that the [H] could be used to promote to regenerate Fe(II) and self-generate H 2 O 2 . Using only a trace amount of ferrous (25 μM) and without H 2 O 2 , the trimethoprim (20 mg·L −1 ) could be thoroughly removed within 90 min. Moreover, the stability of Pd@UiO-66(Zr) was slightly superior to that of Pd/UiO-66(Zr) because of the confinement effect of pore wall on Pd 0 NPs, as well as the interception effect on the intermediate products that can be complexed with Pd 0 NPs.
研究领域:
环境科学
·
催化化学
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产品关联
DOI
高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2022
·
IF 5.518
Zhongmin Feng,Jingwen Yang,Liangyuan Zhu,Ting Sun
Fe–based metal–organic frameworks (Fe–MOFs) have been widely used in heterogeneous Fenton-like processes. However, the catalytic performance of Fe-MOFs is limited by the relatively slow Fe (III)/Fe (II) redox cycle. For Fe-MOFs, increasing the interfacial electron transfer and reducing the electron density of Fe-MOFs are expected to accelerate the reduction of Fe (III) and improve the catalytic performance. Here, by mixing Fe/Cu metal species and introducing bromine groups, we successfully prepared bromine-functionalized bimetallic MOFs–FeCu(BDC-Br), and we used it to effectively degrade phenol in a Fenton-like process. Compared with most other catalysts, FeCu(BDC-Br) achieved a higher phenol degradation kinetic rate of 0.106 min –1 at a low dose. Effects of pH, humic acid (HA) and coexisting ions on the degradation of phenol were examined. The FeCu(BDC-Br) /H 2 O 2 system can remove phenol in the near neutral pH range of 4–6 and 0–50 mg/L HA range. Chloride ion , sulfate, or phosphate with a concentration of 100 mg/L showed an inhibitory effect on the catalytical performance of phenol degradation. This work provides insights for the preparation of Fe-MOFs Fenton-like catalyst in water/wastewater treatment.
研究领域:
环境科学
·
催化材料
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DOI
高影响因子
WATER RESEARCH
·
2022
·
IF 13.4
Zheng-Yu Dong,Yi-Li Lin,Tian-Yang Zhang,Chen-Yan Hu,Yang Pan,Renjie Pan,Yu-Lin Tang,Bin Xu,Nai-Yun Gao
To improve the performance of the conventional coagulation process, a permanganate (Mn(VII)) pre-oxidation combined with Fe(III)/peroxymonosulfate (PMS) coagulation process (Mn(VII)-Fe(III)/PMS) that can significantly improve the removal of dissolved organic carbon (DOC), turbidity, and micropollutants is proposed in this study. Compared with conventional Fe(III) coagulation, the Mn(VII)-Fe(III)/PMS process can also significantly enhance the removal of iohexol and sulfamethoxazole in raw water. During this process, the primary reduction product, Mn(IV), after Mn(VII) pre-oxidation was adsorbed on the floc surfaces and involved in the Fe(III)/PMS process. The natural organic matter (NOM) in raw water mediated the redox cycle of iron. The synergistic effect of NOM, Fe, and Mn facilitated the redox cycle of Mn(III)/Mn(IV) and Fe(III)/Fe(II) to promote the activation of PMS. The sulfate radical (SO 4 •− ) played an important role in the degradation of micropollutants. The formation potential of the detected volatile disinfection by-product (DBP) during the subsequent chlorination was reduced by 21.9% after the Mn(VII)-Fe(III)/PMS process. This study demonstrated the promising application of the Mn(VII)-Fe(III)/PMS process for coagulation and micropollutant control and illustrated the reaction mechanism. This study provides guidance for improving conventional drinking water treatment processes.
研究领域:
环境科学
·
水处理工程
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DOI
PubMed
高影响因子
WATER RESEARCH
·
2018
·
IF 7.051
Wei Ding,Jing Xu,Tao Chen,Chengshuai Liu,Jinjun Li,Feng Wu
Previous studies have shown that the oxidation of Fe(II) by molecular oxygen can lead to the co-oxidation of As(III) at neutral pH. However, the mechanism of As(III) oxidation in the presence of Fe(II) with respect to the interaction between As(III) and Fe(II) is still unclear. In this work, we examined the oxidation of As(III) in the presence of Fe(II) in air-saturated water, which is affected by pH, co-existing phosphate, and scavengers ( tert -butanol, superoxide dismutase, catalase and dimethylsulfoxide). Results confirm that the formation of the Fe(II)–As(III) complex (formation constant, K Fe(II)–As(III) = 10 3.86 M –1 ) plays an extremely important role in the initial stage of As(III) oxidation at pH 7.25. The oxidation of Fe(II)–As(III) promotes the production of H 2 O 2 and colloidal ferric hydroxide. H 2 O 2 reacts with the Fe(II)–As(III) complex through oxidizing Fe(II) to Fe(IV), which then causes the partial oxidation (ca. 50%) of As(III). The other part of As(III) oxidation by H 2 O 2 occurs, in the form of Fe(III)–As(III) complex, through direct electron transfer from As(III) to H 2 O 2 but not through Fe(IV). This work provides new mechanistic insight into arsenic and iron redox chemistry in the environment and furthers our understanding of Fenton reactions at neutral pH.
研究领域:
环境化学
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氧化还原化学
·
水处理
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产品关联
DOI
PubMed
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2020
·
IF 16.683
Cong Gao,Yan Su,Xie Quan,Virender K. Sharma,Shuo Chen,Hongtao Yu,Yaobin Zhang,Junfeng Niu
Heterogeneous Fenton-like reaction was a promising approach for generating •OH. However, the heterogeneous catalysts generally exhibited low activity because of slow reduction of Fe(III) in Fe(III)/Fe(II) redox cycle. Here, decreasing electron density was expected to quicken Fe(III) reduction and consequently enhance the catalytic activity of heterogeneous catalysts. This hypothesis was validated by the enhanced hydroxyl radicals generation and accelerated Fe(III) reduction on MIL-88B(Fe)-X (2-X-terephthalic acid, X = NH 2 , CH 3 , H, Br and NO 2 ) by reducing electron density of Fe(III) with substituent of higher electrophilicity. MIL-88B(Fe)-NO 2 , with the substituent of highest electrophilicity among these catalysts, has the lowest electron density of Fe(III) and highest redox potential ( E Fe(III)/Fe(II) = 0.35 V). As a result, it exhibited the best catalytic performance, which was 1.7–20 times higher than that for other MIL-88B(Fe)-X and was comparable to that of homogeneous Fe 2+ . This study provides scientific basis for rational construction of highly effective heterogeneous Fenton-like catalyst.
研究领域:
环境科学
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催化化学
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产品关联
DOI
高影响因子
Science Advances
·
2024
·Vol. 10
·期 28
·
IF 11.7
Hanrong Li,Yifan Li,Lingpu Zhang,Nan Wang,Dong Lu,Dongsheng Tang,Yitong Lv,Jinbo Zhang,Heben Yan,He Gong,Ming Zhang,Kaili Nie,Yi Hou,Yingjie Yu,Haihua Xiao,Chaoyong Liu
Celastrol (CEL), an active compound isolated from the root of Tripterygium wilfordii, exhibits broad anticancer activities. However, its poor stability, narrow therapeutic window and numerous adverse effects limit its applications in vivo. In this study, an adenosine triphosphate (ATP) activatable CEL-Fe(III) chelate was designed, synthesized, and then encapsulated with a reactive oxygen species (ROS)–responsive polymer to obtain CEL-Fe nanoparticles (CEL-Fe NPs). In normal tissues, CEL-Fe NPs maintain structural stability and exhibit reduced systemic toxicity, while at the tumor site, an ATP-ROS–rich tumor microenvironment, drug release is triggered by ROS, and antitumor potency is restored by competitive binding of ATP. This intelligent CEL delivery system improves the biosafety and bioavailability of CEL for cancer therapy. Such a CEL-metal chelate strategy not only mitigates the challenges associated with CEL but also opens avenues for the generation of CEL derivatives, thereby expanding the therapeutic potential of CEL in clinical settings.
研究领域:
药理学
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纳米技术
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癌症研究
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药物递送系统
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产品关联
DOI
PubMed
高影响因子
ACS Applied Materials & Interfaces
·
2021
·
IF 9.229
Dan Mu,Wenshen Wang,Jianhui Li,Pin Lv,Renyuan Liu,Ying Tan,Chongxia Zhong,Yu Qi,Xuan Sun,Yihai Liu,Song Shen,Yuyu Li,Biao Xu,Bing Zhang
Macrophage accumulation is central to the pathogenesis of atherosclerotic plaques. Reducing macrophages in plaques is an appealing approach to attenuate the development of atherosclerosis. Chemodynamic therapy, specifically inhibiting hydrogen peroxide (H2O2)-rich cells in slightly acidic microenvironment, has emerged as a new method in tumor treatment. Herein, we manufactured ultrasmall dopamine-modified hyaluronic acid (HD)-stabilized Fe(III)-tannic acid nanoparticles (HFTNPs). HFTNPs can specifically accumulate in inflammatory macrophages in atherosclerotic plaques, provide brighter magnetic resonance images, promote reactive oxygen species (ROS) generation, and induce the death of inflammatory macrophages without damaging normal cells and tissues. In conclusion, HFTNPs have a tremendous potential as safe and effective diagnostic and therapeutic reagents for atherosclerosis.
研究领域:
纳米技术
·
心血管疾病
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诊疗一体化
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生物医学工程
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产品关联
DOI
PubMed
高影响因子
RSC Advances
·
2017
·Vol. 7
·期 46
·28637-28646
·
IF 3.108
Pei Song,Lisha Zhang,Hao Long,Meng Meng,Ting Liu,Yongmei Yin,Rimo Xi
In this research, we developed a multianalyte fluorescence sensing system through a carbon dots (CDs)-based fluorescent probe that can specifically recognize Fe(III) by fluorescence quenching. The CDs prepared using black tea by a hydrothermal method show outstanding properties like low cytotoxicity, high photostability, excellent biocompatibility, and high sensitivity. It was found that the fluorescence of CDs can be quenched by micromolar concentrations of Fe(III) in both aqueous solutions as well as living cells. It is well known that glucose can be oxidized by glucose oxidase (GOx) to release H2O2, which, in turn, can oxidize Fe(II) to Fe(III). Based on this consideration, a multianalyte sensing system was established. Therefore the quantitative analysis of Fe(III), H2O2, and glucose with detection limits of 0.25 μM, 0.82 μM, and 1.71 μM, respectively, was achieved by the simple and cost-effective multianalyte CDs sensing system constructed. The sensing system showed high photostability and negligible cytotoxicity toward HeLa cells, which enables it to be applied in the visualization of Fe(III) or H2O2 in living cells. The system was further applied in the detection of Fe(III) or glucose in human serum, and satisfactory results were obtained.
研究领域:
分析化学
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材料科学
·
生物化学
·
生物医学工程
✓ 已验证
产品关联
DOI
高影响因子
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
TALANTA
·
2018
·
IF 4.244
Hao Zhang,Chen Nie,Jiahui Wang,Ruifang Guan,Duxia Cao
Organic-inorganic hybrid fluorescent microspheres (OI-FMs) without typical fluorophores were prepared. Fluorescence quantum yield of OI-FMs is up to 70.0% after being heated in an oven at 120 °C (named as OI-FMs-120). Interestingly, OI-FMs-120 shows different detection performances in different solvents. It can be used for qualitative and quantitative detection of Fe 3 + with a detection limit of 37.8 nM in absolute ethanol. While in aqueous solution, it can be applied as an ON-OFF-ON fluorescent probe . Fluorescence of the probe is quenched by Hg 2 + and later recovered by biothiols. The detection limit is as low as 34.9 nM for Hg 2 + , 91.0 nM for Cys, 0.12 μM for Hcy and 0.13 μM for GSH in aqueous medium, respectively.
研究领域:
分析化学
·
材料科学
·
环境科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Acta Biomaterialia
·
2022
·
IF 10.633
Longyi Nan,Jie Liu,Chao Liu,Peng Quan,Jianpeng Guo,Liang Fang
Pressure-sensitive adhesives are critical to the product's safety, efficacy, and quality in transdermal drug delivery systems. However, many defects of transdermal patches ( e.g. , insufficient adhesion, patch displacement, and “dark ring” phenomenon) remain. Herein, the N -[tris(hydroxymethyl)methyl]acrylamide (NAT)-modified acrylic pressure-sensitive adhesive coordinated with Fe(III) (AA-NAT/Fe 3+ ) was creatively proposed. Results demonstrated that the adhesiveness and cohesiveness of the optimized AA-NAT/Fe 3+ were higher by 1.8- and 9.7-fold, respectively, than those of commercially available DURO-TAK® 87-4098 due to the hydrogen bonding interaction of NAT-skin interface and coordination of NAT-Fe 3+ . Moreover, compared with that of DURO-TAK® 87-4098, the adhesion time of AA-NAT/Fe 3+ on the human forearm was remarkably prolonged, and no “dark ring” phenomenon was observed for AA-NAT/Fe 3+ after removal. After clonidine (CLO) was loaded into AA-NAT/Fe 3+ , controlled drug release and a drug transdermal behavior were endowed for CLO@AA-NAT/Fe 3+ in vitro and in vivo . AA-NAT/Fe 3+ still maintained superiority in adhesion and cohesion properties after CLO loading. These observations would contribute to the development of pressure-sensitive adhesives with outstanding adhesion and cohesion for transdermal patches. Statement of significance This N -[tris(hydroxymethyl)methyl]acrylamide-modified acrylic pressure-sensitive adhesive coordinated with Fe(III) has enhanced adhesion and cohesion properties, which provide a simple but effective strategy to solve the problems ( e.g. , insufficient adhesion, patch displacement, and “dark ring” phenomenon) in existing transdermal patches.
研究领域:
材料科学
·
药剂学
·
生物医学工程
✓ 已验证
DOI
PubMed
高影响因子
MICROCHIMICA ACTA
·
2017
·Vol. 184
·期 7
·2291-2298
·
IF 4.58
Wu Huifang,Jiang Jiahui,Gu Xiaoting,Tong Changlun
Nitrogen and sulfur co-doped carbon quantum dots (N,S-CQDs) with a high quantum yield (69%) and excellent photoluminescent properties were synthesized via a facile hydrothermal method using citric acid and cysteine as precursors. The cytotoxicity of N,S-CQDs was evaluated through the MTT assays using HepG2 cells as the target. The cell viability is still >95% after a 24 h incubation with particles in a concentration of up to 300 μg·mL −1 , thereby indicating low cytotoxicity and excellent biocompatibility of N,S-CQDs. The emission spectra of the N,S-CQDs are nearly independent of the excitation wavelengths in the range from 280 to 380 nm and have the strongest fluorescence emission centered at 415 nm. Co-doping with N and S promotes the electron-transfer rate and coordination interaction between N,S-CQDs and Fe(III) ions which acts as a quencher of fluorescence. Fluorescence can be recovered, however, by addition of L-Cys. Hence, the N,S-CQDs act as a highly sensitive and selective “turn-off-on” probe for the determination of Fe(III) or Cys. The limits of detection are 14 nM for Fe(III) and 0.54 μM for Cys. The interferences by 17 common metal ions and heavy metal ions, 12 other quenchers and 16 amino acids were investigated and found to be tolerable. The probe was successfully applied for cellular imaging of Fe(III) in HepG2 cells by using fluorescence microscopy.
Nitrogen and sulfur co-doped carbon quantum dots (N,S-CQDs) with a high quantum yield of 69% were prepared through a facile one-step hydrothermal method. They are shown to be a highly sensitive and selective fluorescent “turn-off-on” probe for Fe(III) ions and cysteine.
研究领域:
分析化学
·
生物医学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）