SCIENCE OF THE TOTAL ENVIRONMENT
·
2023
·
IF 9.8
Dongqin He,Dongli Wang,Hongwei Luo,Yifeng Zeng,Ganning Zeng,Jun Li,Xiangliang Pan
The most important factor that restricts the decomposition of H 2 O 2 in the Fe 3+ /H 2 O 2 reaction is the slow cycling efficiency of reducing Fe 3+ to Fe 2+ . In this study, the addition of tungsten disulfide (WS 2 ) as a co-catalyst achieved a rapid cycling of the reaction rate-limiting step and a significant enhancement of H 2 O 2 decomposition, which resulted in the effective degradation of acetaminophen (APAP). Results show that 99.6% of APAP (5 mg L −1 ) could be degraded by H 2 O 2 /Fe 3+ /WS 2 system within 2.5 min. The conversion of Fe 3+ to Fe 2+ occurred mainly on the surface of WS 2 due to the redox reaction of the exposed W 4+ active sites with Fe 3+ after the unsaturated S atoms were bound to protons. Electron paramagnetic resonance (EPR) and radical quenching experiments evaluated the contribution of hydroxyl radical (•OH) and superoxide radical (O 2 • − ) in the degradation of pollutants. WS 2 showed good recoverability after four cycles of the reaction. This study provides a new perspective to improve the efficiency of Fe 3+ /H 2 O 2 and provides a reference for the involvement of transition metal sulfides in advanced oxidation processes (AOPs).
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高影响因子
Foods
·
2023
·Vol. 12
·期 14
·2794
·
IF 5.2
Shushan Gao,Chonghao Zhu,Liangfei Ma,Chenghai Liu,Hongqiong Zhang,Shengming Zhang
To reduce the usage of petroleum-based plastic products, a lignin-based film material named aminated lignin/Fe(III)/PVA was developed. The mixture of 8 g lignin, 12 mL diethylenetriamine, 200 mL NaOH solution (0.4 mol·L−1), and 8 mL formaldehyde was heated at 85 °C for 4 h; after the aminated lignin was impregnated in the Fe(NO3)3solution, a mixture of 3 g aminated lignin/Fe(III), 7 g PVA, and 200 mL NaOH solution (pH 8) was heated at 85 °C for 60 min; after 2 mL of glycerin was added, the mixture was spread on a glass plate to obtain the aminated lignin/Fe(III)/PVA film. This film demonstrated hydrophobicity, an UV-blocking function, and a good slow-release performance. Due to the formation of hydrogen bonds between the hydroxyl groups of lignin and PVA, the tensile strength, the elongation at break, and the fracture resistance of the film were 9.1%, 107.8%, and 21.9% higher than that of pure PVA film, respectively. The iron content of aminated lignin/Fe(III)/PVA was 1.06 wt%, which mainly existed in a trivalent form. The aminated lignin/Fe(III)/PVA film has the potential to be used as a food packaging material with anti-ultraviolet light function and can also be developed as other packaging materials, such as seedling bowls, pots for transplanting, and coating films during transport.Keywords:lignin;polyvinyl alcohol;Fe(III);packaging material;slow-release function
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2023
·
IF 11.4
Yanjing Wang,Minglei Song,Jianrong Wei,Jie You,Siping Chen,Shuangyin Wang,Yanyong Wang
Electrochemically mediated Fe(II)/Fe(III) redox-coupled uranium extraction can efficiently reduce the cell voltage of electrochemical uranium extraction (EUE). How to regulate the surface structure to enhance the uranium acyl ion adsorption capacity and strengthen the Fe(II)/Fe(III) redox cycle process is crucial for EUE. In this work, we developed surface sulfated nanoreduced iron (S-NRI) for EUE and exhibited improved properties for EUE at an ultralow cell voltage (−0.1 V). Compared with a nanoreduced iron (NRI) adsorbent, S-NRI displayed faster electrochemical extraction kinetics properties and higher extraction efficiency and capacity for uranium. In a more complex seawater electrolyte containing uranyl ion concentration ranging from 1 to 20 ppm, the removal efficiency could reach almost ∼100% after EUE for 24 h. At a higher 50 ppm uranium acyl ion concentration in a seawater electrolyte, S-NRI exhibited higher extraction capacity (755.03 mg/g), which is better than 528.53 mg/g of NRI at a cell voltage of −0.1 V. Outstanding EUE property could be attributed to the fact that sulfate species (M–SO42–) on the S-NRI surface not only enhanced selective adsorption of uranyl ions but also strengthened the Fe(II)/Fe(III) redox cycle, which accelerated electron transfer between Fe(II) and U(VI), promoted the regeneration of Fe(II) active sites, and finally enhanced the EUE property.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Chaoqun Tan,Wangqi Yu,Hong Mei,Kaiyang Chen,Tianhui Xu,Huiming Xiang,Yiming Feng,Lin Deng
In this study, Fe(III) catalyzed calcium peroxide (CaO 2 , CP) Fenton-like process assisted by crystal boron (C-boron) was applied for in situ chemical oxidation. Flunixin meglumine (FMME), aspirin (ASA), nitrobenzene (NB) and benzoic acid (BA) were selected as target contaminants. Pollutants decomposition by the CP/Fe(III) and C-boron/CP/Fe(III) systems was proposed in terms of diverse parameters, including C-boron dosage, pH, and temperature, with regard to the pseudo-first-order kinetic model (R 2 > 0.95). About 26.8% of 20 μM FMME was removed by 0.5 mM CP and 0.5 mM Fe(III) after 20 min at pH 4.0, whereas 90.4% of FMME was decomposed in the C-boron/CP/Fe(III) system with 100 mg/L C-boron. The removal rates of the other three pollutants were also improved to varying degrees. The k obs of the C-boron/CP/Fe(III) system for these four pollutants degradation at pH 4.0 was approximately 4.1 ∼ 5.3 times higher compared to the CP/Fe(III) system. Electron paramagnetic resonance and quenching experiments indicated that OH, O 2 − and 1 O 2 were present in both systems and contribution of OH was 71.3% at initial pH 4.0 in C-boron/CP/Fe(III) system, suggesting that it was the main reactive oxygen species for the contaminants elimination. Furthermore, experiments on the characterization of C-boron showed great reactivity and stability. This work manifested the promotion mechanism of pollutant degradation in the C-boron/CP/Fe(III) system.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Wenjuan Wang,Yanfang Huang,Hongfei Ma,Lulu Kou,Bingbing Liu,Hu Sun,Shuzhen Yang,Guihong Han
Eutrophication of water bodies due to excessive phosphate release is becoming a serious issue. Herein, an Fe(III)-fulvic acid carrier with a synergistic effect with a surfactant was fabricated for the first time by a solvothermal method and evaluated for the removal of phosphate via an adsorption flotation strategy. This study indicated that the solvothermal method significantly improved the specific surface area, pore structure and active site distribution of the adsorption carrier and initially enhanced its adsorption performance. In addition, based on the synergistic effect of Fe(III)-fulvic acid and cetyltrimethylammonium bromide (CTAB), the competitive effect of surfactant and target ion in the adsorption flotation process was effectively broken. The theoretical maximum adsorption capacity of Fe(III)-fulvic acid increased from 169.205 ± 0.846 mg·g −1 to 274.725 ± 0.550 mg·g −1 after introducing CTAB, which was improved by 62.32% relative to the adsorption stage. FTIR and XPS analyses verified that the re-enhancement of the adsorption performance of the adsorbent carrier was mainly attributed to the chemisorption of CTAB with the carboxyl groups on the carrier surface, which intensified the electrostatic attraction and ligand exchange between the carrier and phosphate. Additionally, fractal and EDLVO theories revealed that CTAB could obviously improve the floatability of the carrier particles. Concurrently, the regeneration studies suggested that Fe(III)-fulvic acid possessed stable adsorption and flotation separation performance after three cycles. Overall, the Fe(III)-fulvic acid fabricated in this study not only realized the resource utilization of fulvic acid but also had practical application potential for the purification of oxyanions.
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WATER RESEARCH
·
2023
·
IF 12.8
Yu Wang,Yanchun Deng,Lu Yao,Xin Yang
The omnipresence of natural organic matter (NOM) in water bodies traditionally hinders the degradation of trace organic contaminants (TrOCs) in peroxymonosulfate (PMS)-based advanced oxidation processes (AOPs). This study elucidates the positive role of NOM in enhancing the degradation of TrOCs through the Fe(III)/PMS process. During this process, NOM reduces Fe(III), yielding semiquinone-like radical (NOM • ) and concurrently forming NOM-Fe(III) colloids. In addition to the Fe(II)-mediated activation pathway, Fe(III) sites on NOM-Fe(III) colloids effectively transfer electrons from NOM • or some redox-active moieties to PMS, resulting in the generation of long-lived colloid-bound SO 4 •− , which can readily undergo hydrolysis to produce HO • . The stabilization of SO 4 •− and HO • by NOM-Fe(III) colloids, combined with their moderate adsorption of TrOCs, results in surface-confined reactions that significantly enhance TrOC removal, despite the presence of concurrent quenching reactions between radicals and NOM. Further, the significant positive correlation between the phenolic contents of eight NOM types and TrOC degradation kinetics suggests phenolic moieties as the primary electron source for PMS activation. By in-situ utilizing NOM in raw water, a PMS-amended iron coagulation process with 0.2 mM Fe(III) and PMS effectively removes 90–100 % of six coexisting TrOCs. This study unveils the previously unrecognized role of colloid-bound radicals in decontamination processes, offering valuable insights into harnessing NOM's influence in advanced oxidation water treatment processes.
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Environmental Science-Nano
·
2023
·
IF 7.3
Jinli Qiu,Huifang Chan,Wenting Zheng,Yao Feng,Fuqiang Liu
The design of metal–organic framework-derived metal oxides/sulfides is an effective approach for water remediation. A series of Fe–Ce composites (Fe–Ce–S–N) with cluster-like morphology were prepared with prussian blue analogue (PBA) as the precursor in a hydrothermal process. S doping promoted the conversion of Fe(III) to Fe(II), which greatly improved the performance of the Fenton-like reaction. The optimized Fe–Ce–S–N catalyst exhibited superior catalytic activity towards sulfamethoxazole (SMZ) degradation (18.63 mgSMZ gcat−1 min−1), showing the largest k value (0.1862 min−1), which was 2.1 and 8.1 times higher than that of Fe–Ce–S–H and Fe–Ce–N, respectively. Moreover, the Fe–Ce–S–N catalyst displayed a remarkable reusability, stability and adaptability in Fenton-like systems. Overall, this work provides new insights into extending novel PBA-derived catalysts to significantly improve heterogeneous Fenton-like performances.
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Journal of Environmental Chemical Engineering
·
2023
·
IF 7.7
Meiling Chen,Lin Ding,Shijun Zhu,Xiuqin Xiong,Xinkai Yuan,Yanhua Peng,Liming Yang,Hui Shi,Penghui Shao,Xubiao Luo
The slow Fe(II)/Fe(III) cycle during the Fenton reaction process strongly impedes oxidation efficiency in practical applications. In this study, an activated carbon (AC) assisted Fenton reaction system was used to treat electroplating wastewater containing Ni-ethylenediaminetetraacetic acid (Ni-EDTA). AC was found to enhance the removal of Ni-EDTA in Fenton/Fenton-like reactions. The reported results revealed that AC could effectively promote the regeneration of Fe(II) from Fe(III) species via electron transfer to improve the reaction rather than directly enhancing the H 2 O 2 decomposition to accelerate the production of hydroxyl radicals (•OH). Quenching experiments and EPR also demonstrated that •OH and •O 2 − took part in the radical oxidation process, in which the contribution of •OH was dominant. XPS and FT-IR analysis further confirmed that the carbonyl group (C O) on the surface of AC could indeed act as the dominant active site and an electron donor to directly reduce Fe(III). In addition, electrochemical tests indicated that AC could increase the oxidation potential of Fe(III) to boost the reaction between Fe(III) and H 2 O 2 , thus enabling the transfer of electrons from H 2 O 2 to Fe(III) to facilitate the Fe(II)/Fe(III) cycle. This study might contribute to a new insight into the mechanisms of AC-catalyzed Fenton oxidation processes for the decomplexation heavy metal-EDTA.
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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.
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Nano Research
·
2020
·Vol. 13
·期 1
·273-281
·
IF 8.183
Zhang Tao,Jiang Zhenqi,Chen Libin,Pan Chunshu,Sun Shan,Liu Chuang,Li Zihou,Ren Wenzhi,Wu Aiguo,Huang Pintong
As nanomedicine-based clinical strategies have continued to develop, the possibility of combining chemotherapy and singlet oxygen-dependent photodynamic therapy (PDT) to treat pancreatic cancer (PaC) has emerged as a viable therapeutic modality. The efficacy of such an approach, however, is likely to be constrained by the mechanisms of drug release and tumor oxygen levels. In the present study, we developed an Fe(III)-complexed porous coordination network (PCN) which we then used to encapsulate PTX (PCN-Fe(III)-PTX) nanoparticles (NPs) in order to treat PaC via a combination of chemotherapy and PDT. The resultant NPs were able to release drug in response to both laser irradiation and pH changes to promote drug accumulation within tumors. Furthermore, through a Fe(III)-based Fenton-like reaction these NPs were able to convert H 2 O 2 in the tumor site to O 2 , thereby regulating local hypoxic conditions and enhancing the efficacy of PDT approaches. Also these NPs were suitable for use as a T 1 -MRI weighted contrast agent, making them viable for monitoring therapeutic efficacy upon treatment. Our results in both cell line and animal models of PaC suggest that these NPs represent an ideal agent for mediating effective MRI-guided chemotherapy-PDT, giving them great promise for the clinical treatment of PaC.
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ACS Applied Materials & Interfaces
·
2019
·
IF 8.456
Jingmin Wang,Xiaolong Hu,Haizhen Ding,Xin Huang,Mingsheng Xu,Zhenzhen Li,Dong Wang,Xu Yan,Yang Lu,Yunjun Xu,Yan Chen,Paulo Cesar Morais,Yupeng Tian,Ren-Quan Zhang,Hong Bi
Commercial gadolinium-based materials have been widely used as contrast agents for magnetic resonance imaging (MRI), but the high toxicity of leaking free Gd3+ ions still raises biosafety concerns. Here, we develop a novel, safe, and efficient MRI contrast agent based on a stable Fe(III) complex of fluorine and nitrogen co-doped carbon dots (F,N-CDs) that was prepared from glucose and levofloxacin by a simple microwave-assisted thermal decomposition method. The obtained Fe3+@F,N-CD complex exhibits higher longitudinal relaxivity (r1 = 5.79 mM–1·s–1) than that of the control samples of the Fe3+@CD complex (r1 = 4.23 mM–1 s–1) and free Fe3+ (r1 = 1.59 mM–1 s–1) in aqueous solution, as assessed by a 1.5 T NMR analyzer. More importantly, the Fe3+@F,N-CD complex is very stable with a large coordination constant of 1.06 × 107 in aqueous medium. While incubated with HeLa cells, the Fe3+@F,N-CD complex shows clear MR images, demonstrating that it has potential to be an excellent MRI contrast agent. Furthermore, in vivo MRI experiments indicate that the Fe3+@F,N-CD complex provides high-resolution MRI pictures of 4T1 tumor bearing BALB/c mice 15 min after injection and can be completely excreted 2 h after administration. No cytotoxicity was observed with F,N-CDs and Fe concentration up to 0.2 mg/mL and 0.3 mM in 3-(4,5-dimethylthiazol-2-yl)-2,5-diphenyltetrazolium bromide cell proliferation assay, respectively. The possible mechanism of the enhanced MRI effect of the Fe3+@F,N-CD complex is therefore proposed. The extremely low toxicity, high r1 relaxivity, strong photoluminescence, and low synthetic cost enable the Fe3+@F,N-CD complex to be a safe and promising T1-weighted MRI contrast agent for clinical applications.
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Chemical Engineering and Processing-Process Intensification
·
2018
·
IF 2.826
Ding Chen,Peng-fei Feng,Fu-hua Wei
Fe-based metal-organic frameworks(Fe(III)-MOFs)were synthesized by Fe 2 (SO 4 ) 3 and trimesic acid using microwave-assisted ball milling method. The structure of the Fe(III)-MOFs was characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM) and Fourier transform infrared spectrometry (FTIR). The thermostability of the MOFs was analyzed by thermogravimetric analysis (TGA). Fe(III)-MOFs were added in aqueous solutions to remove organic dyes. The removal efficiencies of Orange II, CR and MB reached 95.9%, 98.7%, 95.7% respectively at 10℃ and reached 97.7%, 99.7%, 97.5% respectively at 35℃ in 300 min.
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危险品化学品经营许可证（带存储）