SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Yu-qiong Gao,Yan-yan Rao,Han Ning,Ju-xiang Chen,Qian Zeng,Fu-xiang Tian,Nai-yun Gao
The degradation of diclofenac (DCF), a commonly used nonsteroidal anti-inflammatory drug, by Fe 2+ /chlorine and Fe 2+ /PMS processes was comparatively investigated. The influencing factors of pH, Fe 2+ and oxidant dosage on DCF degradation efficiency were evaluated and optimized. Typically, with an initial solution pH of 5, an Fe 2+ dosage of 70 μM, and a chlorine or PMS dosage of 70 μM, the degradation efficiency of DCF using the Fe 2+ /chlorine and Fe 2+ /PMS processes reached 94.2% and 79.7%, respectively, within 10 min. Quenching tests indicated the coexistence of •OH and RCS in the Fe 2+ /chlorine system, and both SO 4 ●– and •OH were identified in the Fe 2+ /PMS system. In addition, Fe(IV) was also identified to participate in DCF degradation in two systems based on the oxidation of PMSO to PMSO 2 . The degradation products and pathways of DCF were elucidated by LC/TOF/MS analysis and DFT calculations. It was assumed that the degradation pathway of DCF involves hydroxylation, dechlorination, decarboxylation, cleavage of the C-N bond, and chlorine substitution. In addition, trichloromethane (TCM), dichloroacetaldehyde (DCAL), dichloroacetonitrile (DCAN) and trichloronitromethane (TCNM) were also detected in the Fe 2+ /chlorine process, and these chlorinated DBPs initially increased and then decreased with prolonged reaction time, indicating that Fe 2+ /chlorine is capable of controlling DBPs formation. Finally, the acute and chronic toxicity of DCF and its degradation products were evaluated by the ECOSAR program.
研究领域:
环境科学
·
化学工程
·
毒理学
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高影响因子
WATER RESEARCH
·
2022
·
IF 13.4
Siqi Liu,Andrey M. Kuznetsov,Weiqing Han,Alexei N. Masliy,Gregory V. Korshin
Methylated arsenic species are ubiquitous in the environment and resistant to removal by conventional treatment technologies. This study addressed this challenge based on the examination of the removal of dimethylarsinic acid (DMA) in a system that combines zerovalent iron (ZVI) and powdered activated carbon (PAC). The removal of DMA in the ZVI/PAC system was compared to that by coagulation, adsorption, electrochemical and Fenton oxidations, and other conventional methods. While only the electrochemical oxidation using a PbO 2 /Sb-SnO 2 /Ti anode allowed removing up to 60% DMA at several hours-long treatment times, the removal of DMA in the ZVI/PAC system containing 10 g/L ZVI and 2.5 g/L PAC with an initial pH of 2.0 was 95% for a 30 min reaction time. Specific roles of PAC, ZVI and its oxidation products in DMA removal were examined based on the spectroscopic data and quantum chemical modeling for the DMA/Fe(II) and DMA/Fe(III) systems. These methods demonstrated the formation of moderately strong DMA/Fe(II) and DMA/Fe(III) complexation. These results and relevant kinetic data were interpreted to indicate that the removal of DMA is governed by the rapid generation of Fe 2+ ions released as a result of accelerated ZVI corrosion in the galvanic ZVI/PAC microcells and ensuing formation of DMA/ Fe 2+ complexes that are readily adsorbed by PAC.
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高影响因子
APPLIED SURFACE SCIENCE
·
2023
·
IF 6.7
Yuxiang Mao,Jun Cheng,Hao Guo,Lei Qian,Jiacan Tu,Weijuan Yang
To enhance catalytic acid-base sites in ZIFs and efficiently promote conversion of microalgal lipids, a bifunctional catalyst with single-atom Fe-N 4 sites and Fe nanoparticles (NPs) was synthesized by pyrolyzing Fe-doped ZIF-8. Compared with ZIF precursors, Fe nanoparticles and coordinated Fe ions in Fe-N 4 sites enhanced Lewis acidity, while increased uncoordinated N atoms enhanced Lewis basicity. Therefore, the acidity of Fe-NC increased from 0.473 to 1.845 mmol/g, while basicity increased from 0.172 to 0.439 mmol/g. DFT calculations showed that the adsorption energies of acetic acid on the Fe–N 4 and Fe NP were −0.536 eV and −0.397 eV, respectively, exceeding that (-0.190 eV) on the Zn–N 4 site. The energy barriers for rate-determining steps over the Fe-N 4 and Fe NP were + 0.32 eV and + 0.21 eV, respectively, which were lower than that (+1.01 eV) over the Zn-N 4 site. The maximum biodiesel yield reached 98.3% over Fe-NC catalyst, higher than that (84.5%) over ZIF-8 catalyst.
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高影响因子
NEW JOURNAL OF CHEMISTRY
·
2024
·Vol. 48
·期 12
·5223-5231
·
IF 2.7
Tingli Ren,Yuanfeng Liu,Xiaoqiu Lin,Congju Li
The fairly low power density, mainly resulting from poor electroactive bacterial (EAB) adhesion and the sluggish extracellular electron transfer (EET) at the anode interface, constrains the practical implementation of microbial fuel cells (MFCs). Therefore, the properties of the anode material are considered to be a crucial factor for the long-term operational performance of MFCs. In order to enhance the power production performance of MFCs, an aerogel composed of Fe, N, and S co-doped carbon nanofibers (CNFs) and reduced graphene oxide (rGO) was employed as a high-performance anode material by electrospinning, high-temperature pyrolysis and freeze-drying. The doping of Fe, N and S elements induced the formation of abundant reactive sites on the CNFs, which enhanced the electrochemical performance of the anode and the EET process. The huge electroactive area of the samples facilitated the formation of dense biofilms. Therefore, an MFC with the FeS/Fe3C@NCNFs/rGO-modified anode achieved a maximum power density of 2792.56 mW m−2 and the highest output voltage of 0.658 V, both of which were significantly higher than those of the carbon cloth anode (773.97 mW m−2 and 0.443 V). Considering the great improvement in power production, it has considerable potential as a low-cost but high-performance anode material for MFCs.
研究领域:
材料科学
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环境工程
·
电化学
·
生物技术
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DOI
高影响因子
RSC Advances
·
2015
·Vol. 5
·期 115
·94694-94701
·
IF 3.84
Xue-ming Lin,Yong-wen Ma,Yan Wang,Jin-quan Wan,Ze-yu Guan
Lithium iron phosphate (LiFePO4) was prepared and applied in the heterogeneous activation of persulfate (PS) for Orange G (OG) degradation in water. Scanning electron microscopy, X-ray diffraction, Raman spectroscopy and X-ray photoelectron spectroscopy (XPS) were used to characterize the properties of the material before and after activation. The effects of several parameters on its catalytic activity were also investigated. It was found that the catalyst presented ultrafast activity for OG and other organic dye degradations. The results from XPS further suggested that the highly catalytic efficiency possibly involved the activation of PS to sulfate radicals as main radical meditated by the redox pair of Fe(II)/Fe(III) of LiFePO4/FePO4.
研究领域:
环境科学
·
材料科学
·
化学工程
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DOI
高影响因子
JOURNAL OF MEMBRANE SCIENCE
·
2025
·
IF 9
Zheng Wang,Keizo Nakagawa,Kecheng Guan,Aiwen Zhang,Yasunao Okamoto,Atsushi Matsuoka,Eiji Kamio,Tomohisa Yoshioka,Hideto Matsuyama
s The stability of solvent-resistant nanofiltration (SRNF) membranes, such as integrally skinned asymmetric (ISA) and thin-film composite (TFC) membranes, in polar aprotic solvents must be improved if they are to meet increasingly complex industrial demands. The stability of the former membranes can be improved by forming crosslinked rigid chains, such as polybenzimidazoles and polyimides, but this requires time-consuming treatment processes. Conversely, the latter membranes are easy to fabricate but lack efficient active sites for crosslinking and structural rigidity. Herein, we present a fabrication strategy combining the characteristics of both types of membranes. We first utilize amino-functional porphyrins as polyaromatic units to form rigid polyamide networks by vacuum-assisted interfacial polymerization, simultaneously providing active sites for further crosslinking, which is accomplished by immersion in FeCl 2 /dimethyl sulfoxide (DMSO) solution to directly establish Fe-O-Fe bridges between porphyrin centers to form a stable network. The Fe-O-Fe-bridged porphyrin networks are solvent-stable in DMSO. Furthermore, they achieve outstanding molecular separation (96.2% rejection of methyl orange, 327 Da) and limited molecular-weight-cutoff change (from 360 to 420 Da) during alternating MeOH and DMSO filtration, along with long-term recovery efficiency (> 96.7% over seven days). Thus, our study provides a promising strategy for the facile development and fabrication of efficient, robust SRNF membranes.
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JOURNAL OF ENVIRONMENTAL ENGINEERING
·
2024
·Vol. 150
·期 6
·04024020
·
IF 1.6
Dawei Wang,Tingyue Chen,Yilan Jiang,Xinyang Cai,Yingying Li,Yuanyuan Chen,Guang Yang,Feng Pan
Promoting the Fe(II)/Fe(III) cycle efficiency is of wide interest for the broader applications of the Fenton process in water treatment sector. In this study, the alternating magnetic field (AMF) was employed to accelerate the reduction from Fe(III) to Fe(II). To achieve this purpose, a composite of nano-zero valence iron and NiFe2O4 was fabricated (denoted as Fe@NiFe2O4). Under the optimal reaction conditions, bisphenol A (BPA) was removed completely within 15 min by the Fe@NiFe2O4/H2O2 system in the presence of AMF, while only ∼60% was removed in the absence of AMF. The faster removal rate in the presence of AMF was ascribed to the elevated temperature caused by the inductive heating of Fe@NiFe2O4 (∼41°C according to the simulation). The simulator of the Fenton process was considered to be the leaked Fe(II) from the Fe part of the composite, as an equal concentration of Fe(II) (∼5.7 mg/L) resulted into a similar removal kinetic. However, the system with Fe@NiFe2O4 as the catalyst consumed less H2O2 in this process, indicating its different activation pathway from the conventional Fenton process. Electrochemical analysis confirmed that the AMF can generate the internal electric field within the composite particle. This field may facilitate the reduction from Fe(III) to Fe(II), which further benefitted the Fenton reactions.
研究领域:
环境科学
·
材料科学
·
化学工程
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DOI
高影响因子
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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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.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Jinbin Lin,Yuye Hu,Junyang Xiao,Yixin Huang,Mengyun Wang,Haoyu Yang,Jing Zou,Baoling Yuan,Jun Ma
Fe(II)/peracetic acid (Fe(II)/PAA) process exhibits a great potential in abatement of micropollutants because of the fast reaction between Fe(II) and PAA. Similar to Fenton system, the slow reduction from Fe(III) to Fe(II) leads to the high dosage of Fe(II) in Fe(II)/PAA process. This study introduced 2,2′-azino-bis(3-ethylbenz- -othiazoline-6-sulfonate) (ABTS) as electron shuttle to improve the oxidation capacity of Fe(II)/PAA process by accelerating the redox cycle of Fe(III)/Fe(II). ABTS/Fe(II)/PAA process possessed high elimination efficiency of diclofenac in acidic conditions. Alcohols quenching experiments confirmed that ABTS •+ was the primary reactive species responsible for diclofenac elimination, although Fe IV O 2+ and carbon-centered radicals (R-O • ) also existed in ABTS/Fe(II)/PAA process. ABTS •+ was generated via various pathways, including the reactions of ABTS with Fe(III), Fe IV O 2+ and R-O • . ABTS was not an ideal electron shuttle because R-O • could decompose partial ABTS •+ to sulfoxides and sulfones. Two possible degradation pathways of diclofenac were proposed based on the detected transformation products. ABTS/Fe(II)/PAA process was highly-efficient for diclofenac elimination in underground water and reservoir water, while high concentration of humic acid had inhibition effect on diclofenac degradation. The present study provides a promising way to alleviate the intrinsic drawbacks of Fe(II)/PAA process and might advance its potential application in water treatment.
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高影响因子
ENVIRONMENTAL RESEARCH
·
2025
·
IF 7.7
Dawei Gao,Haixiang Wang,Qiaoli Lu,Chao Ye,Jingsheng Cai,Lili Wang
Antibiotics, widely used to treat bacterial infections and as agricultural feed additives, pose significant environmental threats due to their persistence, particularly sulfamethoxazole (SMX), which is frequently detected in various ecosystems. Traditional wastewater treatment methods are often ineffective in their removal. This study presents a cost-effective three-dimensional CCF@MoS 2 @GA-Fe (CMGF) catalyst, with cotton fabric as a support to enhance peroxymonosulfate (PMS) activation in advanced oxidation processes (AOPs). Findings indicates that Mo(IV) active sites in CMGF significantly enhanced electron transfer and redox cycling of Fe(II)/Fe(III), ensuring sustained PMS activation and achieving approximately 3.8 times higher degradation efficiency compared to non-catalytic processes. After five cycles, CMGF retains its high catalytic activity. Key active species during PMS activation include singlet oxygen ( 1 O 2 ), hydroxyl radicals (•OH), and sulfate radicals (SO 4 − •). This research elucidates the catalytic mechanisms and degradation pathways of the CMGF/PMS system, highlighting its potential for removing organic pollutants from water.
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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.
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高影响因子
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