JOURNAL OF HAZARDOUS MATERIALS
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2022
·
IF 14.224
Ying Cai,Jinhong Fan,Zhigang Liu
This study constructed a FeS-based Fenton-like process to explore the degradation of TTC in the presence of copper ions . The acidic condition of pH 3 was more favorable to the H 2 O 2 decomposition and TTC degradation , and it was slightly enhanced by Cu(II). The production of •OH from H 2 O 2 was revealed through radical scavenging and benzoic acid probe experiments, and the ratio of H 2 O 2 decomposition to •OH production was about 1–1.5, which is comparatively consistent with the theoretical ratio. FeS-based Fenton process was proved to be a homogenous system, the slow release of Fe(II) source and the autocatalytic cycle of Fe(III) to Fe(II) resulting from the reductive species of TTC and dissolved S(-II) improved the production of •OH and the degradation of TTC, which was proved by comparing TTC degradation, TOC removal, H 2 O 2 decomposition and Fe(II) concentration with different iron sources (FeS, Fe(II) and Fe(III)) and external addition of dissolved S(-II). The possible degradation pathways of TTC were subsequently inferred according to the detected products by LC-MS. Understanding these autocatalytic processes is essential to reveal the transformation of redox-active substances in environments and may have potential significance in applying FeS-based Fenton-like process for the treatment of wastewater containing reductive organic matters.
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CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Sitao Wang,Zhijie Liu,Bolun Pang,Yuting Gao,Santu Luo,Qiaosong Li,Hailan Chen,Michael G Kong
Antibiotics are widely used to treat or prevent infectious diseases in human and veterinary medicine. Excessive residues in the aquatic environment lead to increasingly prominent antibiotic pollution; therefore, it is urgent to develop sustainable strategies for rapidly degrading antibiotics. In this study, a highly synergetic effect for norfloxacin (NOR) remediation is achieved by coupling underwater bubble plasma formation with a Fe (III)–S (IV) system due to the efficient utilization of reactive species in chain reactions. The degradation rate using synergetic approach can reach 76.4% within 50 min discharge, and further increases significantly to 94.4% after 5 h post-discharge. The effects of pulsed peak voltage and Fe (III)/S (IV) dosage on NOR removal are characterized. The existence of hydroxyl radicals ( • OH) and sulfate radicals (SO 4 •− ) are proved by electron spin resonance spectrometer (ESR) during degradation. Furthermore, radical scavenger experiments demonstrate that • OH and SO 4 •− play a crucial role in degradation. Underwater bubble plasma provides the oxic and acidic liquid environment for the Fe (III)–S (IV) system to accelerate the self-perpetuating chain reactions. These reactions not only introduce SO 4 •− and generate more • OH during plasma-on, but also induce their regeneration and further prolong the degradation process during plasma-off through plasma-generated effects. Finally, the degradation intermediates of NOR are identified, and a possible degradation pathway is proposed. The possible contribution weight of each approach on the degradation rate is speculated. These new findings offer promising applications for developing a technology with real potential for the treatment of organic compounds in industrial wastewater treatment.
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WATER RESEARCH
·
2023
·
IF 12.8
Wenyu Liu,Li Long,Zhe Yang,Li Wang,Qimao Gan,Shenghua Zhou,Pulak Sarkar,Hao Guo,Chuyang Y. Tang
Nanofiltration technology has been applied in a variety of water treatment scenarios. However, conventional thin-film composite (TFC) membranes fail to remove emerging organic micropollutants (OMPs) efficiently. Here we applied thin-film nanocomposite membrane with an interlayer (TFNi) of Fe (III)-tannic acid to remove various types of OMPs, such as endocrine disrupting chemicals (EDCs), pharmaceutically active compounds (PhACs), and perfluoroalkyl substances (PFASs). Compared to the pristine TFC membrane, TFNi membrane exhibited crumpled morphology and its rejection layer was denser, better cross-linked and possessed smaller average pore size with narrower distribution. Significant enhancement in water-OMPs selectivity of PhACs and PFASs was observed. The mechanism lies in the effects of interlayer in improving the membrane permeance to water and meanwhile reducing the permeance to some OMPs by enhancing size exclusion effects. This work confirms the effectiveness of using TFNi membrane to simultaneously enhance the OMPs rejection and water permeance. The unraveled mechanism might inspire the future development of high-performance nanofiltration membranes targeting OMPs removal.
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CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Xiaomeng Zhang,Yang Zong,Longqian Xu,Yunfeng Mao,Deli Wu
Abiotic humification can be facilitated by iron-containing minerals or oxides, but most studies have focused on well-crystallized and stable iron phases, the catalytic effect of which is generally unremarkable. In the present study, we report an enhanced abiotic integrated polyphenol-Maillard humification reaction catalysed by Mg/Fe-layered double hydroxide (Mg/Fe-LDH) with high surface reactivity. The results demonstrated that Mg/Fe-LDH could effectively promote the humification reaction at a lower dosage compared with Fe 2 O 3 . As an iron-chelating ligand, catechol rapidly induced iron dissolution from Mg/Fe-LDH through the formation of an Fe(III)-catechol complex, which strengthened the catalytic effect of Fe(III). The photochemical behaviour of Fe(III)-catechol complex and its impact on the Fe(III)-catalysed humification process were investigated. Under light irradiation, environmentally persistent free radicals (EPFRs) originated from the Fe(III)-catechol complex were formed and stabilized in the presence of Mg/Fe-LDH particles, which inhibited the oxidation of catechol and the humification process. Hence, the formation of humic substances (HS) catalysed by Mg/Fe-LDH was more efficient under darkness. Iron redox cycling and generation of reactive oxygen species (ROS), HO• and O 2 •- , were also involved. According to transformation products (TPs) analysis, ortho -aminophenol was proposed to be a key product in the humification reaction. Self-coupling of catechol radical and ortho -aminophenol radical, ring cleavage were likely to occur in the Fe(III)-catalysed humification process. Higher relative abundance of CHO products was observed in the presence of Mg/Fe-LDH by Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR MS), suggesting that iron is effective on promoting C–C bonds formation. The above results provide more comprehensive insights into Fe(III)-catalysed humification and a guidance to improve the efficiency of HS formation and carbon sequestration in organic wastes utilization.
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ACS Biomaterials Science & Engineering
·
2019
·
IF 4.511
Sihui Chen,Yixian Wang,Mengxiao Zhong,Dahai Yu,Ce Wang,Xiaofeng Lu
In the past decade, nanomaterials-based artificial enzymes have emerged as a hot spot in the field of catalysis. However, it is a significant challenge to fabricate functional nanomaterials for multiple-enzyme mimetic activity. In this work, we have presented an efficient catalytic platform to mimic peroxidase, oxidase, and catalase-like activity by Fe3C decorated carbon nanofibers (Fe3C/C NFs). First, polyacrylonitrile nanofibers (PAN NFs) are prepared via an electrospinning technique. Next, an Fe(III)-tannic acid (TA) complex is formed on the surface of PAN NFs through a wet chemical reaction. Finally, Fe3C/C NFs are obtained from the carbonization of the PAN/Fe(III)-TA complex nanofibers. The prepared Fe3C/C NFs show an excellent triple-enzyme mimetic property including peroxidase-like, oxidase-like, and catalase-like activity, which is investigated thoroughly by the colorimetric experiment of the 3,3′,5,5′-tetramethyl benzidine oxidation and the degradation of H2O2. Thanks to the superior catalytic performance of Fe3C/C NFs for oxidase mimicking, a facile and colorimetric way to determine glutathione with a high sensitivity and favorable selectivity has been achieved. This work provides an efficient platform for multiple-enzyme mimicking, which may expand their promising applications in biosensing, biomedicine, and environmental technology.
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JOURNAL OF FLUORESCENCE
·
2019
·Vol. 29
·期 3
·769-777
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IF 1.913
Luo Kuan,Jiang Xinyu
Nitrogen-sulfur co-doped carbon quantum dots (N, S-CQDs) with good photoluminescence properties were prepared by hydrothermal method using citric acid (CA) and methionine (Met) as precursors. Co-doping with N and S facilitates the electron transfer rate and coordination interaction between N,S-CQDs and Fe(III) ions which acts as a quencher of fluorescence. Based on a simple redox principle, a highly sensitive and selective method for the detection of ascorbic acid (AA) and H 2 O 2 was successfully developed. The calibration curves obtained are linear for the current versus AA and H 2 O 2 concentration over the range 50–500 μM and 10–140 μM, respectively. And the detection limits for AA and H 2 O 2 are 4.2 μM and 1.9 μM, respectively. The quantitative analysis of AA and H 2 O 2 in various juices and H 2 O 2 disinfectant with Fe 3+ /CQDs or Fe 2+ /CQDs gave the recoveries of 87.8%–117.5% and 99.2%–106.4% with relative standard deviations ( RSD ) of 1.6–5.1% and 1.7–3.1%, respectively, showing satisfactory results for the determination of AA and H 2 O 2 in actual application. The proposed strategy may provide a new pathway to developing inexpensive and sensitive way for the detection of various redox reaction–involved system.
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TALANTA
·
2018
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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.
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Journal of Materials Chemistry A
·
2014
·Vol. 3
·期 5
·2120-2127
·
IF 0
Fangyuan Gai,Tianlei Zhou,Yunling Liu,Qisheng Huo
In this study, a water-soluble Fe3+ ratiometric fluorescent sensor was designed and synthesized by encapsulating a donor–acceptor (D–A) dye 4-formacyl-triphenylamine (FTA) into silica cross-linked micellar nanoparticles (SCMNPs). The quenching of FTA-encapsulated SCMNPs (FTA-SCMNPs) on Fe3+ sensing was confirmed using the fluorescence titration method. FTA-encapsulated functionalized SCMNPs (FTA-NH2-SCMNPs and FTA-SO3H-SCMNPs) were synthesized to demonstrate the surface charge effect of nanoparticles on Fe3+ fluorescence sensing. The sensing ability of Fe3+ followed in this order: FTA-SO3H-SCMNPs > FTA-SCMNPs > FTA-NH2-SCMNPs, which indicates that particles with stronger negative charge have better sensing abilities. Moreover, linear correlation between the quenching intensity and lower concentration of Fe3+ was in accordance with the Stern–Volmer equation in FTA-SCMNPs and FTA-SO3H-SCMNPs. FTA-SO3H-SCMNPs showed good selectivity for Fe3+ detection. Because of the charge effect of functionalized SCMNPs on a dye-doped Fe3+ sensing system, these kinds of nanoparticles offered possibilities to construct sensing ability-enhanced fluorescence-quenching sensors by tuning the surface charge.
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Water
·
2024
·Vol. 16
·期 24
·3658
·
IF 3
Jialin Chen,Yi Xie,Jun Xia,Xiaolin Zhang,Dong Chen
An advanced photochemical reduction system involving the UV/Fe(III)–oxalate system was developed for the reduction of nitrate (NO3−) to harmless N-gaseous species, primarily nitrogen (N2), by carbon dioxide radical (·CO2−) generated in the presence of dissolved oxygen (DO). Electron paramagnetic resonance (EPR) analyses confirmed the presence of both ·CO2−and ·OH radicals. Systematic investigations were conducted on various operational parameters, such as the initial Fe(III) concentration, oxalate concentration, and pH levels, to assess their impacts on the efficiency and products of NO3−reduction. Notably, solution pH played a significant role in influencing the NO3−reduction efficiency and the final products. At pH 2, approximately 75% of NO3−was converted into N2with an 80% selectivity. In the pH range of 3 to 5, a remarkable NO3−removal rate of about 90% was achieved. Furthermore, higher concentrations of Fe(III) (2 mM) and oxalate (10 mM) were found to enhance NO3−removal to 91.95% and 88.71%, respectively. The presence of DO increased the oxidative potential in the reaction system, subsequently enhancing the selectivity conversion of NO3−to N2. In summary, the UV/Fe(III)–oxalate system exhibits significant potential for effective removal of NO3−while achieving high selectivity for the production of N2in water remediation applications.
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MICROCHEMICAL JOURNAL
·
2024
·
IF 4.9
Fang Li,Nuotong Shen,Qingcheng Li,Chen Yang,Limin Zhang,Mingjin Wang
The development of microfluidic flow injection analysis (FIA) system for simultaneous and real-time detection of multiple metal ions is of great importance for environmental monitoring, food safety and industrial field. In this work, a multiplexed microfluidic chip based FIA system was fabricated for simultaneous determination of three metal ions, by using Fe(III), Mn(II) and Cu(II) as models. The multiplexed microfluidic chip based FIA system is composed of three parts, including a multi-channel FIA system for solution manipulation, a group of microfluidic chips for reagents mixing and reaction, and one fiber optic spectrometer for fast and real-time absorbance signal detection. The sample solution and chromogenic reagents were injected into the microfluidic chips to carry out specific colorimetric reactions. Fe(III), Mn(II) and Cu(II) reacts with 5-sulfosalicylic acid, formaldoxime, and bis(cyclohexanone) oxalyldihydrazone, respectively, to generate orange, ember and blue colored solution with peak absorbance at 420 nm, 450 nm, and 600 nm, respectively. The absorbance signal of the generated three channels of solution can be sequentially detected by using only one mini spectrometer. The linear detection range for Fe(III), Mn(II) and Cu(II) is 0.1–20 mg/L, 0.1–12 mg/L and 0.2–12 mg/L, respectively. The limit of detection for Fe(III), Mn(II) and Cu(II) is 0.07, 0.02 and 0.1 mg/L respectively. And the limit of quantification for Fe(III), Mn(II) and Cu(II) is 0.2, 0.07 and 0.3 mg/L, respectively. The recoveries of spiked Fe (III), Mn (II), and Cu (II) in real water samples are between 95.3 % to 106 %. Finally, the developed microfluidic chip based FIA system was successfully applied to simultaneous determination of three metal ions in environmental water samples and zinc smelting solution from zinc hydrometallurgy industry with satisfied results.
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MOLECULES
·
2024
·Vol. 29
·期 17
·4194
·
IF 4.2
Kaiwei Ding,Tingsheng Qiu,Xianhui Qiu,Guanfei Zhao,Qinghao Jiao,Jiangjie Fang,Ruisen Lai,Wenhui Yang
The floatability of fluorite and calcite exhibit similar properties, rendering their flotation separation challenging. Macromolecular polysaccharide reagents containing the polyhydroxyl group have shown broad promising application. The selectivity of polysaccharide is relatively low. In this study, the introduction of Fe3+was employed to enhance the selective adsorption capacity of Pullulan polysaccharide towards fluorite and calcite minerals, thereby achieving effective flotation separation. Furthermore, the mechanism underlying intramolecular interactions was elucidated. The DFT calculation and XPS analysis revealed that the adsorption of Fe3+on the calcite surface was more favorable, leading to the formation of a Ca-O-Fe structure. The MD simulation, XPS analysis, and Zeta potential analysis revealed that the Fe-OH groups on the surface of calcite reacted with the -OH groups in Pullulan and formed bonds, resulting in the formation of a Calcite-Fe-Pullulan structure. This facilitated the attachment of a significant number of Pullulan molecules to the calcite surface. The formation of a hydrophilic layer on the outer surface of calcite by Pullulan, in contrast to the absence of such layer on fluorite’s surface, results in an increased disparity in surface floatability between these two minerals, thereby enhancing the efficiency of flotation separation.
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JOURNAL OF HAZARDOUS MATERIALS
·
2025
·
IF 11.3
Jingye Cui,Huan He,Wanqi Shi,Zhicheng Liao,Danni Cui,Jianxiang Yang,Yixin Liu,Chaochao Lai,Bin Huang,Xuejun Pan
Microbial-derived extracellular polymeric substances (EPS) and iron minerals are ubiquitous in aquatic environments, and they can influence the fate of organic micropollutants such as 17α-ethinylestradiol (EE2). However, the interactions between EPS and iron minerals, and their influence on EE2 photodegradation, are seldom addressed in the literature. This study explored the effects of EPS derived from different aerobic or anaerobic microbials on the reductive dissolution of ferrihydrite (Fhy) and subsequent EE2 photodegradation, with emphasis on the impact of Fe-EPS complexes formation. In the dark, EPS could promote the reductive dissolution of Fhy via ligand-metal charge transfer, accompanied by Fe(III)-EPS complexes formation. Irradiation could further enhance such a dissolution process. Dissolved iron could accelerate the photolysis of protein and humic substances, triggering Maillard-like reactions that form the unsaturated medium- or high-molecular-weight polymers. The aerobic-EPS containing more proteins and humic substances photodegraded EE2 more effectively than anaerobic-EPS, with the triplet excited state playing a crucial role. In contrast, Fhy inhibited EPS-mediated EE2 photodegradation via light-shielding effect or photosensitizers oxidative decomposition. The information obtained in this research would contribute to the understanding of photochemistry involving EPS, iron minerals, and steroid estrogens, providing new insights into their environmental behavior.
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