CHEMICAL ENGINEERING JOURNAL
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2020
·
IF 10.652
Zhuozhi Ouyang,Chen Yang,Junheng He,Qian Yao,Bijie Zhang,Hanming Wang,Yu Jiang,Jini Zhou,Yurong Deng,Yanjun Liu,Jingjing Yang,Guining Lu,Zhi Dang
Sulfamethazine (SMT), taken as model compound, have been exposed to a photocatalytic system driven by ultraviolet light (UV) irradiation with Fe(III) and three carboxylic acids (citric, tartaric and malic acid). The kinetic experiments, quenching experiments, electron paramagnetic resonance (EPR), species model theoretical calculation, density functional theory (DFT) and intermediates analyses, were conducted to analyze the formation of reactive oxygen species (ROS) and underlying mechanism of Fe(III)-carboxylate complexes on photocatalytic degradation of SMT. The results indicated the complexes easily induced the degradation under UV irradiation. Enough hydroxyl radicals ( · OH) were produced and the singlet oxygen ( 1 O 2 ) originated from the self-sensitized oxidation. An interaction among ROS, Fe(III)-carboxylate complexes and SMT was firstly proposed. The active sites and groups were characterized through Frontier electron densities (FEDs), Fourier Transform-Infrared (FTIR) and Two-dimensional correlation FTIR spectroscopy (2D-FTIR-CoS) analyses. The transformation pathway mainly included four reactions: hydroxylation, SO 2 extrusion, Smiles-type rearrangement and S-N bond cleavage. The system also had an application potential for removing SMT from practical water.
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HYDROMETALLURGY
·
2020
·
IF 3.338
Xintao Yi,Guangsheng Huo,Wei Tang
The extraction of Fe(III), Ni(II) and Co(II) from a Ni(II)-Co(II) solution containing Fe(III) was analyzed in a chloride medium using a mixed extractant consisting of 50% ( v /v) tributyl phosphate (TBP), 20% (v/v) 2-octanol and 30% (v/v) kerosene. The extraction of 0.5 mol/L Fe(III) in 4 mol/L hydrochloric acid reached 97%, and the consumption of chloride ions was investigated. Nickel(II) ions were not detectably extracted by TBP, with an inclusion of <1.1%. Compared with Fe(III), TBP extracted only a small amount of Co(II). The iron complexes formed by TBP and 2-octanol were [H 2 FeCl 4 · 2TBP] and [H 2 FeCl 4 · 5(2-octanol)], and the possible compositions of Co-containing extracts were [H 2 CoCl 4 · 2TBP] and [H 2 CoCl 4 ] · n[2-octanol]. An industrial process consisting of two-step extraction was designed to achieve the separation of Co(II) and Fe(III), resulting in a decrease in the Fe/Co mass ratio from 0.46 to <3.5 × 10 −4 in the raffinate.
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POLYMER INTERNATIONAL
·
2021
·Vol. 71
·期 2
·169-174
·
IF 2.99
Yinyan Chen,Yiban Wu,Yifan Zhu,Saiqi Tian
Rhodamine salicylaldehyde was synthesized, and its structure was determined using Fourier transform infrared spectroscopy, 1 H NMR analysis as well as electrospray ionization mass spectrometry. Then a fluorescent polyurethane foam was obtained via incorporation of the prepared rhodamine salicylaldehyde, and the fluorescence sensing behavior for Fe 3+ was systematically investigated. Results showed that the fluorescent polyurethane foam produced higher fluorescence in the presence of Fe 3+ in pure water, due to the coordination for Fe 3+ binding leading to ring-opened amide form. The limit of detection was calculated to be 1.64 × 10 −6 mol L –1 . This fluorescent polyurethane foam can also recognize Fe 3+ with good selectivity. © 2021 Society of Industrial Chemistry.
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Scientific Reports
·
2017
·Vol. 7
·期 1
·1-11
·
IF 4.259
Liu Renlan,Zhu Xiaoying,Chen Baoliang
Graphene oxide (GO) contains not only aromatic carbon lattice but also carboxyl groups which enhanced the aqueous solubility of GO. To study the transformation of GO nanosheets in natural environments, GO aqueous dispersion was mixed with Fe 3+ ions to form photoactive complex. Under visible light irradiation, Fe(III) of the complex would be reduced to Fe(II) which could subsequently reduce highly toxic Cr(VI) to Cr 3+ . The electron of the reduction was contributed by the decarboxylation of carboxyl groups on GO and iron was acting as a catalyst during the photoreduction. On the other hand, the consumption of carboxyl groups may convert GO to rGO which are tend to aggregate since the decreased electrostatic repulsion and the increased π-π attraction. The formed Cr 3+ may be electrostatically adsorbed by the rGO sheets and simultaneously precipitated with the aggregated rGO sheets, resulting the effective removal of chromium and GO nanosheets from the aqueous environment. This study may shed a light on understanding the environmental transformation of GO and guide the treatment of Cr(VI).
研究领域:
环境科学
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材料科学
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2023
·
IF 11.4
Jinzhao Wang,Di Huang,Fengxia Chen,Jianhua Chen,Hongyu Jiang,Yifan Zhu,Chuncheng Chen,Jincai Zhao
Fe(III) and carboxylic acids are common compositions in atmospheric microdroplet systems like clouds, fogs, and aerosols. Although photochemical processes of Fe(III)–carboxylate complexes have been extensively studied in bulk aqueous solution, relevant information on the dynamic microdroplet system, which may be largely different from the bulk phase, is rare. With the help of the custom-made ultrasonic-based dynamic microdroplet photochemical system, this study examines the photochemical process of Fe(III)–citric acid complexes in microdroplets for the first time. We find that when the degradation extent of citric acid is similar between the microdroplet system and the bulk solution, the significantly lower Fe(II) ratio is present in microdroplet samples due to the rapider reoxidation of photogenerated Fe(II). However, by replacing citric acid with benzoic acid, no much difference in the Fe(II) ratio between microdroplets and bulk solution is observed, which indicates distinct reoxidation pathways of Fe(II). Moreover, the presence of •OH scavenger, namely, methanol, greatly accelerates the reoxidation of photogenerated Fe(II) in both citric acid and benzoic acid situations. Further experiments reveal that the high availability of O2 and the citric acid- or methanol-derived carbon-centered radicals are responsible for the rapider reoxidation of Fe(II) in iron–citric acid microdroplets by prolonging the length of HO2•- and H2O2-involved radical reaction chains. The results in this study may provide a new understanding about iron–citric acid photochemistry in atmospheric liquid particles, which can further influence the photoactivity of particles and the formation of secondary organic aerosols.
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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.
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Journal of Materials Chemistry C
·
2022
·Vol. 10
·期 46
·17472-17480
·
IF 8.067
Xiaowei Zhu,Yijiang Li,Tianchen Wei,Yichen Li,Tieling Xing,Matthew D. Shawkey,Guoqiang Chen
Photonic structures constructed from colloidal nanospheres present an attractive prospect for structural coloration in an ecological manner. However, the application of structural color in the field of textile coloration is usually blocked by their uncorrelated scattered light and feeble mechanical properties. Here, a non-iridescent structural color coating with high color saturation and mechanical stability is developed by assembling PS@TA–Fe(III) core–shell nanospheres. The rough surface and low surface charge are favorable for forming amorphous colloid arrays (ACAs) by restricting the crystalline alignment during the assembly process, resulting in non-iridescent structural colors. In addition, the as-prepared structurally colored cotton fabric possesses high color saturation and mechanical stability thanks to the intense light absorption and interface adhesion of the TA–Fe(III) shell. The preparation approach of this structural color coating is facile, low-cost, and environment-friendly, showing promising applications in textile coloration and smart displays.
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INORGANIC CHEMISTRY
·
2019
·
IF 4.85
Wei Wang,Mehran Amiri,Tao Huang,Lev N. Zakharov,Yining Zhang,May Nyman
Isolating Fe(III) clusters from water without stabilizing ligands is significantly challenged by the high acidity of Fe3+-bound water, leading to uncontrolled precipitation of iron oxyhydroxides. Here we demonstrate a freeze-drying solvent-exchange method that enabled the isolation of a metastable Fe(III) sulfate decameric cluster formulated [Fe10O2(SO4)12(OCH3)2]·14CH3OH (Fe10). Without stabilization by solvent-exchange, the aqueous species undergoes rapid conversion to the iron sulfate mineral schwertmannite. Monitoring the hydrolysis process from cluster intermediates to schertmannite by small-angle X-ray scattering, we observe the progression from Fe10 to 37 Å soluble nanoparticles prior to the precipitation process. This condensation behavior of Fe10 is further exploited to develop a simple laboratory synthesis of schwetmannite. In addition, we demonstrate the versatility of the freeze-drying solvent-exchange method by isolating Al(III), Zn(II), and Cd(II) substituted Fe(III) sulfate clusters. The freeze-drying solvent-exchange method provides a unique opportunity to isolate cluster intermediates and models to aid in our understanding of metal-ion hydrolysis processes in environmental, material science, and geological studies.
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SCIENCE OF THE TOTAL ENVIRONMENT
·
2024
·
IF 8.2
Quantao Cui,Yuyin Dong,Weiwei Zou,Ziyu Song,Wei Zhang,Qiting Zuo,Xiaoli Zhao,Fengchang Wu
Sulfite-based advanced oxidation technology has received considerable attention for its application in organic pollutants elimination. However, the potential of natural sediments as effective catalysts for sulfite activation has been overlooked. This study investigates a novel process utilizing suspended sediment/sulfite (SS/S(IV)) for degradation of metronidazole (MNZ). Our results demonstrate that MNZ degradation efficiency can reach to 93.1 % within 90 min with 12.0 g SS and 2.0 mM sulfite. The influencing environmental factors, including initial pH, SS dosage, S(IV) concentration, temperature, and co-existing substances were systematically investigated. Quenching experiments and electron paramagnetic resonance analyses results indicate that SO 3 •− is the primary active substance responsible for MNZ degradation, with involvement of SO 4 •− , SO 5 •− , and • OH. X-ray photoelectron spectroscopy and Mössbauer spectra reveal that Fe (III)-silicates play a crucial role in activating S(IV). Furthermore, analysis of degradation intermediates and pathways of MNZ is conducted using liquid chromatography with mass spectrometry (LC -MS). The toxicity of MNZ and its intermediates were also systematically evaluated by the T.E.ST. program and wheat seeds germination test. This study offers valuable insight into the activation of sulfite by natural sediments and could contribute to the development of SS-based advanced oxidation processes (AOPs) for the in-situ remediation of antibiotics-contaminated water environments.
研究领域:
环境科学
·
水处理
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污染物降解
·
催化
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CHEMICAL ENGINEERING JOURNAL
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2015
·
IF 4.321
Zhouwei Miao,Xiaogang Gu,Shuguang Lu,Mark L. Brusseau,Xiang Zhang,Xiaori Fu,Muhammad Danish,Zhaofu Qiu,Qian Sui
The performance of Fe(III)-based catalyzed sodium percarbonate (SPC) for stimulating the oxidation of tetrachloroethene (PCE) for groundwater remediation applications was investigated. The chelating agents citric acid monohydrate (CIT), oxalic acid (OA), and glutamic acid (Glu) significantly enhanced the degradation of PCE. Conversely, ethylenediaminetetraacetic acid (EDTA) had a negative impact on PCE degradation, which may due to its strong Fe chelation and HO scavenging abilities. However, excessive SPC or chelating agent will retard PCE degradation. In addition, investigations using free radical probe compounds and radical scavengers revealed that PCE was primarily degraded by HO radical oxidation in both the chelated and non-chelated systems, while O 2 − also participated in the non-chelated system and the OA and Glu modified systems. According to the electron paramagnetic resonance (EPR) studies, the presence of HO in the Fe(III)/SPC system was maintained much longer than that in the Fe(II)/SPC system. The results indicated that the addition of CIT, OA or Glu indeed enhanced the generation of HO in the first 10 min and promoted degradation efficiency by increasing the amount of Fe(III) and maintaining the concentration of HO radicals in solution. In conclusion, chelated Fe(III)-based catalyzed SPC oxidation is a promising method for the remediation of PCE-contaminated groundwater.
研究领域:
环境科学
·
化学
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WATER RESEARCH
·
2022
·
IF 13.4
Shuang Meng,Peng Zhou,Yiming Sun,Peng Zhang,Chenying Zhou,Zhaokun Xiong,Heng Zhang,Juan Liang,Bo Lai
Reduction of Fe(III) is the rate-limiting step of iron induced Fenton-like systems, such as the iron/peroxydisulfate system, reducing agents (RAs) were frequently employed as electron donors to directly reduce Fe(III) to further promote the formation of reactive oxygen species (ROS), mainly including hydroxyl radical ( • OH), sulfate radical (SO 4 •− ), and ferryl ion (Fe(IV)). However, the intrinsic distinctions among these ROS cause the substrate specific reactivity towards oxidation of diverse organic contaminants. In this study, various RAs (representative solid amorphous boron (A-Boron) and dissolved hydroxylamine (HA)) were added to enhance the Fe(III)/PDS system for investigating the substrate specific reactivity of ROS. It is demonstrated that RAs remarkably boost the Fe(III)/Fe(II) cycles to produce • OH, SO 4 •− , and Fe(IV) in the RAs/Fe(III)/PDS systems, based on the results of EPR analysis, quenching tests, and chemical probe analysis. Furthermore, the different yields of methyl phenyl sulfone (PMSO 2 ) indicate that the distribution of multiple oxidizing species changed with various factors (i.e., type and dosage of RAs added, solution pH, Fe(III) and PDS dosage). This work provides the possibility for the adjustment of oxidation selectivity of RAs/Fe(III)/PDS systems by regulating contribution of radicals and non-radical for oxidizing organic contaminants due to the substrate specific reactivity of • OH, SO 4 •− , and Fe(IV), moreover, the comparison of homogeneous and heterogeneous RAs provides assistance in the application of RAs for environmental remediation.
研究领域:
环境科学
·
化学
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DYES AND PIGMENTS
·
2019
·
IF 4.018
Yingting Zheng,Hailong Wang,Jianzhuang Jiang
A fluorescent porous tetraphenylethylene-based organic polymer ( PTOP ) was constructed by the reaction of 5,5',5'',5‴-(ethene-1,1,2,2-tetrayltetrakis(benzene-4,1-diyl))tetrakis(pyrimidin-2-amine) and cyanuric chloride in the presence of potassium carbonate. CO 2 sorption experiment at 195 K reveals the permanent porosity of PTOP with a Brunauer-Emmett-Teller surface area of 227 m 2 g −1 . In particular, the existence of rich secondary amines and pyrimidine nitrogen atoms surrounding the 1,3,5-triazine moieties in PTOP provides abundant chelating sites for metal ions, endowing a fast-response and sensitive fluorescence sensing Fe(III) with a low limit of detection of 4.5 μM. In addition, this polymer also shows an excellent sensing performance towards nitrobenzene with good selectivity and a low detection limit of 1.6 nM.
研究领域:
材料科学
·
分析化学
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危险品化学品经营许可证（带存储）