Scientific Reports
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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).
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Journal of Materials Chemistry C
·
2015
·Vol. 3
·期 39
·10232-10241
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IF 4.696
Hualiang Lv,Guangbin Ji,Wei Liu,Haiqian Zhang,Youwei Du
Hierarchical hollow carbon@Fe@Fe3O4 nanospheres were synthesized by a simple template method and another pyrolysis process. Interestingly, the thickness of hollow carbon spheres is tunable by a simple hydrothermal approach. The as-prepared carbon@Fe@Fe3O4 shows excellent microwave absorption properties. In detail, the maximum effective frequency is up to 5.2 GHz with an optimal reflection loss value of −40 dB while the coating thickness is just 1.5 mm. Meanwhile, such absorption properties can be maintained via controlling the thickness of the hollow carbon. For instance, in another coating layer of 2 mm, the effective frequency is still more than 5 GHz as the carbon thickness declines to 12 nm. As novel electromagnetic absorbers, the composites also present the lower density feature due to the hollow carbon sphere frame. The excellent electromagnetic absorption mechanism may be attributed to the obvious interface polarization, and strong magnetic loss ability resulting from the Fe and Fe3O4 shell. Besides, owing to the dielectric feature of carbon, the hollow carbon core is beneficial for the attenuation ability.
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
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2013
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IF 5.257
Zhihui Ai,Zhiting Gao,Lizhi Zhang,Weiwei He,Jun Jie Yin
In this study, core–shell Fe@Fe2O3 nanowires with different iron oxide shell thickness were synthesized through tuning water-aging time after the reduction of ferric ions with sodium borohydride without any stirring. We found that these Fe@Fe2O3 nanowires exhibited interesting core–shell structure dependent reactivity on the aerobic degradation of 4-chlorophenol. Characterization results revealed that the core–shell structure dependent aerobic oxidative reactivity of Fe@Fe2O3 nanowires was arisen from the combined effects of incrassated iron oxide shell and more surface bound ferrous ions on amorphous iron oxide shell formed during the water-aging process. The incrassated iron oxide shell would gradually block the outward electron transfer from iron core for the subsequent two-electron molecular oxygen activation, but more surface bound ferrous ions on iron oxide shell with prolonging aging time could favor the single-electron molecular oxygen activation, which was confirmed by electron spin resonance spectroscopy with spin trap technique. The mineralization of 4-chlorophenol was monitored by total organic carbon measurement and the oxidative degradation intermediates were analyzed by gas chromatography–mass spectrometry. This study provides new physical insight on the molecular oxygen activation mechanism of nanoscale zerovalent iron and its application on aerobic pollutant removal.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2014
·
IF 6.007
Qi Huang,Menghua Cao,Zhihui Ai,Lizhi Zhang
In this study, an environmentally benign polyaminocarboxylic ligand diethylenetriamine pentacetate (DTPA) was first used to promote the aerobic 4-chlorophenol (4-CP) degradation with Fe@Fe 2 O 3 core–shell nanowires, and then compared with the most used counterpart ethylenediamine tetraacetate (EDTA) of poor biodegradability. Although the 4-CP removal rate in the Fe@Fe 2 O 3 /DTPA/Air system was slower owing to the preferential degradation of DTPA, the total organic carbon removal rate in the Fe@Fe 2 O 3 /DTPA/4-CP/Air system was much faster than that in the Fe@Fe 2 O 3 /EDTA/4-CP/Air system. We interestingly found that hydroxyl radicals could more easily react with DTPA to produce DTPA radicals than with EDTA to produce EDTA radicals. Ligands (DTPA or EDTA) could significantly accelerate the hydroxyl radicals production with Fe@Fe 2 O 3 , while more hydroxyl radicals were generated in the Fe@Fe 2 O 3 /DTPA/Air system. We also employed gas chromatography-mass spectrometry and ion chromatography to detect organic intermediates and chloride ions to probe the 4-chlorophenol degradation pathways, and found its degradation pathways were dependent on the reactive oxygen species generated in the different systems. This study can clarify the roles of polyaminocarboxylic ligands on the molecular oxygen activation with nanoscale zero-valent iron, and also provide a green chlorophenols removal method.
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CHEMICAL ENGINEERING JOURNAL
·
2015
·
IF 4.321
Xiaori Fu,Xiaogang Gu,Shuguang Lu,Minhui Xu,Zhouwei Miao,Xiang Zhang,Yacong Zhang,Yunfei Xue,Zhaofu Qiu,Qian Sui
In this study, the application of sodium percarbonate (SPC) catalyzed by various chelated-Fe(II) to stimulate the degradation of benzene in groundwater remediation was investigated. Effective oxidation of benzene was achieved in CIT/SPC/Fe(II) and OA/SPC/Fe(II) systems. The reaction mechanism for benzene degradation in CIT/SPC/Fe(II) and OA/SPC/Fe(II) systems was elucidated by free radical probe compound tests, free radical scavenger tests and electron paramagnetic resonance (EPR) analysis. And hydroxyl radical (HO ) and superoxide anion radical ( O 2 - ) were confirmed as the predominant species responsible for benzene degradation. Besides, the effects of various factors, such as the solution characteristics including the presence of anions (Cl − , HCO 3 − , SO 4 2− and NO 3 − ), natural organic materials (NOM), and the initial solution pH on benzene degradation were also evaluated. The influences caused by SO 4 2− , NO 3 − , Cl − and NOM were negligible, but HCO 3 − anion had a slightly inhibitive effect in low concentration (1 mM) and an apparently inhibitive effect in high concentration (10–100 mM). However, the additions of CIT and OA eliminated the adverse influence of HCO 3 − and ensured a high benzene degradation efficiency at wider pH range. Finally, results obtained in actual groundwater test strongly demonstrated that Fe(II)-CIT and Fe(II)-OA catalyzed SPC systems are applicable for the remediation of benzene-contaminated groundwater in practice.
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Analytical Methods
·
2015
·Vol. 8
·期 6
·1239-1248
·
IF 1.821
Shaolin Li,Yangyang Ding,Wei Wang,Hong Lei
Zero valent iron (ZVI) is increasingly used in large quantities for water treatment. In large-scale application of ZVI, a common question that engineers encounter is ZVI selection or its quality assurance and quality control (QA/QC). A facile method for assessing ZVI quality is proposed and studied in this work. The method is based on the Fe(III)–Fe(0) reaction that has a fast reaction rate, a known and simple stoichiometry, and an easy-to-assay product. The method is conducted by mixing the sample (e.g., testing ZVI) with concentrated Fe(III) solution (up to 3.0 g L−1) for 3–4 hours. The metallic iron (Fe(0)) content of the sample is obtained by assaying the final increase of the total dissolved iron, and its reactivity is quantified using the observed dissolution rate constants. The method is experimentally validated using 23 iron-based materials. Studies with reference iron powder and iron oxide demonstrate that the Fe(III) solution has satisfactory specificity in selecting Fe(0). Replicate experiments and t-test evaluation show the complete dissolution of the Fe(0) content in micron-scale ZVI and the high reproducibility of the method for measuring Fe(0). The accuracy and reliability of the method are studied using 15 commercial ZVIs of known Fe(0) purity, in a series of experiments using Fe(III), Cu(II) or trichloroethylene. The experiments show that the results from the proposed method are accurate and reliable, and that the method is a strong tool more effective than conventional techniques such as X-ray diffraction and BET-N2 adsorption. This work provides an easy and facile way for the quantitative assessment of the quality of metallic iron used for environmental clean-up, especially for the quick survey of a large number of iron samples on site. The method may also serve as a QA/QC procedure for ZVI in industrial-scale production.
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CHEMICAL ENGINEERING JOURNAL
·
2015
·
IF 4.321
Donghui Han,Jinquan Wan,Yongwen Ma,Yan Wang,Ying Li,Dongya Li,Zeyu Guan
Persulfate (PS) oxidation of aniline activated by several chelating agents (CAs) mediated ferrous iron (Fe(II)) was investigated. The effects of CAs structure, CA/Fe(II) ratios and pH on PS activation were studied in batch experiments ran for 120 min. Results showed that the accessible Fe(II) in the CA–Fe(II) complex was responsible for PS activation and appropriate Fe(II) accessibility was favored for more efficient utilization of Fe(II), which could improve the PS activation. Due to the steric hindrance, the number of chelating functional groups and the molecule size of CAs determined the Fe(II) accessibility. In addition, the Fe(II) accessibility was affected by the CA/Fe(II) ratio. When the ratio was 5/1, the Fe(II) accessibility followed the sequence: citric acid > oxalic acid > tartaric acid > (S,S)-ethylenediamine-N,N′-disuccinic acid (EDDS), but when the ratio was lower than 3/1, the accessibility followed the sequence: oxalic acid > tartaric acid > citric acid > EDDS. In tartaric acid processes, as high as 91.7% PS decomposition was obtained at initial pH 9. Although the acidification of solution might contribute to the high PS decomposition, Fe(II) buffering and Fe(II) recovery possibly played more important roles. Citric acid and tartaric acid were more effective in promoting PS activation and larger PS decomposition was observed in these processes under various initial pH. However, the intense competition for radicals by tartaric acid decreased the PS efficiency for aniline removal. The results of Electron Spin Resonance (ESR) and radicals quenching experiments indicated that both SO 4 − and OH contributed to the overall oxidation performance, but OH was the dominant oxidative species.
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ELECTROCHIMICA ACTA
·
2017
·
IF 4.798
Jia Liu,Jinshuo Qiao,Hong Yuan,Jie Feng,Chao Sui,Zhenhua Wang,Wang Sun,Kening Sun
Ni modified Ce 0.6 Mn 0.3 Fe 0.1 O 2 (Ni-CMF) material is evaluated as an anode material for hybrid direct carbon fuel cell (HDCFC). The Temperature Programmed Reaction (TPR) and GC test results show that the Ni additive significantly promotes the oxidation of carbon and consequently accelerates the formation rate of CO. Moreover, the Ni-CMF material is found to show a high electrical conductivity compared to pure CMF in HDCFC operating conditions. Taking advantage of the excellent catalytic activity and high conductivity, the electrolyte-supported HDCFC with Ni-CMF anode shows a high maximum power density of 580.7 mW cm −2 at 800 °C, when activated carbon is used as the fuel. Furthermore, the cell displays good stability under galvanostatic operation at current density of 50 mA cm −2 at 750 °C. These results indicate that the designed Ni-CMF composite material has the potential to be developed as an alternative anode for HDCFCs.
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Scientific Reports
·
2017
·Vol. 7
·期 1
·1-11
·
IF 4.259
Laipan Minwang,Fu Haoyang,Zhu Runliang,Sun Luyi,Zhu Jianxi,He Hongping
Recycling solid waste as functional materials is important for both environmental remediation and resource recycling. This study attempts to recycle spent Cu/Fe layered double hydroxide (Cu/Fe-LDH) which is generated from the adsorption of dyes by converting to Cr(VI) reductant and porous carbon material. Results showed that the obtained reductant was mainly composed of Fe 0 and Cu 0 , and exhibited good reductive activity toward Cr(VI). The species of Fe 0 , Fe 2+ , Cu 0 , and Cu + all favored the reduction of Cr(VI) according to X-ray photoelectron spectroscopy analysis. During Cr(VI) removal, solution pH could increase to neutral which caused the metal ions to precipitate near completion. On the other hand, the spent Cu/Fe-LDH could be employed to produce porous carbon materials, and the generated waste metals solution herein could be reused for LDH synthesis. Specific surface areas of the obtained carbon materials varied from 141.3–744.2 m 2 /g with changes in adsorbed amount of dyes on the LDH. This study illustrates that all the components of wastes can be useful resources, offering a simple recycling approach for similar organic-inorganic solid wastes. This work also enlightens us that designing a proper initial product is crucial to make waste recycling simpler.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2017
·
IF 2.843
Mengqian Yuan,Fan Tian,Guangfang Li,Huiping Zhao,Yunling Liu,Rong Chen
In this work, hierarchical nanostructures Fe(III)-modified BiOBr were successfully prepared via a facile one-step route at room temperature. Compared with pure BiOBr, Fe(III)-modified BiOBr samples possess enhanced photocatalytic abilities for benzyl alcohol oxidation and organic dye degradation in the presence of H2O2 upon light illumination. The improved photocatalytic oxidation and degradation ability of Fe(III)-modified BiOBr is ascribed to the enhanced photogenerated carriers separation efficiency and promoted production of ·OH due to the generation of Fe2+ ions via interfacial charge transfer from Fe3+ ions. This work provides a facial approach to improve photocatalytic efficiency for organic synthesis and environmental remediation.
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IONICS
·
2025
·
IF 2.6
Jiang Zhuwu,Tu Zhehan,Xu Dongdong,Chen Jinfeng,Yang Jiahan,Zhang Fengying,Lin Weixin,Bai Xue,Zhang Hongyu
In the process of sterilization and disinfection, chemical reagents will react with natural organic matter and inorganic matter in water, and inevitably generate disinfection byproducts. These harmful substances are carcinogenic, teratogenic and mutagenic, and their content is low and difficult to detect. Therefore, in this study, we prepare Fe/CoFe-LDH electrodes by in-situ co-precipitation method, and their special structures and morphologies are used to achieve efficient removal of disinfection byproducts. On this basis, the prediction model of trichloroacetamide removal rate is constructed by using the backpropagation neural network, and the prediction model is used to predict the trichloroacetamide removal rate under different experimental parameters and the experiment is verified. The optimal process conditions are obtained, and the maximum trichloroacetamide removal rate is up to 81.62%. The feasibility of the data analysis and processing method based on machine learning in the prediction of disinfection by-products in drinking water is effectively proved.
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JOURNAL OF MATERIALS SCIENCE-MATERIALS IN ELECTRONICS
·
2024
·Vol. 35
·期 26
·1-11
·
IF 2.8
Li Xiao-Bing,Ma Xiao-Ye,Zhang Xue-Feng,Jia Guo-Liang,Zhao Zhao-Ye,Wang Jun-Chuan,Wang Hui,Wu Xiang-Feng
In this work, PCN-224(Fe) porphyrin-based metal–organic frameworks and a Poly(ionic liquids) (PILs) were used to prepare PCN-224(Fe)@PIL(Cl − ) composite films by UV polymerisation. The structure, morphology, chemical composition, and electrochemical properties of the as-prepared composite film were investigated. PCN-224(Fe) was coated with a kind of P(1-vinylpyridinium chloride as monomer) on the outside to improve the electron transfer efficiency, while an electrochemical system was employed to catalysis the persulfate (PS) decomposition for the efficient degradation of tetracycline (TC). Because of the cathodic reduction reaction, the continuous redox cycle between Fe 3+ /Fe 2+ was facilitated, which enhanced the degradation activity of persulfate on tetracycline. The PCN-224(Fe)@PIL(Cl − ) composite demonstrated a superior electrocatalytic degradation efficiency of 95.8% in just 40 min for the TC model pollutant, surpassing the 63.3% efficiency of pure PCN-224(Fe) within 60 min. This work shows a successful example of using PILs to enhance catalytic degradation activity and points out a direction of preparation of catalysts for activating persulfate (PS).
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