WATER RESEARCH
·
2017
·
IF 6.942
Xing Ding,Shengyao Wang,Wanqiu Shen,Yi Mu,Li Wang,Hao Chen,Lizhi Zhang
In this study, an electrochemical/electro-Fenton oxidation (EC/EF) system was designed to degrade atrazine, by utilizing boron-doped diamond (BDD) and Fe@Fe 2 O 3 core-shell nanowires loaded active carbon fiber (Fe@Fe 2 O 3 /ACF) as the anode and the cathode, respectively. This EC/EF system exhibited much higher degradation rate, decholorination and mineralization efficiency of atrazine than the electrochemical (EC) and electrochemical/traditional electro-Fenton (EC/TEF) oxidation counterpart systems without Fe@Fe 2 O 3 core-shell nanowires. Active species trapping experiment revealed that Fe@Fe 2 O 3 could activate molecular oxygen to produce more OH through Fenton reaction, which favored the atrazine degradation. High performance liquid chromatography , high performance liquid chromatography-mass spectrometry and gas chromatography-mass spectrometry were applied to probe the decomposition and mineralization of atrazine during this novel EC/EF process, which revealed that two intermediates of triazinons (the isomerization of hydroxylated atrazine) were generated during the electrochemical/electro-Fenton oxidation of atrazine in the presence of Fe@Fe 2 O 3 core-shell nanowires. The experimental and theoretical calculation results suggested that atrazine might be degraded via a triazinon ring opening mechanism, while the presence of Fe@Fe 2 O 3 notably accelerated the decholorination process, and produced more hydroxylated products to promote the generation of trazinons and the subsequent ring cleavage as well as the final complete mineralization. This work provides a deep insight into the triazine ring opening mechanism and the design of efficient electrochemical advanced oxidation technologies (EAOTs) for persistent organic pollutant removal .
研究领域:
环境科学
·
化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
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.
研究领域:
环境科学
·
化学
✓ 已验证
产品关联
DOI
高影响因子
WATER RESEARCH
·
2014
·
IF 5.323
Jingu Shi,Zhihui Ai,Lizhi Zhang
In this study we demonstrate Fe@Fe 2 O 3 core–shell nanowires can improve Fenton oxidation efficiency by two times with rhodamine B as a model pollutant at pH > 4. Active species trapping experiments revealed that the rhodamine B oxidation enhancement was attributed to molecular oxygen activation induced by Fe@Fe 2 O 3 core–shell nanowires. The molecular oxygen activation process could generate superoxide radicals to assist iron core for the reduction of ferric ions to accelerate the Fe(III)/Fe(II) cycles, which favored the H 2 O 2 decomposition to produce more hydroxyl radicals for the rhodamine B oxidation. The combination of Fe@Fe 2 O 3 core–shell nanowires and ferrous ions (Fe@Fe 2 O 3 /Fe 2+ ) offered a superior Fenton catalyst to decompose H 2 O 2 for producing OH. We employed benzoic acid as a probe reagent to check the generation of OH and found the OH generation rate of Fe@Fe 2 O 3 /Fe 2+ was 2–4 orders of magnitude larger than those of commonly used iron based Fenton catalysts and 38 times that of Fe 2+ . The reusability and the stability of Fe@Fe 2 O 3 core–shell nanowires were studied. Total organic carbon and ion chromatography analyses revealed the mineralization of rhodamine B and the releasing of nitrate ions. Gas chromatograph-mass spectrometry was used to investigate the degradation intermediates to propose the possible rhodamine B Fenton oxidation pathway in the presence of Fe@Fe 2 O 3 nanowires. This study not only provides a new Fenton oxidation system for pollutant control, but also widen the application of molecular oxygen activation induced by nanoscale zero valent iron .
研究领域:
环境科学
·
材料科学
✓ 已验证
DOI
高影响因子
ENVIRONMENTAL POLLUTION
·
2023
·
IF 8.9
Xiangyu Wang,Min Jiang,Iseult Lynch,Zhiling Guo,Peng Zhang,Lisi Wu,Jun Ma
Although Fe/Fe 2 O 3 has potential application compared with nanoscale zero-valent iron (nZVI), its smooth structure largely limits the catalytic performance. To address this challenge, we innovatively constructed highly efficient composite Fe/Fe 2 O 3 @UiO-66 via employing an urchin-like core-shell structure of Fe/Fe 2 O 3 onto UiO-66 through a facile ion exchange precipitation method without inert gas protection. The characterization results show the urchin-like core-shell configuration can extend the life span of Fe 0 and produce more active sites. Besides, the absorption spectrum is broadened by Fe 2 O 3 which has narrow band gap and the high-efficiency separation of photogenerated electron-hole pairs is obtained with the load of Fe/Fe 2 O 3 . Moreover, Two-parameter pseudo-first-order decay model fits well with the reduction and adsorption of composites in the dark reaction, and a plausible pathway for tetracycline (TC) degradation is also proposed. The findings of this research provide a promising method for promoting the catalytic properties of MOF-based materials and Fe/Fe 2 O 3 .
研究领域:
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2013
·
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.
研究领域:
环境科学
·
材料科学
·
化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF MOLECULAR LIQUIDS
·
2019
·
IF 4.561
Hongwei Luo,Yaoyao Zhao,Dongqin He,Qing Ji,Ying Cheng,Daoyong Zhang,Xiangliang Pan
Fe@Fe 2 O 3 core-shell nanowire is a promising heterogeneous Fenton iron catalyst to degrade organic pollutants. So far, the roles of hydroxylamine (HA) in Fe@Fe 2 O 3 /HA system for pollutant degradation still remain unknown. In this study, the HA-facilitated degradation of rhodamine B (RhB) and p-nitrophenol (PNP) by Fe@Fe 2 O 3 was reported and the underlying mechanisms were explored. Results show that addition of HA significantly enhanced degradation of organic pollutants and a higher HA dosage caused a faster degradation rate . The degradation process was completely inhibited by scavengers, indicating the hydroxyl radical (HO ) from bulk solution dominated the reactions. HA in the Fe@Fe 2 O 3 /H 2 O 2 /HA system was highly efficient to promote the generation of HO by accelerating both the Fe 3+ /Fe 2+ cycle and the H 2 O 2 decomposition. Meanwhile, HA itself was rapidly decomposed along with the pollutants degradation. About 50.5% of RhB and 46.4% of PNP were mineralized in the presence of HA. The effective pH value for degradation was expanded from 4.0 to 5.0. The EE/O calculations demonstrate that a higher energy input for PNP was required than that for RhB. This study will shed lights on the reactivity of the Fe@Fe 2 O 3 /HA system and provide an alternative pathway for removal of organic contaminants.
研究领域:
环境科学
·
化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2019
·
IF 7.65
Zhiwei Wang,Yahuan Wang,Shuai Cao,Shaohua Liu,Zhimin Chen,Jiafu Chen,Yong Chen,Jianwei Fu
The rational design of novel adsorption materials is imperative to remove toxic metal species from the polluted water. Herein, a core@shell structural Fe-Fe 2 O 3 @poly (hexachlorocyclotriphosphazene-co-polyethylenimine) (Fe-Fe 2 O 3 @PHCP) magnetic nanochain with high saturation magnetization was fabricated and used for effective adsorption and reduction of hexavalent chromium. The morphology and microstructure of Fe-Fe 2 O 3 @PHCP were characterized by scanning electron microscopy, transmission electron microscopy , Fourier transform infrared spectroscopy , X-ray diffraction and X-ray photoelectron spectroscopy. The effects of concentration, pH, contact time, temperature and coexisting ions on Cr (VI) removal were studied. Four kinetic models (pseudo-first-order, pseudo-second-order, Bangham and intraparticle diffusion models) and two isotherm models (Freundlich and Langmuir) were used to fit experimental data. Results show the adsorption capacity of Fe-Fe 2 O 3 @PHCP for Cr (VI) is up to 229.0 mg g −1 . The excellent performance was ascribed to the favorable reduction of Cr (VI) to Cr (III), followed by the chelation of Cr (III) with imino groups. Meanwhile, the residual Cr (VI) were adsorbed on protonated amino and imino groups. The adsorption process is exothermic and spontaneous and nicely follows pseudo-second-order kinetics, intraparticle diffusion model and Langmuir isotherm model. These results indicated that easily separable Fe-Fe 2 O 3 @PHCP magnetic nanochains could be a promising adsorbent to remediate chromate wastewater.
研究领域:
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
SN Applied Sciences
·
2019
·Vol. 1
·期 10
·1-11
·
IF 0
Geng Yuqing,Wang Zhiwei,Wang Yahuan,Song Jiayang,Chen Zhimin,Chen Jiafu,Chen Yong,Fu Jianwei
The development of excellent dye adsorbent with high adsorption capacity and good separation function is imperative to clean the wastewater. Herein, an innovative magnetic Fe–Fe 2 O 3 @poly(cyclotriphosphazene- co -polyethyleneimine) (named as Fe–Fe 2 O 3 @PCP) composite was fabricated through a facile copolymerization between hexachlorocyclotriphosphazene and polyethyleneimine in the presence of Fe–Fe 2 O 3 nanoparticles. With the help of scanning electron microscope, transmission electron microscope, Fourier transform infrared spectroscope and vibrating sample magnetometer, the microstructure of the resulting magnetic Fe–Fe 2 O 3 @PCP composite was characterized. Then, the adsorption performance of magnetic Fe–Fe 2 O 3 @PCP composite was evaluated by removing anionic dye acid chrome blue K (ACBK) from aqueous solution. The effects of contact time, initial solution pH and temperature on the adsorption of ACBK onto magnetic Fe–Fe 2 O 3 @PCP composite were systematically studied. The kinetics, isotherms and mechanism of the adsorption process were analyzed. Results show that the maximum adsorption capacity of the magnetic Fe–Fe 2 O 3 @PCP toward ACBK dye could be up to 260 mg g −1 at 25 °C in neutral solution. The adsorption kinetics follows both the pseudo-second-order kinetic model and the Weber’s intraparticle diffusion model well. And the Freundlich isotherm model can nicely fit the adsorption equilibrium data. The electrostatic attraction between Fe–Fe 2 O 3 @PCP and ACBK plays a dominant role in the adsorption process. Moreover, the magnetic Fe–Fe 2 O 3 @PCP composite owns a high saturation magnetization of 30.1 emu g −1 , rendering it rapid magnetic separability and good reusability. After five adsorption–desorption cycles, the magnetic composite still kept 75% of removal efficiency with the adsorption capacity of 195 mg g −1 . The excellent adsorption capacity and good magnetic separability make the magnetic Fe–Fe 2 O 3 @PCP composite a promising adsorbent for efficient removal of anionic dyes including ACBK from contaminated wastewater.
研究领域:
环境科学
·
材料科学
·
化学工程
✓ 已验证
产品关联
DOI
FOOD CHEMISTRY
·
2023
·
IF 8.8
Yu-Han Sun,Liu Yang,Xian-Xian Ji,Yuan-Zhen Wang,Yu-Long Liu,Ying Fu,Fei Ye
Flusilazole is a triazole fungicide with residues that are potentially toxic to humans. It enters the human body mainly through food, although its bactericidal activity is substantial. In this study, an electrochemical sensor Fe/Fe 2 O 3 @C with a core–shell structure was constructed to efficiently detect flusilazole by annealing MIL-53(Fe) which was prepared by a simple solvothermal method. Transmission electron microscopy and scanning electron microscopy were used to characterize the apparent morphology of MIL-53(Fe) and Fe/Fe 2 O 3 @C , and their structures were further characterized by X-ray photoelectron spectroscopy, Raman spectroscopy, powder X-ray diffraction, and the mapping of elements by energy dispersive spectroscopy. The electrochemical behavior of Fe/Fe 2 O 3 @C in the detection of flusilazole was evaluated by differential pulse voltammetry under optimal conditions. The results of the study indicate that the Fe/Fe 2 O 3 @C electrochemical sensor displayed excellent detection capabilities for flusilazole, where the sensor exhibited a wide detection range from 1.00 × 10 −4 to 1.00 × 10 −12 mol/L with an incredibly low LOD of 593 fM, making it highly sensitive to trace amounts of flusilazole. Moreover, Fe/Fe 2 O 3 @C demonstrated superior reproducibility, stability, and resistance to interference, highlighting its reliability in practical applications. The sensor was also successfully utilized to quantitatively detect flusilazole in various real samples, which suggests that Fe/Fe 2 O 3 @C has broad-spectrum environmental resistance and can effectively and rapidly detect flusilazole residues in different types of food items and environmental matrices. The study also delved into the mechanism of Fe/Fe 2 O 3 @C for the detection of flusilazole, providing a deeper understanding of the functionality of this sensor. Overall, these findings emphasize the practical significance of Fe/Fe 2 O 3 @C as an electrochemical sensor, showcasing its potential for real-world applications in food safety and environmental monitoring.
研究领域:
分析化学
·
食品安全
·
环境科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2016
·
IF 5.31
Wenjuan Shen,Fangjing Lin,Xu Jiang,Hefei Li,Zhihui Ai,Lizhi Zhang
In this study, we systematically investigated the removal of bromate (BrO 3 − ) with core-shell Fe@Fe 2 O 3 nanowires at neutral pH, especially the effects of surface bound ferrous ions and molecular oxygen. In the presence of Fe@Fe 2 O 3 nanowires, bromate was reduced to Br − efficiently with the generation of HOBr intermediates. Bromide species analyses and nanowires characterizations indicated that surface bound ferrous ions of core-shell Fe@Fe 2 O 3 nanowires could effectively promote the BrO 3 − removal. Meanwhile, molecular oxygen competed electrons from both Fe 2+ and Fe 0 to generate reactive oxygen species of O 2 − , H 2 O 2 , and OH during the bromate removal process. Among the generated reactive oxygen species, O 2 − and H 2 O 2 favored of bromate removal, but OH inhibited. We proposed a bromate removal mechanism with core-shell Fe@Fe 2 O 3 nanowires, which suggested that the effect of surface bound Fe(II) and molecular oxygen was taken into consideration when using nZVI for bromate remediation in waters. This study can not only deepen our understanding on the bromate removal with zero valent iron, and also shed light on the design of high performance bromate removal materials.
研究领域:
环境科学
·
材料科学
✓ 已验证
DOI
高影响因子
APPLIED PHYSICS A-MATERIALS SCIENCE & PROCESSING
·
2023
·Vol. 129
·期 10
·1-14
·
IF 2.7
Shi Lin,Bi Qinling,Zhu Jiamei,Yan Shili,Chen Dongxiang
A magnetic molybdenum disulfide (Fe–Fe 2 O 3 @PDA@MoS 2 ) was prepared and evaluated as a dispersive viscosity reducing catalyst for the heavy oil. The catalysts were analyzed using a variety of characterization methods, and the effects of preparation method and oleic acid treatment on performance were also compared. The particle size of Fe–Fe 2 O 3 magnetic nanochains was about 80 nm, the saturation magnetization strength was 110 emu/g, and the components in the nanochains were mainly iron elements. The catalyst further prepared by liquid phase precipitation had unique flower-like structure and good viscosity reduction ability. The loading amount of MoS 2 was 16.7 wt% and the saturation magnetization was 36.3 emu/g, while the saturation magnetization of the oleic acid treated sample was 28.9 emu/g. The as-prepared Fe–Fe 2 O 3 @PDA@MoS 2 can reach more than viscosity reduction 99% under 10 MPa hydrogen pressure and 400 ~ 415 °C. In addition, the component analyses of four groups (saturate, aromatic, resin, and asphaltenes) for the liquid products in the heavy oil were conducted to analysis the mechanism of viscosity reduction of catalyst.
研究领域:
催化化学
·
材料科学
·
石油加工工程
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2014
·
IF 3.065
Xing Ding,Zhihui Ai,Lizhi Zhang
In this study a dual-cell wastewater treatment system was constructed by coupling anodic photo-electrochemical/electro-Fenton (PEC) cell and cathodic electro-Fenton (EF) cell (D-PEC-EF), with the Bi 2 WO 6 nanoplates deposited on fluorine-tin oxide glass as the anode (Bi 2 WO 6 /FTO) and Fe@Fe 2 O 3 core–shell nanowires supported on activated carbon fiber (Fe@Fe 2 O 3 /ACF) as the gas diffusion cathode. The two separated cells could degrade rhodamine B (RhB) simultaneously and thus enhance the degradation efficiency and the TOC removal significantly in comparison with that of counterpart single-cell PEC-EF system (S-PEC-EF) because of more hydrogen peroxide electro-generated on the Fe@Fe 2 O 3 /ACF cathode by photo-generated electrons transferred from the Bi 2 WO 6 /FTO anode and less hydrogen peroxide consumed by anodic oxidation owing to the partition of two cells, which enhanced both PEC and EF oxidation ability and improved both photocatalytic quantum efficiency and overall current efficiency significantly. This study could not only provide a high effective and energy-saving advanced oxidation technology for wastewater treatment, but also deepen understanding of the synergic effect in dual-cell electrochemical process.
研究领域:
环境科学
·
化学工程
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）