MICROCHIMICA ACTA
·
2017
·Vol. 184
·期 8
·2981-2990
·
IF 4.58
Wang Ting,Liu Siyu,Gao Guihua,Zhao Pan,Lu Nan,Lun Xiaowen,Hou Xiaohong
The authors describe a method for magnetic solid phase extraction (MSPE) combined with ultra-high performance liquid chromatography-tandem mass spectrometry (UPLC-MS/MS) for the quantitation of eight non-steroidal anti-inflammatory drugs (NSAIDs) in wastewater and environmental water samples. Specifically, the NSAIDs were directly extracted by using a magnetic nanocomposite of type Fe 3 O 4 /MIL-101(Cr) (Matérial Institute Lavoisier, MIL) from 50 mL water samples without any further cleanup. The effects of the amount of adsorbent, pH value, salt concentration, ultrasonic extraction time, desorption solvent nature and volume and desorption time were investigated. Under the optimal conditions, UPLC-MS/MS based detection resulted in the following figures of merit: (a) Linear calibration plots that typically extend from 0.1 (0.2, 0.05, 0.02) to 50 μg·L −1 , depending on the compound; (b) detection limits between 3 to 60 ng·L −1 ; and (c), recoveries varying from 81.2% to 116.8% with relative standard deviations between 0.4% and 10.8%. The adsorption of NSAIDs on Fe 3 O 4 /MIL-101(Cr) was characterized by adsorption isotherms, kinetics and thermodynamics studies and provides a deeper insight into the adsorption mechanism. Compared to other method for pretreatment and preconcentration of NSAIDs, the new method is more rapid, sensitive, accurate and eco-friendly. The method was successfully applied to the determination of the NSAID residues in a variety of real environmental and wastewater samples.
Schematic of a method for determination of non-steroidal anti-inflammatory drugs (NSAIDs) in environmental water by magnetic solid phase extraction based on Fe 3 O 4 /MIL-101(Cr) combined with UPLC-MS/MS. The adsorption mechanism of NSAIDs on Fe 3 O 4 /MIL-101(Cr) was studied.
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CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Shi-Wen Lv,Qiuyu Zheng,Lingjie Ye,Chun-Yang Li,Jing-Min Liu,Yanqing Cong,Shuo Wang
Nowadays, simultaneous removal of organic pollutants and heavy metals from wastewater is still a complicated task with great challenge. Herein, a newly-designed Fe-g-C 3 N 4 /α-Fe 2 O 3 composite with an active N-Fe-O bridge was prepared by coupling Fe-doped g-C 3 N 4 (namely Fe-g-C 3 N 4 ) and α-Fe 2 O 3 . Interestingly, the combination of Fe-g-C 3 N 4 with α-Fe 2 O 3 broadened the light absorption region and restrained the photoinduced electron-hole pair recombination. Meanwhile, elaborate construction of N-Fe-O bridges based on coordination interaction can reduce electrochemical impedance and facilitate electron transfer, thereby prolonging the charge lifetime. As expected, the Fe-g-C 3 N 4 /α-Fe 2 O 3 composite displayed excellent photocatalytic performance in simultaneous removal of tetracycline (TC) and Cr(VI). More importantly, Fe-g-C 3 N 4 /α-Fe 2 O 3 -mediated electron transfer from TC to Cr(VI) also played an essential role on TC oxidation and Cr(VI) reduction under visible light. Both experimental analyses and theoretical calculations revealed that the migration route of photogenerated carriers followed a direct Z-scheme heterojunction mechanism under built-in electric field. The Fe-g-C 3 N 4 /α-Fe 2 O 3 composite with great stability also displayed promising practical application potential. In short, the current work not only provided a highly-efficient photocatalyst with N-Fe-O bridges but also shared new insights into the simultaneous removal of organic pollutants and heavy metals.
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APPLIED CATALYSIS A-GENERAL
·
2019
·
IF 4.63
Ziai Huang,Kexin Li,Liushui Yan,Huiqin Guo,Shenglian Luo
In this paper, bio-based acidic nonmetals co-doped titanium dioxide (C-SO 3 H/CN-TiO 2 ) with core/shell microstructure is successfully fabricated by a simple method. The synergistic effect of surface hydrogen ions (H + ) provided by sulfonic acid groups ( SO 3 H) functionalized bio-based carbon cores and photogenerated electrons generated by the visible-light excitation of nonmetals co-doped titanium dioxide (TiO 2 ) shells makes the as-prepared C-SO 3 H/CN-TiO 2 can rapidly reduce aqueous hexavalent chromium [Cr(VI)] under original pH condition. The addition of inorganic or organic acid is avoided during the photocatalytic reduction of aqueous Cr(VI). Therefore, the secondary pollution is effectively prevented during Cr(VI) reduction. The SO 3 H can be easily loaded on the surface of bio-based carbon cores by the thermal effect of light irradiation in concentrated H 2 SO 4 due to the aromatic carbon framework of bio-based carbon cores. The successful introduction of C and N elements into TiO 2 shells allows the as-prepared C-SO 3 H/CN-TiO 2 to exhibit a visible-light photocatalytic activity. Aqueous Cr(VI) having a concentration of 10 mg/L can be completely reduced after 180 min of visible-light irradiation under original pH condition.
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TALANTA
·
2016
·
IF 4.035
Xiuna Jia,Pan Zhao,Xiu Ye,Lianjun Zhang,Ting Wang,Qinyu Chen,Xiaohong Hou
As a novel material, metal-organic framework/graphite oxide (MIL-101(Cr)@GO) has great potential for the pretreatment of trace analytes. In the present study, MIL-101(Cr)@GO was synthesized using a solvothermal synthesis method at the nanoscale and was applied as sorbent in the dispersive micro-solid phase extraction (DMSPE) for the enrichment of the trace sulfonamides (SAs) from milk samples for the first time. Several experimental parameters including kinds of sorbents, the effect of pH, the amount of MIL-101(Cr)@GO, ionic strength , adsorption time, desorption solvent and desorption time were investigated. Under the optimal conditions, the linear ranges were from 0.1 to 10 μg/L, 0.2–20 μg/L or 0.5–50 μg/L for the analytes with regression coefficients ( r ) from 0.9942 to 0.9999. The limits of detection were between 0.012 and 0.145 μg/L. The recoveries ranged from 79.83% to 103.8% with relative standard deviations (RSDs)<10% ( n =3). MIL-101(Cr)@GO exhibited remarkable advantages compared to MIL-101(Cr), MIL-100(Fe), activated carbon and other sorbent materials used in pretreatment methods. A simple, rapid, sensitive, inexpensive and less solvent consuming method of DMSPE-ultra-high performance liquid chromatography-tandem mass spectrometry (DMSPE-UHPLC-MS/MS) was successfully applied to the pre-concentration and determination of twelve SAs in milk samples.
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高影响因子
ANALYST
·
2015
·Vol. 140
·期 15
·5308-5316
·
IF 4.107
Ting Wang,Jian Wang,Conglu Zhang,Zhao Yang,Xinpeng Dai,Maosheng Cheng,Xiaohong Hou
An attractive metal–organic framework (MOF) MIL-101(Cr) material was synthesized at the nanoscale and applied as a sorbent in the porous membrane-protected micro-solid-phase extraction (μ-SPE) device for the pre-concentration of phthalate esters (PAEs) in drinking water samples for the first time. Parameters influencing the extraction efficiency, such as the selection of sorbent materials, pH adjustment, the effect of salt, magnetic-stirring extraction time, the desorption solvent and the desorption time, were investigated. Under the optimum conditions, the limits of detection from gas chromatography-mass spectrometric analysis for PAEs varied from 0.004 to 0.02 μg L−1. The linear ranges were from 0.1 to 50 μg L−1 or from 0.2 to 50 μg L−1 for the analytes with the relative standard deviations fluctuating from 0.8 to 10.9% (n = 5). The enrichment factors (EFs) for the target PAEs were varied from 143 to 187. MIL-101(Cr) exhibited remarkable advantages compared to activated carbon and MIL-100(Fe). On the other hand, the computational method was first used to predict the adsorption of MIL-101(Cr) towards PAEs. The molecular interactions and the free binding energies between MIL-101(Cr) and PAEs were observed and calculated in terms of the molecular modeling method. MIL-101(Cr) showed high potential in the analysis of PAEs at trace levels in drinking water. The computational result was consistent with the detected enrichment factors. The computational modeling accurately predicted the extraction efficiency of MOF-based material towards the target analytes. Therefore, the combination of experimental and computational study provided a new strategy on the trace contaminant analysis.
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NEW JOURNAL OF CHEMISTRY
·
2019
·Vol. 43
·期 30
·12126-12136
·
IF 3.069
Lingzhe Suo,Jing Zhao,Xinyi Dong,Xun Gao,Xinzhu Li,Jianfeng Xu,Xiumei Lu,Longshan Zhao
A novel polyaniline–polypyrrole functionalized SiO2-coated magnetic graphene oxide composite (MGO/SiO2@PANI–PPy) was prepared as a new magnetic solid-phase extraction (MSPE) adsorbent for separation and pre-concentration of chromium (Cr) and lead (Pb) at trace levels in food and environmental water samples followed by the use of inductively coupled plasma mass spectrometry (ICP-MS). Fourier transform infrared (FTIR) spectroscopy, vibrating sample magnetometry (VSM), scanning electron microscopy (SEM), transmission electron microscopy (TEM) and X-ray diffraction (XRD) were used to characterize the nanocomposite. Various parameters affecting the extraction yield of heavy metals were optimized using a Box–Behnken design (BBD) through the response surface methodology (RSM). Under optimum conditions, the limits of detection (LODs) were 4.808 ng L−1 for Cr(III) and 3.401 ng L−1 for Pb(II) with relative standard deviations (RSDs) of less than 5% (n = 6). Furthermore, the maximum adsorption capacities of this new sorbent were 188.9 and 213.3 mg g−1 for Cr(III) and Pb(II), respectively. Finally, the developed method was successfully applied for determination of trace Cr(III) and Pb(II) in rice, milk, wine and environmental water samples with recoveries within 95.4–105%.
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MICROCHIMICA ACTA
·
2018
·Vol. 186
·期 1
·1-10
·
IF 5.705
Zhang Li,Li Shaobin,Xin Jianjiao,Ma Huiyuan,Pang Haijun,Tan Lichao,Wang Xinming
A Cr-based metal-organic framework MIL-101(Cr) was used to load platinum nanoparticles (PtNPs) that were placed on a glassy carbon electrode (GCE). The modified GCE was used as a non-enzymatic xanthine sensor. Compared to bare GCE, it requires a strongly decreased working potential and an increased signal current for xanthine oxidation. This is due to the crystalline ordered structure and large specific surface of the MIL-101(Cr), and to the high conductivity of the Pt NPs. Differential pulse voltammetry (DPV) shows the sensor to have a wide linear range (0.5 – 162 μM), a low detection limit (0.42 μM), and high selectivity. It was applied to the simultaneous determination of dopamine, uric acid, xanthine and hypoxanthine at working potentials of 0.13, 0.28, 0.68 and 1.05 V, respectively (vs. Ag/AgCl) and to quantify xanthine in spiked serum samples.
This is the first report of non-enzymatic xanthine electrochemical sensor based on metal-organic framework loaded with nanoparticles.
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ANALYTICAL AND BIOANALYTICAL CHEMISTRY
·
2016
·Vol. 408
·期 29
·8515-8528
·
IF 3.125
Lu Nan,Wang Ting,Zhao Pan,Zhang Lianjun,Lun Xiaowen,Zhang Xueli,Hou Xiaohong
In the presented work, metal-organic framework (MOF) material MIL-101(Cr) (MIL, Matérial Institute Lavoisier) was used as a sorbent for vortex assisted dispersive micro-solid-phase extraction (VA-D-μ-SPE) of trace amount of metronidazole (MNZ), ronidazole (RNZ), secnidazole (SNZ), dimetridazole (DMZ), tinidazole (TNZ), and ornidazole (ONZ) in different environmental water samples. Ultra-high-performance liquid chromatography coupled with tandem mass spectrometry (UPLC-MS/MS) was used to quantify the target analytes. The extraction conditions, including type of sorbents, amount of MIL-101(Cr), solution pH, extraction method, extraction time, effect of salt, and elution conditions were investigated. Upon the optimal conditions, the developed method showed an excellent extraction performance with the average recovery ranging from 75.2 to 98.8 %. Good sensitivity levels were achieved with the detection limits of 0.03∼0.06 μg/L and the quantitation limits of 0.09∼0.20 μg/L. The linear ranges were varied from 0.1 to 20 for SNZ and ONZ and from 0.2 to 40 μg/L for MNZ, RNZ, DMZ, and TNZ ( r
2 > 0.992), and repeatability of the method was satisfactory with the relative standard deviations (RSD) <8 %. Ultimately, the applicability of the method was successfully confirmed by the extraction and determination of 5-nitroimidazoles (5-NDZs) in 12 real water samples, showing the positive findings of MNZ and TNZ ranging from 0.3 to 1.0 μg/L. Furthermore, molecular docking was applied to explain the molecular interactions and free binding energies between MIL-101(Cr) and 5-NDZs, providing a deep insight into the adsorption mechanism. The proposed method exhibited the advantages of simplicity, rapidly, less solvent consumption, ease of operation, higher sensitivity, and lower matrix effect.
Schematic diagram of the extraction process and molecular docking investigation
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JOURNAL OF PHARMACEUTICAL AND BIOMEDICAL ANALYSIS
·
2019
·
IF 2.983
Qianqian Cai,Tianyu Zhao,Lianjun Zhang,Pan Zhao,Yajie Zhu,Haiyan Xu,Xiaohong Hou
Dispersive micro-solid-phase extraction (DMSPE) combined with dispersive liquid–liquid microextraction based on the solidification of a floating organic droplet (DLLME-SFO) was successfully developed for extraction and depuration of pantoprazole in rat plasma. The remarkable metal organic framework (MOF), MIL-101(Cr) was used as DMSPE adsorbent. The detection of pantoprazole was performed by convenient HPLC-UV. In the extraction of pantoprazole from plasma samples, small molecule compounds, including the target and abundant impurities, were easily admitted into the porous structure of MIL-101 (Cr) material in DMSPE; while, macromolecular compounds were handily excluded from the adsorbent. Next, the depuration process was achieved by removal of small polar impurities in DLLME-SFO. Influential factors were systematically optimized for ideal enrichment and depuration efficiency. Under the optimal conditions, a satisfactory linearity range from the lower limit of quantification (LLOQ, 100 ng/L) to 10 000 ng/L with the correlation coefficients ( r ) of 0.9934 was obtained. The LLOQ was 100 ng/mL and the relative recoveries were ≧ 73.2 ± 4.8%. The approving reproducibility, acceptable accuracy, and stability were all within the acceptance limits. This proposed method presented the advantages of environment-friendly, low-cost, recyclable, low impurity, and preferable applicability. It could offer a new idea for the pretreatment and pharmacokinetic study of pantoprazole in rat plasma.
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