ANALYTICAL AND BIOANALYTICAL CHEMISTRY
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2021
·Vol. 413
·期 7
·1983-1997
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IF 4.157
Jing Qi,Chen Liyuan,Zhao Qiaowei,Zhou Peipei,Li Yanyan,Wang Huili,Wang Xuedong
Herein, we developed a novel effervescence-assisted dual microextraction method, abbreviated as EM-LPSH, using lighter-than-water phosphonium-based ionic liquids (LPILs) and switchable hydrophilic/hydrophobic fatty acids (SHFAs). The EM-LPSH method was utilized for quick enrichment/extraction of polycyclic aromatic hydrocarbons (PAHs) in edible oils. Owing to lower density than water, LPILs used as the first extractant were floated on the upper layer of the aqueous phase, leading to a convenient separation/collection compared with traditional heavier-than-water imidazolium-based ionic liquids. Interestingly, SHFAs play triple functions: a dispersive solvent in the microextraction process, an acidic source in effervescent reaction, and the second extractant in dual microextraction, due to switchability from hydrophilicity to hydrophobicity. Consequently, the integration of LPILs with SHFAs greatly enhanced the extraction efficiency for PAHs owing to the quick dual microextraction process. Some important variables were rigorously optimized using a one-factor-at-a-time approach. Under optimized conditions, the EM-LPSH/HPLC-FLD method provided a wide linear range (0.07~0.63–200 μg kg −1 ), satisfactory recovery (80.12–103.27%), and low limit of detection (0.02–0.19 μg kg −1 ), as well as high intra-day and inter-day precision (0.03–6.55) for six PAHs in edible oils. By using certified reference material in olive oil samples (GBW10162), the recoveries ranged from 97.40 to 98.39%, demonstrating high accuracy and precision. According to the detected levels of PAHs in six unheated and heated oils, their edible safety was evaluated in detail. In short, the newly developed method is simple, convenient, and highly efficient, thereby showing great prospects for application in conventional monitoring of trace-level PAHs in edible oils.
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RSC Advances
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2021
·Vol. 11
·期 22
·13530-13536
·
IF 3.361
Yaxiong Zeng,Ming Zhang,Daohui Lin,Kun Yang
Recycling of washing effluent by selective sorption using resins is a feasible method to lower the operation costs of surfactant enhanced remediation (SER). In this study, correlations capable of predicting the selective sorption removal of polycyclic aromatic hydrocarbons (PAHs) by resin SP850 from TX100 solution to recycle washing effluent in SER were developed. A negative relationship of sorption coefficients (log Kf) of PAHs by resin SP850 with TX100 initial concentrations (log C0,TX100) and water solubilities (log Sw) of PAHs was observed, which indicated that solubility enhancement of PAHs in TX100 micelles was responsible for the decreasing of the selective sorption. Freundlich exponential coefficients (1/n) of PAHs were relatively constant (0.775 ± 0.012), suggesting that the sorption of PAHs by SP850 in the presence of surfactant is a surface adsorption process. The modified selectivity parameter (S*), having a relationship with log C0,TX100 and PAHs log Sw as well, could be employed to evaluate the efficiency of the selective sorption process and select the optimal TX100 concentration in washing effluents. For example, at the given SP850 dose of 1.0 g L−1, the optimal TX100 concentrations (CopTX100) for naphthalene, acenaphthene, phenanthrene, pyrene, anthracene and benzanthracene were about 4200, 7100, 8000, 10 000, 18 000 and 19 500 mg L−1, respectively, having a negative relationship with their log Sw. Moreover, the CopTX100 was independent of the solid-to-solution ratio of SP850 and TX100 solution containing PAHs. These correlations would be helpful for the application of SER in contaminated soils by giving a method to quantitatively predict the selective sorption behaviors of PAHs by SP850 from TX100 solution, especially for the CopTX100, using the Sw of organic compounds and surfactant concentrations.
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SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
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2021
·
IF 4.098
Maogang Li,Yaozhou Feng,Yan Yu,Tianlong Zhang,Chunhua Yan,Hongsheng Tang,Qinglin Sheng,Hua Li
Infrared spectroscopy (IR) combined with multivariate calibration technology can be used as a potential method to quantitative analysis of polycyclic aromatic hydrocarbons (PAHs) in soil, which provides a rapid data support for soil risk assessment. However, IR spectrum contains lots of useless information, its predictive performance is poor. Variable selection is an effective strategy to eliminate irrelevant wavelengths and enhance predictive performance. In this study, IR combined with partial least squares (PLS) was proposed to quantify anthracene and fluoranthene in soil. In order to improve the predictive performance of the PLS calibration model, the synergy interval PLS (siPLS) method was first used for “rough selection” to select feature bands; on this basis, “fine selection” was performed to extract the feature variables. In “fine selection”, three different feature variables selection methods, such as successive projection algorithm (SPA), genetic algorithm (GA), and particle swarm optimization (PSO), were compared for their performance in extracting effective variables. The results show that the siPLS-GA calibration model receive a lowest root mean square error (RMSE) and a largest determination coefficient (R 2 ). Results of external validation demonstrate an excellent predictive performance of siPLS-GA calibration model, with the R 2 = 0.9830, RMSE = 0.5897 mg/g and R 2 = 0.9849, RMSE = 0.4739 mg/g for anthracene and fluoranthene, respectively. In summary, siPLS combined with GA can accurately extract the effective information of the target substance and improve the predictive performance of the PLS calibration model based on IR spectroscopy.
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MICROCHEMICAL JOURNAL
·
2021
·
IF 4.821
Min Sun,Sen Han,Herman Maloko Loussala,Juanjuan Feng,Chunying Li,Xiangping Ji,Jiaqing Feng,Haili Sun
In order to develop an online detection method for polycyclic aromatic hydrocarbons (PAHs) in honey, graphene oxide-functionalized mesoporous silica was prepared and introduced as the coating in the field of in-tube solid-phase microextraction. An extraction tube was coupled to high performance liquid chromatography with diode array detector, and the online analytical system was constructed. After the main extraction and desorption conditions were optimized, a sensitive and online method based on matrix-matched calibration was established towards trace PAHs in honey. The method exhibited wide linear range from 0.8 ng g −1 to 250 ng g −1 and low detection limit of 0.25 ng g −1 , and the enrichment effect reached 2719. The proposed method was validated and successfully applied to the analysis of six honey samples. The extraction tube showed good durability and acceptable chemical stability during the experiment.
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FOOD CHEMISTRY
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2021
·
IF 7.514
Wenwen Deng,Anqi Huang,Qutong Zheng,Long Yu,Xiao Li,Hankun Hu,Yuxiu Xiao
A novel density-tunable liquid-phase microextraction (DT-LPME) system was developed with high-density deep eutectic solvents (DESs) as extractant and low-density organic solvents as emulsifier and density regulator. DES-rich phase was induced to form in the bottom or in the top by adjusting the emulsifier amount. This system was used to directly extract polycyclic aromatic hydrocarbons (PAHs) from liquid and solid foods, and the obtained DES-rich phase was easy to be collected for quantification. The method (LPME with HPLC-fluorescence detector) has linearity (R 2 > 0.9974), detection limits of 0.6–4.2 ng L -1 for liquid foods and 0.05–0.35 ng g −1 for solid foods, recoveries of 86.2–114.9%, and intra-day/inter-day RSDs below 6.6%. The method was applied to detect PAHs in real samples, and the PAHs residue was found in honey and five solid foods. The DT-LPME method is simple, fast, green and suitable for direct extraction of analytes from both liquid and solid samples.
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Scientific Reports
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2021
·Vol. 11
·期 1
·1-11
·
IF 4.38
Yang Zuoyi,Mao Xingchen,Cui Jiahao,Wang Yujie,Zhang Yaping
This study examines the specific effect of Tween 80 on the conversion of anthracene (ANT) in laccase medium system regarding surfactant chemical changes and mechanism. The conversion rate and degradation products of ANT were investigated in different concentrations of Tween 80 solution. Between Tween 80 concentration 0–40 critical micelle concentrations (CMC), the kinetic parameter-k (h −1 ) and corresponding half-life T 1/2 decreased with increasing concentration. When Tween 80 was above 20 CMC the laccase-medium system converted > 95% of ANT to anthraquinone within 12 h. During the entire enzymatic reaction, the laccase activity in the system increased with increasing Tween 80 concentration. Combined with GC/MS analysis of the product, it was speculated that hydrogens belonging to the ether-oxygen bond and carbon–carbon double bond α-CH of Tween 80, were removed by the laccase-media system, promoting its degradation. Additionally, enhanced activity caused by oxygen free radicals (ROS) such as RO• and ROO•, continuously oxidized Tween 80, which in turn produced free radicals while converting ANT. This study provides new theoretical support toward the application of surfactants in the elimination of polycyclic aromatic hydrocarbons.
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ACS Applied Materials & Interfaces
·
2021
·
IF 9.229
Shuquan Cui,Yiman Wei,Qiao Bian,Yan Zhu,Xiaobin Chen,Yaping Zhuang,Mingyan Cai,Jingyu Tang,Lin Yu,Jiandong Ding
Endoscopic submucosal dissection is an established method for the removal of early cancers and large lesions from the gastrointestinal tract but is faced with the risk of perforation. To decrease this risk, a submucosal fluid cushion (SFC) is needed clinically by submucosal injection of saline and so on to lift and separate the lesion from the muscular layer. Some materials have been tried as the SFC so far with disadvantages. Here, we proposed a thermogel generated by the “block blend” strategy as an SFC. This system was composed of two amphiphilic block copolymers in water, so it was called a “block blend”. We synthesized two non-thermogellable copolymers poly(d,l-lactide-co-glycolide)-b-poly(ethylene glycol)-b-poly(d,l-lactide-co-glycolide) and blended them in water to achieve a sol–gel transition upon heating in both pure water and physiological saline. We explored the internal structure of the resultant thermogel with transmission electron microscopy, three-dimensional light scattering, 13C NMR, fluorescence resonance energy transfer, and rheological measurements, which indicated a percolated micelle network. The biosafety of the synthesized copolymer was preliminarily confirmed in vitro. The main necessary functions as an SFC, namely, injectability of a sol and the maintained mucosal elevation as a gel after injection, were verified ex vivo. This study has revealed the internal structure of the block blend thermogel and illustrated its potential application as a biomaterial. This work might be stimulating for investigations and applications of intelligent materials with both injectability and thermogellability of tunable phase-transition temperatures.
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SCIENCE OF THE TOTAL ENVIRONMENT
·
2021
·
IF 7.963
Zhen-Zong Bao,Zhi-Feng Chen,Si-Qi Lu,Guangzhao Wang,Zenghua Qi,Zongwei Cai
Pollutant-attached microplastics have received increasing attention in recent years. However, information regarding the influence of hydroxyl group content of pollutants on the adsorption and desorption behavior is unclear, which affects their fate and risks in the aquatic environment. In this study, we investigated the adsorption and desorption behavior of anthracene (ANT) and its hydroxy derivatives (OHAs), including 2-hydroxyanthracene (MOHA), 2,6-dihydroxyanthracene (DOHA), and 1,8,9-trihydroxyanthracene (TOHA) on polyvinyl chloride (PVC) microplastics, and their interaction mechanism through the batch, characterization, and computational experiments. The results showed that the adsorption of ANT and OHAs on PVC microplastics conformed to the pseudo-second-order kinetic model and was exothermic spontaneously. The adsorption efficiency on PVC followed the order of ANT > MOHA > DOHA > TOHA, indicating that increase in hydroxyl group substitution degree will inhibit pollutant adsorption on PVC microplastics. Conversely, the release amounts of MOHA from PVC into simulated gastric fluids were higher than those of ANT. Experimental and computational results suggested that the affinity of ANT/OHAs to PVC microplastics was the most likely outcome in hydrophobic effect, electrostatic repulsion, and CH-π interaction forces. These findings help elucidate the mechanisms of pollutant adsorption on microplastics and evaluate the risk of pollutant-attached microplastics in the aquatic environment.
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JOURNAL OF CHROMATOGRAPHY A
·
2020
·
IF 4.049
Xiaohuan Zang,Yachao Pang,Hongda Li,Qingyun Chang,Shuaihua Zhang,Chun Wang,Zhi Wang
A covalent organic framework modified graphitic carbon nitride (g-C 3 N 4 @TpBD) was synthesized by modifying the graphitic carbon nitride (g-C 3 N 4 ) with a covalent organic framework (COF-TpBD). The synthesis conditions including the mass ratio between g-C 3 N 4 and benzidine (BD), solvent type, reaction temperature and reaction time were optimized. Under the optimal synthetic conditions, a novel spiny dendritic g-C 3 N 4 @TpBD adsorbent was obtained. The g-C 3 N 4 @TpBD was then coated on stainless-steel wire by sol-gel technique and the coated fiber was used for the solid phase microextraction of polycyclic aromatic hydrocarbons prior to gas chromatography-mass spectrometric detection. The established method was successfully applied to determine eight PAHs in six environmental water samples. Under the optimal extraction conditions, a wide linear quantification range for the analytes was obtained from 0.07 to 60.0 ng mL −1 with the coefficients of determination varying from 0.9979 to 0.9998, and the limits of detection (S/N = 3) ranged from 0.02 to 0.05 ng mL −1 . The relative recoveries of the analytes for the six environmental water samples at the spiked concentrations of 0.2, 0.5, 3.0 and 30.0 ng mL −1 were between 83.6% and 118% with the relative standard deviations ranging from 2.4% to 11.3%.
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CHINESE JOURNAL OF CHEMICAL ENGINEERING
·
2020
·
IF 2.627
Cui-Ping Ye,Ya-Fei Qiao,Rui-Nan Wang,Wen-Ying Li
To identify the effect of solvents and anthracene on the purification of carbazole, the solvent crystallization of carbazole was investigated with xylene, chlorobenzene and tetrachloroethylene (TCE) as solvents under two forced circulation cooling (FCC) modes. The co-crystalline experimental data were obtained from runs carried out at different anthracene levels between 1% (mass) and 10% (mass). The results showed that a uniform flake carbazole crystal obtained when using xylene and chlorobenzene under the FCC-1 mode with gradual cooling rate. Nevertheless, fine flake crystals grown under shock cooling of FCC-2 mode. It is beneficial to improving the purity of carbazole with chlorobenzene as solvent under cooling mode of FCC-1. Anthracene could promote the growth of carbazole in solution, and it has a significant influence on the purification of carbazole.
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MICROCHEMICAL JOURNAL
·
2020
·
IF 3.594
Zhengdong Shen,Haiying Wang,Qian Yu,Qiang Li,Xiaomin Lu,Xianming Kong
The accumulated polycyclic aromatic hydrocarbons (PAHs) in edible oil can bring serious health concerns because of their carcinogenic features. PAHs could accumulate in edible oil from contaminated environment or food stuff. In this study, the combination uses of on-site thin layer chromatography and surface enhanced Raman scattering (SERS) spectroscopy has been successfully displayed to identify PAHs from edible oil samples. Diatomite which is a kind of porous biosilica was used to construct stationary phase on TLC plate, the photonic crystal feature of diatomite is beneficial for SERS enhancement. The highly-porous stationary phase composed of porous diatomite with void shell structure could promote mobile phase interaction with the stationary phase, which leading to improved mass transfer, uniformity and analyte resolution compare with the conventional silica gel plate. The edible oil (1 µL) was directly applied to the diatomite plate without pretreatment, and subjected to TLC separation. The polarity of target analytes was calculated for eluent optimization, on which four compounds of PAHs(benzo[a]pyrene, pyrene, anthracene and indeno[1,2,3-cd] pyrene) were successfully separated by using hexane/chloroform (15/1, v/v) as eluent, including compounds with similar polarity(benzo[a]pyrene 0.0477, indeno[1,2,3-cd] pyrene 0.6545, pyrene and anthracene are 0). 2 µL of Au colloid at 2.4 × 10 −7 M were transferred onto the diatomite plate for the SERS measurement. The limit of detection was found to be nearly at 1 ppm. The obtained results can easily identify the four compounds of PAHs in edible oil by their own characteristic Raman peaks. This proposed method provides a simple, instant and effective strategy for on-site identification PAHs from food samples.
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Catalysts
·
2020
·Vol. 10
·期 12
·1379
·
IF 3.52
He Liu,Shiguang Fan,Xu Gong,Jian Wang,Aijun Guo,Kun Chen,Zongxian Wang
Partial hydrogenation of anthracene under CO-H2O, N2-H2O, and H2-H2O over Fe-based catalysts was studied at 400 °C and 10 MPa. Results show that the Fe-based catalysts display obvious catalytic activity for anthracene hydrogenation under CO-H2O instead of hydrogenation under N2-H2O and H2-H2O. The activity follows in the order of Fe(NO3)3·9H2O > Fe naphthenate > FeSO4·7H2O. Even though the amount of molecular hydrogen remains higher than that of in situ hydrogen, the anthracene conversion with in situ hydrogen is remarkably higher. It demonstrates that the in situ hydrogen is more active than molecular hydrogen for PAH hydrogenation. To further reveal the exact fate of these Fe-based catalysts, the decomposed products under CO-H2O, N2-H2O and H2-H2O were characterized by TG, XRD, and TEM. Results indicate that the Fe3O4species play a key role in hydrogenation of anthracene under CO and H2O. Higher catalytic activity for Fe(NO3)3·9H2O is due to its complete decomposition at 350 °C to acquire higher concentration of active Fe3O4species. The possible form of in situ hydrogen during this process is also discussed. Given that heavy oil contains abundant polyaromatics, these results are meaningful for enhancing hydrogen shuttling to heavy oil by producing natural hydrogen donors and, thus, benefiting the high-efficient upgrading.Keywords:PAH hydrogenation;in situ hydrogen;water gas shift reaction;natural hydrogen donors
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