ANALYST
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2021
·Vol. 146
·期 21
·6643-6649
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IF 4.616
Qiaoyan Li,Zhentao Li,Yuanyuan Fu,Igor Clarot,Ariane Boudier,Zilin Chen
Covalent organic frameworks (COFs) are a class of porous materials with high surface area, high porosity, good stability and tunable structure that have been widely used in the separation area. In this work, we have proposed the in situ synthesis of a novel COF composed of 4,4′,4′′-(1,3,5-triazine-2,4,6-triyl)trianiline (Tz) and 1,4-dihydroxyterephthalaldehyde (Da) onto the capillary inner surface for electrochromatographic separation. Fourier transform infrared (FT-IR) spectroscopy, elemental analysis (EA) and scanning electron microscopy (SEM) have facilitated the characterization of the prepared capillary columns. The COF (TzDa) modified OT-CEC column exhibited satisfactory separation selectivity towards neutral compounds (such as chlorobenzenes and alkylbenzenes), acidic and basic compounds (such as phenols and anilines), food additives (vanillin and its analogues) and small biomolecules (such as amino acids and polypeptides). Furthermore, the TzDa modified capillary was quite stable and reproducible. The relative standard deviations for retention times of the test analytes (alkylbenzenes) were as follows: for intra-day (n = 3) runs (≤1.74%), inter-day (n = 3) runs (≤2.25%) and between columns (n = 3) (≤4.83%). This new type of COF-based stationary phase has tremendous potential in separation science.
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CHEMICAL ENGINEERING JOURNAL
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2021
·
IF 13.273
Luyi Chen,Junlong Huang,Yueru Shi,Xiaoru Peng,Yixin Kuang,Suxin Zhou,Juan Zheng,Xin Yang,Gangfeng Ouyang
Systematic investigation on the adsorption performance of polystyrene-based nanospheres towards persistent organic pollutants (POPs) is of great importance to the design of high-capacity adsorbent and the toxicological risk assessment of nano plastic. In this study, a series of polystyrene-based nanospheres with controllable microstructures, have been constructed successfully as model adsorbents, by the strategies of emulsion polymerization, hyper-crosslinking and direct carbonization. In the form of Solid phase microextraction (SPME) coatings, the impacts of microstructures on the adsorption performance of constructed nanospheres have been highlighted, by employing benzene series, polycyclic aromatic hydrocarbons (PAHs) and polychlorinated biphenyls (PCBs) as target adsorbates. Moreover, it is surprisingly found that the grafted F atoms make PS demonstrate better enrichment effects towards PCBs than the Cl atoms, mainly due to stronger sigma (σ)-hole interactions between F atoms and PCBs. In consideration of the most outstanding performance, the F-functionalized nanospheres (xFFNs)-coated SPME fiber is employed for the enrichment of PCBs from water samples, and the enrichment factors range from 1500 to 10030. After coupling the xFFNs-coated fiber with gas chromatography-mass spectrometry (GC-MS), highly sensitive analytical method is developed with detection limits of 0.08–0.89 ng L −1 , realizing precise quantifications of trace PCBs in treated sewage samples.
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TALANTA
·
2019
·
IF 4.916
Xiaohui Yang,Guangping Wan,Shujuan Ma,Hongjun Xia,Jun Wang,Jiawei Liu,Yanna Liu,Gang Chen,Quan Bai
Recently, superficially porous particles (SPPs) have been intensively studied and employed for highly efficient and fast separations. In this paper, the SiO 2 @SiO 2 SPPs were synthesized by an improved polymerization-induced colloid aggregation (PICA) method using urea-formaldehyde polymer as the template. The agglomeration of silica core during modification with ureidopropyltrimethoxysilane (UPS) can not only be avoided by reflux in neutral ethanol solution, but also the secondary nucleation of the colloidal silica sol can be inhibited via optimizing the reaction conditions including pH, temperature, colloidal silica sol concentration and the reaction time. The shell thickness and pore size of SPPs can be controlled successfully by adjusting the weight ratio of silica core/colloidal silica sol and the particle size of colloidal silica sol, respectively. The SPP-C18 columns packed using octadecyltrichlorosilane (ODS) modified SPPs with different pore sizes were employed to separate small solutes and proteins. The baseline separations of 6 kinds of alkyl benzenes and 5 kinds of aromatic alcohol homologues were achieved within 4 min by the SPP-C18 column with 8 nm pore size. Compared with the commercial BEH-C18 column, more than 50,000/m of the plate number of propylbenzene was obtained, and the former provided higher column efficiency to separate small solutes than the latter. Meanwhile, 6 kinds of proteins were also separated completely within 2 min using the SPP-C18 column with 40 nm pore size. In addition, the SPP-C18 capillary column was applied to separate and identify the BSA/HeLa/mouse liver digests with capillary LC-MSMS, respectively. The results indicate that more proteins and peptides can be identified using SPP-C18 capillary column compared with commercial silica-C18 capillary column. The result demonstrates that the prepared SPP-C18 column provides higher column efficiency and the SPPs synthesized with the improved PICA method shows a great potential application for the fast separation of small solutes and proteins.
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JOURNAL OF CHROMATOGRAPHY A
·
2019
·
IF 3.858
Yike Huang,Gaoyi Yi,Baian Ji,Die Gao,Yuntian Bai,Yao Liu,Lujun Wang,Zhining Xia,Qifeng Fu
Mussel-inspired polydopamine (PDA) based materials are attractive as stationary phase for open-tubular capillary electrochromatography (OT-CEC) due to their many fascinating properties. However, all of the existing strategies for fabricating PDA based OT-CEC columns are limited in aqueous solutions. Consequently, it is a challenge work to directly immobilize the hydrophobic functional materials onto the inner wall of PDA modified capillary. Herein, by using the organic amine-inducing co-deposition strategy, a novel preparative method was developed for in situ one-pot synthesis of PDA/octadecylamine (ODA) co-deposited coating inside capillary as OT-CEC stationary phase. The formation and morphology of the PDA/ODA co-deposited coating were characterized by field emission scanning electron microscopy , atomic force microscope, attenuated total reflectance Fourier transform infrared spectroscopy and contact angle measurements. The separation performance of the fabricated PDA/ODA modified columns was validated by the separation of alkylbenzenes and steroids, which could achieve baseline separation with high separation efficiency. Their separation was found to follow the reversed phase chromatographic retention mechanism. The co-deposited column showed good stability and long lifetime. The repeatability of the PDA/ODA co-deposited column was also evaluated, with the relative standard deviations for intra-day and inter-day runs less than 5% and column-to-column runs less than 6%.
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Separation Science Plus
·
2019
·Vol. 2
·期 12
·432-439
·
IF 0
Yu-Yu He,Qing Pu,Jun-Hui Zhang,Sheng-Ming Xie,Xue-Xian Chen,Li-Ming Yuan
Mesoporous materials are promising functional materials due to their properties, such as a large surface area, tunable pore size, structure and morphology. Chiral mesoporous silica is an indispensable part of mesoporous materials. Considering that chirality is rare in inorganic mesoporous materials, there are very few reports on chiral inorganic mesoporous silica for chromatographic separations. In this work, we report the use of chiral inorganic mesoporous silica based on the template of myristyl chloride- l -valine sodium as the stationary phase for enantioselective separation in gas chromatography. Thirteen chiral compounds were resolved on a fabricated column using dynamic coating, including chiral alcohols, epoxides and amino acid derivatives. In addition, n -alkanes, n -alcohols and aromatic hydrocarbons have also been separated.
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Nanoscale
·
2019
·Vol. 11
·期 6
·2805-2811
·
IF 6.97
Xingru Hu,Chaohai Wang,Rui Luo,Chao Liu,Junwen Qi,Xiuyun Sun,Jinyou Shen,Weiqing Han,Lianjun Wang,Jiansheng Li
Efficient extraction of pollutants with different chemical properties from environmental samples has attracted great attention in the development of analytical chemistry. However, it is still a challenge to develop an appropriate and sensitive adsorbent for determining broad-spectrum analytes. Herein, zeolitic imidazole framework-8 (ZIF-8)-derived double-shelled hollow zinc oxide/carbon (ZnO/C) nanocubes were reported as a novel coating for solid-phase microextraction (SPME). The nanocubes with a unique structure and composition were obtained by controlled etching of ZIF-8 with tannic acid (TA) followed by pyrolysis. When a ZnO/C nanocube-coated fiber (ZnO/C–F) was used to extract the complex environmental samples containing both nonpolar (benzene compounds (BTEX)) and polar (chlorophenols (CPs)) pollutants, excellent extraction performance was achieved; we obtained low detection limits (0.14–0.56 ng L−1 for BTEX and 1.10–2.84 ng L−1 for CPs), good repeatability (2.2–5.9% for six replicated extractions) and excellent reproducibility (0.61–7.8%, fiber to fiber). The broad-spectrum SPME performance was ascribed to the synergistic effect between the composition and structure of ZnO/C nanocubes. Compositionally, the uniform dispersion of ZnO and carbon framework could provide abundant adsorption active sites, where Zn-OHs bound CPs by hydrogen bonding and carbon absorbed BTEX through π–π stacking interaction and hydrophobic interaction. Structurally, the double-shelled hollow morphology of the nanocubes was favorable for the sensitive extraction. Finally, the established ZnO/C–F-based headspace-SPME method was used for the preconcentration and determination of abundant analytes from real water samples. These findings open the door for the practical use of double-shelled hollow multicompositional inorganic materials.
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ELECTROPHORESIS
·
2019
·
IF 2.754
Yuan-Yuan Cui,Huan Yao,Cheng-Xiong Yang,Xiu-Ping Yan
Microporous organic networks (MONs) are a new class of porous materials synthesized via Sonogashira coupling reactions between organic building blocks. Here we report an in situ synthesis approach to fabricate MONs coated capillary column for high resolution GC separation of hydrocarbons. The McReynolds constant evaluation reveals the MONs coated capillary is a non-polar column. The MONs coated capillary column shows good resolution for GC separation of diverse important industrial hydrocarbons such as linear and branched alkanes, alkylbenzenes, pinene isomers, ethylbenzene and styrene, cyclohexane and benzene. The MONs coated capillary column gave a high column efficiency of 1542 plates per meter for hexane and good precision for replicate separations of the selected hydrocarbons with the RSDs of 0.2–0.3, 1.5–3.1, and 1.9–3.3% for retention time, peak height and peak area, respectively. The MONs coated capillary also offered better resolution than commercial Inert Cap-1 and Inert Cap-5 capillary columns for hexane and heptane isomers. These results reveal the potential of MONs as novel stationary phases in GC.
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JOURNAL OF HAZARDOUS MATERIALS
·
2019
·
IF 7.65
Qun Zhao,Yingjie Li,Xiaolong Chai,Linzhen Xu,Linfeng Zhang,Ping Ning,Jianhong Huang,Senlin Tian
Exposure of volatile organic compounds (VOCs) towards lung leads to pulmonary dysfunctions and various lung diseases. However, the interaction of VOCs with pulmonary surfactant (PS) that directly comes into contact with inhaled VOCs is unknown. Here, simulated PS extracted from porcine lungs (EPS) was used to study the interaction with BTEX (i.e., benzene, toluene, ethylbenzene, and p -xylene) as representatives of VOCs. Surface pressure-area (π-A) isotherms showed that in the presence of individual BTEX, EPS monolayer’s phase conversion from gas to liquid expanded phase was dramatically influenced and its collapse pressure decreased greatly compared to those of EPS alone, which was attributed to the alteration of EPS monolayer’s microstructure characterized by atomic force microscopy and Brewster angle microscopy. Solubilization experiments manifested that EPS and its major components (dipalmitoyl phosphatidylcholine, DPPC; bovine serum albumin, BSA) exhibited obvious solubilization effects on individual BTEX. The solubilization capacity followed an order: EPS > DPPC > BSA, which was positively correlated with hydrophobicity of individual BTEX. Synergistic solubilization test unveiled that the mixed phospholipid components were largely responsible for the solubilization capacity of EPS. These findings indicate that VOCs exposure may induce potential pulmonary health risk due to the alteration of gas-liquid interfacial properties of PS.
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ACS Catalysis
·
2019
·
IF 12.221
Yanfu Ma,Banlan Chi,Wei Liu,Lina Cao,Yue Lin,Xiaohui Zhang,Xuxu Ye,Shiqiang Wei,Junling Lu
Atomically dispersed metal atoms on supports, so-called single-atom catalysts (SACs), have recently attracted extensive attention in the catalysis field. It has been found that besides the primary metal atom, the proximial atoms also contribute to the catalytic activity significantly. Here, we show that tailoring of the local coordination environment of Pt1 single atoms on CeO2 using phosphorus gives rise to an activity enhancement up to a 10 times higher than Pt1/CeO2 SAC in hydrogenation of styrene, cyclohexene, phenylacetylene, and nitrobenzene. X-ray absorption, photoelectron, and infrared spectroscopies showed that the Pt1 single atoms modulated by phosphorus have a higher valence state. Infrared spectroscopy and temperature-programmed reduction further unveiled that significantly stronger adsorption of reactant and facilitated hydrogen spillover on phosphorus-doped CeO2 both play important roles for the dramatic activity enhancement. These findings point out an avenue to design an advanced SACs with high activity.
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MICROPOROUS AND MESOPOROUS MATERIALS
·
2019
·
IF 4.182
Yeqing Wang,Jian Zhang,Xiangju Meng,Shichao Han,Qiuyan Zhu,Na Sheng,Liang Wang,Feng-Shou Xiao
In this work, we show sustainable and efficient synthesis of nanosized EMT zeolite under organotemplate-free and solvent-free conditions, which not only completely avoids the use of organic templates for production of NOx and CO 2 but also effectively reduces the formation of polluted water. In addition, the yield of EMT zeolite is significantly enhanced by this route, compared with conventional hydrothermal synthesis . The nanosized EMT zeolite obtained has good crystallinity, uniform crystal size distribution, and high surface area. Ion-exchange tests show that the nanosized EMT zeolite owes high Ca 2+ and Mg 2+ ion exchange capacity at room temperature, which is potentially important for softening hard water in the industrial processes. Catalytic tests in Knoevenagel condensation show that the nanosized EMT zeolite exhibits higher activity than that of the EMT zeolite synthesized using organic template, indicating the importance of the nanosized EMT zeolite as a base catalyst.
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FUEL PROCESSING TECHNOLOGY
·
2019
·
IF 4.507
Chen Zhu,Jing-Pei Cao,Xiao-Yan Zhao,Tao Xie,Ming Zhao,Xian-Yong Wei
The synergistic catalysis in the catalytic hydrogenolysis (CH) of lignin and its model compounds over a Ni-Ru/AC bimetallic surface was well established. The Ni-Ru/AC exhibits excellent activity and stability for catalytic hydrogenolysis of lignin and its model compound. The additions of Ru into supported Ni/AC can not only improve the overall reactants conversion, but also modify the product distribution. The apparent activation energy (E a ) of BPE hydrogenolysis over Ni-Ru/AC is measured approximately to be 18.3 kJ/mol. This value is considerably lower than the values measured for monometallic Ni/AC (42.4 kJ/mol). Additionally, the turnover frequency (TOF) of Ni-Ru/AC (62.7 h −1 ) was much higher than that of Ni/AC (5.1 h −1 ). In case of CH of lignin, Ni-Ru/AC gave better total liquid yield and higher relative content of main aromatic monomers . The enhancement in the overall hydrogenolysis activity of reactants over bimetallic Ni-Ru/AC is related to the synergistic effect of Ni and Ru. Various characterization methods (XRD, XPS , TEM-EDS, SEM-EDX and BET) are performed to elucidate the formation of synergistic effect. This synergistic effect could originate from the generation of additional surface active sites, small size of metal particles and high dispersion of metal particles.
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TOXICOLOGICAL AND ENVIRONMENTAL CHEMISTRY
·
2019
·
IF 0.971
Ronghui Yuan,Fang Huang,Jun Jiang,Jinfei Huang,Chang Su
Simulated with small environmental chambers, the emission characteristics of total volatile organic compounds from plastic runway surfaces were investigated by thermal desorption–gas chromatography–mass spectrometry. This quantitative approach was validated using a dynamic recovery experiment, and the variation of emission factors from mixed-type plastic surfaces was determined. Also, the photodegradation of volatile organic compounds in chambers was introduced to decrease the background interference.
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