CHEMICAL ENGINEERING JOURNAL
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2019
·
IF 8.355
Yan Cui,Lei Qin,Weiwei Kang,Jinghong Ma,Yongzhen Yang,Xuguang Liu
Magnetic carbon nanospheres (MCNSs) dotting with Fe 3 O 4 nanoparticles were synthesized by a simple solvothermal method. Furtherly, KOH activation and HNO 3 acidification of MCNSs were carried out to tune surface structure and property of MCNSs for the sake of adsorption improvement. The results show that both MCNSs and modified MCNSs (MCNSs-KH) have magnetic properties, and can be used as adsorbents for rapid separation and reutilization towards quinoline in coking wastewater. After KOH activation and HNO 3 acidification, the saturated adsorption capacity of MCNSs-KH is improved to 297.21 mg g −1 , much better than that of MCNSs (99.43 mg g −1 ). According to BET and NH 3 -TPD characterizations, KOH activation introduced a large number of pore structures, which significantly increased the specific surface area of MCNSs; HNO 3 acidification further increased the surface acidity of MCNSs, especially C O functional group, which promoted the acid–base interaction with weakly basic quinoline. From the results of adsorption kinetics, isotherm and thermodynamics, the spontaneous and exothermic adsorption process conformed to pseudo-second-order and Langmuir–Freundlich models better.
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CHEMICAL ENGINEERING JOURNAL
·
2019
·
IF 8.355
Mengqi Zheng,Chunyan Xu,Dan Zhong,Yuxing Han,Zhengwen Zhang,Hao Zhu,Hongjun Han
In current study, the degradation of aromatic cyclic organics (ACOs) of coal pyrolysis wastewater (CPW) by lignite activated coke-active sludge (LAC-AS) process was investigated through the insight into synergistic effect of LAC and microbial community. As a contrast, the study on single AS process revealed that high phenols (>200 mg·L −1 ) exerted irreversible toxicity by eliminating biomass. Meanwhile, quinoline and naphthalene exhibited joint inhibition with phenols on bio-community. Absence of functional genus and insufficient interspecific cooperation caused interrupted biological reaction, leading to degenerated ecosystem and vicious circle. However, LAC-AS performed synergistic degradation of ACOs, leading to developed ecosystems and benign substance metabolisms. Specifically, LAC alleviated toxicity on suspended AS by ACOs adsorption, and the facultative bacteria enriched by LAC exerted synergistic degradation in biochemical processes. Firstly, the bacteria on biofilm facilitated direct interspecies electron transfer for ring-cleavage reaction, and electroactive bacteria ( Cloacibacterium , Hydrogenophaga and Stenotrophomonas ) were critical for the process. Secondly, suspended AS further degraded ring-cleavage products, achieving the interspecific cooperation with biofilm. The synergistic nitrogen metabolism by different paths also contributed to the benign metabolic circulation.
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GREEN CHEMISTRY
·
2019
·Vol. 21
·期 17
·4732-4747
·
IF 9.405
Shenghui Zhou,Fanglin Dai,Chao Dang,Ming Wang,Detao Liu,Fachuang Lu,Haisong Qi
Exploring both high-performance catalytic materials from non-edible lignocellulosic biomass and selective hydrodeoxygenation of bioderived molecules will enable value-added utilization of renewable feedstocks to replace rapidly diminishing fossil resources. Herein, we developed a scale-up and sustainable method to fabricate gram-quantities of highly dispersed cobalt nanocatalysts sheathed in multilayered N-doped graphene (Co@NG) by using a biomacromolecule carboxymethyl cellulose (CMC) as a raw material. The ionic gelation of CMC, urea and Co2+ ions leads to uniform dispersion and chelation of different species, consequently resulting in the formation of highly distributed Co nanoparticles (NPs) (10.91 nm) with N-enriched graphene shells in the solid-state thermolysis process. The usage of urea as a non-corrosive activation agent can introduce a porous belt-like nanostructure and abundant doped nitrogen. Among all the prepared catalysts in this work, the optimized Co@NG-6 with the largest specific surface area (627 m2 g−1), the most and strongest basic sites, and the highest proportion of pyridinic-N (37.6%) and mesopores exhibited excellent catalytic activity (99% yield of 2-methoxy-p-cresol) for base-free transfer hydrodeoxygenation (THD) of vanillin using bioderived formic acid (FA) as a H source at 160 °C for 6 h. The poisoning tests and electron paramagnetic resonance (EPR) spectra verified that the strong interaction between N atoms and encapsulated Co NPs provided synergistic effects, which were essential for the outstanding catalytic performance of Co@NG-6. The deuterium kinetic isotope effect study clearly demonstrated that the formation of Co-H−via β-hydride elimination and protonation was the rate-determining step, and protic N–H+ and hydridic Co-H− were considered to be active intermediate species in the THD reaction. Furthermore, Co@NG-6 was highly stable for recycling owing to the graphene shells preventing Co NPs from corrosion and aggregation.
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JOURNAL OF PHARMACEUTICAL AND BIOMEDICAL ANALYSIS
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2019
·
IF 2.983
Xue-Mei Han,Yan-Jie Qin,Ying Zhu,Xin-Lin Zhang,Nan-Xi Wang,Ying Rang,Xue-Jia Zhai,Yong-Ning Lu
Sensitive and comprehensive measurement of systemic metabolites of tryptophan, phenylalanine and glutamate metabolism in biological samples is effective for understanding the pathogenesis of depression and other neurological diseases. Therefore, this study developed an underivatized liquid chromatography tandem mass spectrometry (LC–MS/MS) method for simultaneous monitoring the 3 components of glutamate metabolism in rat hippocampus and 11 components of tryptophan and phenylalanine metabolism in rat hippocampus, plasma and urine, and applied it to investigate their changes in rats induced by chronic unpredictable mild stress (CUMS). The investigated analytes are as follows: tryptophan, serotonin, 5-hydroxyindoleacetic acid, kynurenine, kynurenic acid, xanthurenic acid, 3-hydroxyanthranilic acid, quinolinic acid, phenylalanine, tyrosine, tyramine, glutamate, glutamine and gamma-aminobutyric acid. The method was verified to be sensitive and effective with satisfactory linearity, accuracies in the range of 78.2%–120.4%, and precisions less than 17.8% for all identified analytes. A series of significant changes in CUMS-induced rats can be detected: tryptophan, serotonin and tyrosine levels decreased and quinolinic acid increased in both hippocampus and plasma. In addition, the kynurenine/tryptophan ratios increased in hippocampus and plasma, the kynurenic acid/quinolinic acid ratios of plasma and urine were significantly reduced. These findings demonstrated that the CUMS procedure could lead to the central and peripheral imbalances of tryptophan and phenylalanine metabolism. In conclusion, a LC–MS/MS method for simultaneous measurement of several neurotransmitters in rat hippocampus, plasma and urine was developed and successfully applied to investigation of the central and peripheral changes in CUMS-induced rats. The method would be expected to provide applicability to the study of the mechanisms of depression and other related diseases associated with these neurotransmitters.
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PubMed
高影响因子
GREEN CHEMISTRY
·
2018
·Vol. 20
·期 13
·3112-3120
·
IF 8.586
Zhiheng Li,Dong Liu,Zhuowu Men,Linhua Song,Yijun Lv,PingPing Wu,Bin Lou,Yadong Zhang,Nan Shi,Qingtai Chen
Tremendous attention has been paid to removal of N-/S-containing compounds from liquid fuel due to the necessity of reducing NOx and SOx emissions. In this work, the compatibility index (CI or PCI) was developed as a new criterion to evaluate the removal efficiency (Re) of quinoline, carbazole and dibenzothiophene (DBT) in deep eutectic solvents (DESs). For alkaline quinoline, acid–base extraction was pronounced, and ChCl/mandelic acid was the optimal extractant to achieve a removal efficiency of 99.2 wt% (CI = 0.37). For near-neutral carbazole and DBT, polarity compatible extraction was the predominant mechanism. The highest Re value of 94.9 wt% for carbazole removal was obtained in the ChCl/mandelic acid extractant (PCI = −0.044). DBT was difficult to remove directly because of its low molecular polarity. After adding H2O2, the desulfurization efficiency was found to increase to 99.1 wt% in the ChCl/p-toluenesulfonic acid extractant (PCI = 0.014). Furthermore, experiments with real diesel confirmed that the highest desulfurization and denitrification efficiency was 67.7 wt% and 63.7 wt%, respectively, in ChCl/p-toluenesulfonic acid. The compatibility index developed in this study has the potential to simplify the filtration operation of extractants and to intensify the removal efficiency of N-/S-containing compounds in the category of “green extraction”.
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ENVIRONMENTAL TECHNOLOGY
·
2018
·
IF 1.666
Hanjiang Xu,Xiaoping Zhang,Yudong Zhang
The biochar produced by pyrolysis at 600°C from powdered mango bark impregnated with iron, namely Fe2O3/biochar, was recognized as a multifunctional material for environmental applications. This work aims at using the above material for the removal of pyridine and quinoline from aqueous solutions. The physico-chemical properties of synthesized biochars were studied systematically with several commonly used material characterization methods including scanning electron microscope (SEM), energy dispersive spectroscopy (EDS), X-ray diffraction (XRD) and Fourier transform infrared spectrometer (FTIR). Structural and morphological analyses of the biochars showed that Fe2O3 particles were nanosized and distributed evenly on the surface of biochar, and thus exhibited great adsorption capacity for the removal of pyridine and quinoline. In addition, the results suggested that the main magnetic phase is maghemite (Fe2O3). The modified biochar showed high removal capacity (99%) for quinoline, but the removal capacity of pyridine was only 73%. The pH experiment in this passage indicated that both pyridine and quinoline reached a maximum adsorption amount at pH near 9.0. Adsorption kinetics suggested that the pseudo-second-order was well fitting the experiment data. The equilibrium study showed that the Langmuir model can adequately describe the adsorption process for pyridine and quinoline. The main mechanism of pyridine and quinoline removal was possibly electrostatic interactions and π–π interactions between the modified biochar and the adsorbate.
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高影响因子
SCIENCE OF THE TOTAL ENVIRONMENT
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2018
·
IF 4.61
Zaiming Chen,Wenjie Ji
The adsorptive performance of carbonaceous materials (CMs) for the removal and sequestration of ionizable organic contaminants (IOCs) is heavily dependent on the pH-controlled speciation of the objective chemicals. To date, there is no effective method for measuring the sorption of IOC species at a solution pH near the IOC p K a , which is usually of environmental relevance and essential for validating sorption models. In this study, a unique “pH dynamics method” was developed. The method relates the uptake of the IOC species with the solution pH changes during sorption on the basis of the proton mass balance in the adsorptive process. The effectiveness of the method to quantify the sorption of IOC species at a pH near the p K a was validated by determining the extents and mechanisms of the pH change in a series of sorption systems employing graphite, biochar, carbon nanotube and activated charcoal as representative CMs, and 4-methylbenzoic acid, 2,4,6-trichlorophenol, 4-methylaniline and quinoline as model IOCs. Moreover, with the derived species uptake using the pH dynamics method, the effectiveness of already-reported speciation models for predicting species sorption at a pH around the p K a was verified for the first time. It was shown that the speciation models, including the linear speciation model and nonlinear speciation model, were convincing for estimating the sorption of individual species at the pH around the chemical p K a when the collected uptake of individual species could be reliably predicted. This research advances the application of pH dynamics for quantifying the uptake of individual species of IOCs and enhances the understanding of the speciation models and carbonaceous materials in managing risks of IOCs.
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高影响因子
DRUG METABOLISM AND DISPOSITION
·
2018
·Vol. 46
·期 4
·442-450
·
IF 3.64
Huimin Zhao,Siyuan Li,Zixin Yang,Ying Peng,Xiaohui Chen,Jiang Zheng
Erlotinib (ELT), a tyrosine kinase inhibitor, is widely used for the treatment of nonsmall cell lung cancer in clinic. Unfortunately, severe drug-induced liver injury and other adverse effects occurred during the treatment. Meanwhile, ELT has been reported to be a mechanism-based inactivator of cytochrome P450(CYPs) 3A4 and 3A5. The objectives of this study were to identify ketene intermediate of ELT and investigate the association of the acetylenic bioactivation with the enzyme inactivation caused by ELT. A ketene intermediate was detected in human microsomal incubations of ELT, using 4-bromobenzylamine as a trapping agent. CYPs 3A4 and 3A5 mainly contributed to the bioactivation of ELT. Microsomal incubation study showed that the ketene intermediate covalently modified the enzyme protein at lysine residues and destroyed the structure of heme. The vinyl and ethyl analogs of ELT showed minor enzyme inhibitory effect (less than 20%), whereas ELT inactivated more than 60% of the enzyme. The present study provided a novel bioactivation pathway of ELT and facilitated the understanding of the mechanisms of ELT-induced mechanism-based enzyme inactivation and liver injury.
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CHEMICAL ENGINEERING JOURNAL
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2015
·
IF 4.321
Jiajun Gao,Yafen Dai,Wenyan Ma,Huihui Xu,Chunxi Li
Separation of phenolic compounds from coal tar oil has good commercial value. In this paper, we tried to use the H-bonding or Lewis acid–base interaction to chemically adsorb phenolic compounds that were both Brønsted acid and Lewis base. Hexamethylenetetramine (HMT), 1,2,4-triazole, and AlCl 3 were selected as sorbents, and their adsorptive behavior were studied experimentally and theoretically. These sorbents can adsorb phenol from n -hexane oil. HMT showed the amazing phenol adsorbance ( Q e,max > 3500 mg/g), non-corrosiveness, stable physical state, good recycling, and oil-insoluble merit. In contrast, AlCl 3 was unrecoverable and triazole was partially oil-soluble, and thus they were not as good as HMT. Further, naphthalene or benzothiophene hardly hinders phenol adsorption on HMT ( Q e,max > 3400 mg/g in 5 wt% benzothiophene or naphthalene oil); whereas, quinoline interfered with the adsorption ( Q e,max > 970 mg/g in 5 wt% quinoline oil). Therefore, HMT might be an excellent sorbent for phenol, showing the best capacity heretofore.
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JOURNAL OF APPLIED POLYMER SCIENCE
·
2014
·Vol. 132
·期 15
·
IF 1.64
Wenming Yang,Pengfei Ma,Ting Fan,Zhiping Zhou,Hong Liu,Wanzhen Xu
In this study, we examined the rational preparation of molecularly imprinted polymers (MIPs) for the selective removal of quinoline from octane. Before the preparation, density functional theory, as one of the methods of quantum chemical calculation, was used for the simulation of a quinoline-imprinted preassembly system. Methacrylic acid turned out to be the more suitable monomer for quinoline compared with acrylamide, and different template–monomer ratios, including 1:1, 1:2, and 1:3, were studied and are discussed. On the basis of the result of molecular simulation, quinoline-imprinted polymers were prepared with a combination of surface imprinting and living polymerization. The prepared quinoline–MIPs were characterized and used as selective adsorbents for batch-mode binding experiments. The fitting result of the adsorption data indicates that the adsorption kinetics and adsorption isotherms of the quinoline-imprinted polymers fit well a pseudo-second-order kinetics model and the Freundlich model, respectively. A selective recognition ability was demonstrated by equilibrium binding analysis. This study will provide needful guidance and a theoretical basis for the preparation of imprinted materials in the field of industrial denitrification. © 2014 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2015 , 132 , 41730.
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NEW JOURNAL OF CHEMISTRY
·
2013
·Vol. 37
·期 6
·1768-1775
·
IF 2.966
Yanfang Song,Dandan Zhou,Yonggang Wang,Congxiao Wang,Yongyao Xia
Nitrogen-containing mesoporous carbons (NMCs) were prepared from quinoline-polymerized pitch using mesoporous silica as a template. The effects of the ratio of quinoline-polymerized pitch/silica template and carbonization temperature on the capacitive performance of NMCs were extensively studied. The NMC synthesized at a pitch–silica template ratio of 1.5 and carbonized at 750 °C has a high surface area of 1000 m2 g−1 and a high nitrogen content of 5.43%. The unique pore structure and nitrogen functionalities enable the carbon to exhibit a high capacitance of up to 290 F g−1 in 1 mol L−1 H2SO4 aqueous electrolytes.
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RSC Advances
·
2013
·Vol. 4
·期 2
·605-616
·
IF 2.562
Lukuan Liu,Yang Cao,Pengfei Ma,Chunxiao Qiu,Wanzhen Xu,Hong Liu,Weihong Huang
Novel magnetic imprinted polymers are designed by molecular simulation from a comprehensive perspective and prepared rationally by combining the modified surface imprinting technique with the improved atom transfer radical polymerization. The simulation results show that interaction intensity between indole and monomers are simultaneously affected by complex conformation, charge transfer and binding energy. The optimal monomer for the removal of indole is AM and the best ratio is 1 : 4 in the studied three monomers. To verify the reliability and accuracy of the simulation results, three kinds of novel magnetic imprinted polymers are prepared with different monomers. The experimental results show that molecular simulation is reliable in processing the pre-assembled complexes of molecularly imprinted polymers (MIPs). The MIPs using AM as monomer display the highest selectivity (2.561) and bonding percentage (31.062%). Structural superiority of the optimal adsorbent is reflected by using several characterization methods. A series of static adsorption tests such as kinetic, isotherm and selectivity are used to analyse the adsorption performance. The test results show that the novel adsorbents conform to the Elovich kinetic equation and follow the Langmuir isotherm model. Meanwhile, they display higher selectivity towards indole than towards other analogues. The novel adsorbents have potential application value in the denitrogenation field.
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