ANALYTICAL CHEMISTRY
·
2013
·
IF 5.695
Yang Tang,Jie-Mei Chu,Wei Huang,Jun Xiong,Xi-Wen Xing,Xiang Zhou,Yu-Qi Feng,Bi-Feng Yuan
5-Methylcytosine (5-mC), an important epigenetic modification involved in development, can be converted enzymatically to 5-hydroxymethylcytosine (5-hmC). 5-hmC is considered an intermediate of active DNA cytosine demethylation and makes itself serve as an epigenetic mark. 5-hmC content in most mammalian cells is low and the quantification of 5-hmC by liquid chromatography–mass spectrometry (LC–MS) frequently suffers from ion suppression by the presence of unmodified nucleosides. To circumvent this problem, we developed a method to selectively transfer a glucosyl group to the hydroxymethyl moiety of 5-hmC and form a more hydrophilic residue (β-glucosyl-5-hydroxymethyl-2′-deoxycytidine, 5-gmdC) by using T4 β-glucosyltransferase. The more hydrophilic 5-gmdC can be selectively enriched by using NH2-silica via hydrophilic interaction prior to liquid chromatography–tandem mass spectrometry (LC–MS/MS) analysis, which eliminates the ion suppression and significantly improves the detection sensitivity and accuracy. Using this method, we successfully quantified 5-hmC content in genomic DNA of three human cell lines and seven yeast strains. To the best of our knowledge, this is the first report about the existence of 5-hmC in the model organism of yeast. In addition, the contents of 5-hmC in two yeast strains of Schizosaccharomyces pombe are even higher than those of 5-mC, indicating that 5-hmC may play important roles on the physiological functions of yeast.
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Materials Chemistry Frontiers
·
2021
·Vol. 5
·期 18
·7032-7040
·
IF 6.482
Xiaojia Jiang,Mingsong Zang,Fei Li,Chunxi Hou,Quan Luo,Jiayun Xu,Junqiu Liu
Recently, biological nanopore-based techniques have attracted more and more attention in the field of single-molecule detection because they allow real-time, sensitive, high-throughput analysis. Herein, we report an engineered biological nanopore sensor by introducing a macrocyclic host molecule carboxylatopillar[5]arene (CP[5]A) that acts as an aptamer into the lumen of a mutant (E111R/K147R)7 αHL nanopore for detecting highly toxic paraquat (PQ) via host–guest interactions at the single-molecule level. By taking advantage of introducing positively charged arginine (Arg) into the lumen of the αHL nanopore, our engineered nanopore sensor exhibits higher stability. More importantly, this nanopore sensor shows high sensitivity, and the limit of detection (LOD) for PQ can reach a nanomolar level of 0.37 ppb. The CP[5]A-based nanopore sensing strategy developed in this work may bring inspiration for single-molecule detection and hold great potential in public health applications.
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Frontiers in Nutrition
·
2022
·
IF 6.59
Ma Yingjie,Long You,Li Feng,Zhang Yan,Gan Bei,Yu Qiang,Xie Jianhua,Chen Yi
In the “glucose-asparagine-linoleic acid” ternary system, a kinetic model approach was used to explore formation and elimination law of target hazards, including acrylamide (AA) and 5-hydroxymethylfurfural (5-HMF), and their related precursors and intermediate products. The results showed that the elimination of glucose and asparagine and the formation of fructose (generated from glucose isomerization), 3-deoxyglucosone (3-DG), methylglyoxal (MGO), and glyoxal (GO), AA and 5-HMF followed first-order reaction kinetics with high fit coefficients (R2 > 0.9). In addition, the kinetic reaction rate constants increased as the increasing temperature, and all models followed the Arrhenius law. Results of statistical correlations analysis suggested that at lower temperature, the generic amino acid route and the specific amino acid route may paly crucial roles for the formation of AA and 5-HMF, while at high temperature a linoleic acid pathway may be predominantly involved.
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RSC Advances
·
2018
·Vol. 8
·期 57
·32423-32433
·
IF 2.936
Guo Qiu,Xincheng Wang,Chongpin Huang,Yingxia Li,Biaohua Chen
The efficient conversion of carbohydrates to 5-hydroxymethylfurfural (5-HMF) under mild conditions represents a very attractive and promising method of producing important building blocks. In this work, niobium phosphotungstates, with Nb/P molar ratios of 0.6, 1.0, 2.0 and 4.0 (NbPW-06, NbPW-1, NbPW-2, and NbPW-4, respectively) have been prepared by a facile, one-pot, alcohol-mediated thermal process and used for the direct conversion of fructose to 5-HMF. By adding a certain amount of Nb, the surface of the catalyst became enriched in P, and this enrichment was associated with the presence of surface P–OH groups that offered Brønsted acid sites that can activate superficial hydrogen species to facilitate 5-HMF generation. Pyridine-FTIR confirmed the presence of Brønsted and Lewis acid sites, which might play important roles in the dehydration of fructose to 5-HMF. Furthermore, polar aprotic solvents were well-suited for the conversion, and higher yields of 5-HMF were obtained in polar aprotic solvents than in nonpolar solvents. A 5-HMF yield of 96.7% with complete fructose consumption was obtained over NbPW-06 in DMSO at 80 °C after 90 min. In addition, NbPW-06 could be recycled several times without a significant decrease in the catalytic activity. A catalytic mechanism for this reaction was proposed. Moreover, this catalytic system can also be utilized for the dehydration of sucrose and inulin to 5-HMF in satisfactory yields. This study establishes an important platform for the further design of Nb-containing catalysts for the production of 5-HMF from carbohydrates under mild conditions.
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JOURNAL OF MOLECULAR LIQUIDS
·
2019
·
IF 4.561
Zhisheng Zhou,Xing Hu,Xinyue Hong,Jie Zheng,Xia Liu,Deming Gong,Guowen Zhang
5−Hydroxymethyl−2−furaldehyde (5-HMF) is a kind of by-product produced in food processing, which may cause latent hazard to human health. Here, the interaction of 5-HMF with human serum albumin (HSA) was studied by multi-spectroscopic methods, multivariate curve resolution-alternating least squares (MCR−ALS) and molecular docking . The formation of 5-HMF−HSA complex was confirmed by MCR−ALS. The fluorescence quenching mechanism of HSA by 5-HMF was static , and their binding constant was 5.25 × 10 4 L mol −1 at 298 K, the binding site of 5-HMF was located in subdomain IIA of HSA. The main forces of the interaction were hydrogen bonds and van der Waals forces . The molecular docking showed that three hydrogen bonds were formed between –CH 2 OH of 5-HMF and Lys106, Pro147 and Gln29 of HSA. The synchronous fluorescence, three-dimensional fluorescence and circular dichroism spectra showed that 5-HMF induced a structural shrinkage of HSA. Fluorescence phase diagram ascertained that the HSA conformational change was in accordance with all-or-none model. Moreover, the presence of the food nutrients (vitamin C, chlorogenic acid and phloretin) weakened the binding of 5-HMF with HSA. This study is helpful to understand the hazard mechanism of 5-HMF to human body and provides new strategies to reduce the hazard of 5-HMF.
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PHARMACEUTICAL RESEARCH
·
2021
·Vol. 38
·期 4
·693-706
·
IF 4.2
Xu Wenhao,Su Wenjing,Xue Zhencheng,Pu Faxiang,Xie Zhangfu,Jin Kongliang,Polyakov Nikolay E.,Dushkin Alexander V.,Su Weike
Purpose This study aims to overcome the challenges of the current oral targeted drug delivery system, such as the complex preparation process, poor biocompatibility, and delayed drug release. Methods Here, a non-covalent polymer hydrogel was prepared using the mechanochemical method, and the solid phase loading of 5-amino salicylic acid (5-ASA) was realized. Results The results obtained from the thermodynamics study, particle size analysis, and electron microscopy show that chitosan (CS) and sodium alginate (SA) form a pH-sensitive hydrogel under the mechanochemical force and also maintain good stability in aqueous solution. Fluorescent tracers study showed that the pH-sensitive hydrogel could achieve the targeted drug release in the colon and the retention time was over 12 h. Next, in vivo efficacy studies, change in mice body weight, DAI (disease activity index) score, thymus, and spleen index, and the diseased state of the mice colon revealed that the pH-sensitive hydrogel is an improved drug delivery system over 5-ASA API commercial preparations as observed in the efficacy and toxicological studies. Conclusion This method uses an innovative preparation technology that without the need of cross-linking agent to produce an efficient colon-targeted drug delivery system for the treatment of ulcerative colitis.
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APPLIED CATALYSIS A-GENERAL
·
2022
·
IF 5.723
Lin-Cong He,Xu-Fang Wang,Chu-Feng Liu,Bei Li,Meng-Fei Luo,Jian Chen
An efficient MnO x /CeO 2 /ZSM-5 catalyst was developed for selective oxidation of diethylamine (DEA) with high N 2 selectivity in a wide temperature window ( Δ T = 140 °C), owing to the existence of oxidation and selective catalytic reduction (SCR) active sites. MnO x species prefer to locate on the surface of CeO 2 compared to ZSM-5, and the presence of CeO 2 is beneficial to form more Mn 4+ species, the active sites for oxidation reaction. The mechanistic investigation suggests that internal SCR of NO x generated from the over-oxidized DEA is the crucial pathway for N 2 generation. The high SCR activity of the MnO x /CeO 2 /ZSM-5 catalyst in oxidation conditions is mainly attributed to the synergistic catalysis of Mn 4+ species and acid sites of ZSM-5, the active sites for SCR reaction. Thus, it has been clearly clarified that addition of CeO 2 and its addition sequence could modulate the surface active sites of MnO x /ZSM-5 catalyst for the selective catalytic oxidation of DEA.
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RUSSIAN JOURNAL OF GENERAL CHEMISTRY
·
2021
·Vol. 90
·期 12
·2376-2380
·
IF 0.868
Abbas N.,Shabir G.,Saeed A.,Tirmizi S. A.,Echeverría G. A.,Piro O. E.,Erben M. F.
Abstract The present study is devoted to the synthesis of 4-chloro-2-{[5-(diethylamino)-2-hydroxybenzylidene]amino}phenol and its transition metal complexes. Synthesis of the ligand has been achieved by the condensation reaction of N,N -diethylsalicylaldehyde with 4-chloro-2-aminophenol in acidic medium. Metals complexes of the ligand with different transition metal ions [M 2+ = Mn(II), Fe(II), Co(II), Ni(II), Cu(II), Zn(II), Cd(II), Hg(II), and Pd(II)] have been accumulated in alcoholic media and characterized by spectroscopic methods. UV-Vis analysis of the complexes indicates the ligand coordination to the metal ions via both OH groups and the azomethine nitrogen atom, acting as a tridentate ligand. Anticancer tests of selected complexes demonstrate moderate in vitro activity of Cu(II) complex against HeLa cell line.
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CATALYSIS LETTERS
·
2015
·Vol. 145
·期 4
·1080-1088
·
IF 2.307
Liu Wentao,Wang Yanfang,Li Wei,Yang Yan,Wang Ningning,Song Zhanxin,Xia Xiao-Feng,Wang Haijun
Abstract A variety of polyethylene glycol-400-functionalized dicationic acidic ionic liquids (ILs) (PEG 400 -DAILs) were synthesized and tested in the dehydration of fructose. Among these catalysts, hydrogen sulfate anion-based ILs showed the higher catalytic performance in the conversion of fructose. The highest HMF yield of 96.5 % with 100 % consumption of fructose were obtained after 60 min at 110 °C. The effects of catalyst concentration, reaction time, reaction temperature, and solvents were systematically investigated. In addition, the generality of the catalysts was examined by processing inulin and sucrose to HMF with yield of 71.9 and 52.1 % under certain conditions, respectively. PEG 400 -DAILs possess modified physicochemical properties such as low viscosity, strong hydrophilicity and hydrogen bonding with sugars so as to improve activity for the dehydration of fructose into HMF. The used IL catalyst could be separated and recycled repeatedly without significant loss of catalytic activity. The research emphasizes preparation of the novel catalysts combining polymers with functionalized ILs for conversion of renewable biomass. Graphical abstract
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Journal of the Taiwan Institute of Chemical Engineers
·
2019
·
IF 3.834
Yunchao Feng,Miao Zuo,Ting Wang,Wenlong Jia,Xiaoyu Zhao,Xianhai Zeng,Yong Sun,Xing Tang,Tingzhou Lei,Lu Lin
Production of 5-hydroxymethylfurfural (HMF) from glucose with high yield remains a big challenge. Thereinto, assembling catalysts with outstanding performance is the bottleneck at the current stage. In this study, effective catalysts were synthesized by loading SO 4 2− /ZrO 2 (SZ) on a series of H + zeolites to investigate the catalytic dehydration of glucose into HMF. Among all the catalysts applied, 2-SZ-HM-550 (HZSM-5 with Si/Al molar ratios of 80∼150, calcined at 550 °C) gave the yields of HMF 41.32%, 61.14%, 54.67% and 40.71% in 4 applied reaction systems, respectively. Moreover, HMF with desirable yield was obtained while other carbohydrates were dehydrated catalyzed by 2-SZ-HM-550, such as fructose, sucrose, inulin and starch.
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SUPRAMOLECULAR CHEMISTRY
·
2011
·
IF 1.94
Jing Cao,Jun Xiang Feng,Yong Xiang Wu,Xue Qun Pei,Jiao Jiao Yan,Yang Liu,Wen Jie Qin,Xiao Bin Zhang
A novel 15-aza-5-crown ether linked to styryl chemosensory 13-(4-((9H-fluoren-9-ylidene)methyl)-2-nitrophenyl)-1,4,7,10-tetraoxa-13-azacyclopentadecane was designed and synthesised, it would not occur during photoisomerisation under radiation of light but shows special capability of selectively recognising for Sr2+.
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ACS Sustainable Chemistry & Engineering
·
2021
·
IF 8.198
Zhijian Li,Changhui Zhu,Haiyong Wang,Yuan Liang,Haosheng Xin,Song Li,Xiaohong Hu,Chenguang Wang,Qi Zhang,Qiying Liu,Longlong Ma
For the biomass catalytic valorization in the presence of a H2 atmosphere, large amounts of H2O and H2 are necessary to improve the processing efficiency, which resulted in the waste of such generous inputs. As a model reaction, the traditional hydrodeoxygenation of 5-hydroxymethylfurfural (5-HMF) selectively produces 2,5-dimethylfuran (2,5-DMF) under high pressure H2. Meanwhile, the water-gas shift reaction (WGSR) can counteract the harmful CO by simultaneously producing H2 from H2O. The hydrogenolysis of 5-HMF to 2,5-DMF produces H2O because of the hydroxyl group removal. Therefore, adding a trace amount of H2O to initiate 5-HMF hydrodeoxygenation coupled with WGSR to achieve H2O recycling in the reaction process is of great significance but extremely challenging. Herein, we reported a new process for the selective hydrodeoxygenation of 5-HMF to 2,5-DMF coupled with WGSR using a single catalyst, Au/ZrO2. A detailed study showed that the hydrogen species produced in situ by WGSR was used for 5-HMF hydrodeoxygenation to obtain 78.5% of 2,5-DMF yield. The H/H2O cycle in the coupling reactions exhibited a H2 utilization efficiency of 88.2%. Without using external H2, this work provided a new method for 5-HMF hydrodeoxygenation to 2,5-DMF triggered by WGSR and also showed the potential for application in H2O-saving conversion of cellulosic biomass with C–OH or C═O groups to value-added chemicals and fuels.
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