NEW JOURNAL OF CHEMISTRY
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2017
·Vol. 41
·期 15
·7133-7141
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IF 3.269
Yue Hu,Wei Huang,Yukui Tong,Qinfei Xia,Miaomiao Tian
Boronate-affinity hollow molecularly imprinted polymers (h-MIPs) were prepared and applied to the selective enrichment of four nucleosides in traditional Chinese medicine injection samples, followed by HPLC detection. The synthesis mechanism of the h-MIPs was studied. Due to a large amount of boronic acid groups were introduced by 3-aminophenylboronic acid (APBA) in the outermost polymer shell of the MIPs, which was of great importance for improving the enrichment efficiency of the nucleosides. Furthermore, owing to the hollow structure of the h-MIPs, more binding cavities were located on the inner and outer surfaces of the h-MIPs, which could facilitate the removal of template molecules from the polymers and the rebinding of the target molecules to the polymers. Under optimal conditions, the detection limits of the four nucleosides were in the range of 0.012–0.033 μg mL−1. At the different spiked levels, the recoveries of the nucleosides were in the range of 63.8–108.9%. The proposed method was successfully applied to determine four nucleosides in five injection samples. The boronate-affinity h-MIPs provided a promising selective enrichment platform for precise nucleoside analysis.
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NEW JOURNAL OF CHEMISTRY
·
2017
·Vol. 41
·期 17
·9230-9235
·
IF 3.269
Xin Shen,Lei Xu,Wanying Zhu,Bingzhi Li,Junli Hong,Xuemin Zhou
In this paper, a novel turn-on fluorescence aptasensor has been designed for adenosine detection based on fluorescence resonance energy transfer (FRET) from single-stranded DNA labeled carbon dots (ssDNA-CDs) to aptamer modified gold nanoparticles (aptamer-AuNPs). In the absence of adenosine, the fluorescence of ssDNA-CDs was quenched by aptamer-AuNPs via the formation of an aptamer–ssDNA duplex. The introduced adenosine competed to displace ssDNA-CDs by specifically binding to the aptamer, resulting in the recovery of the quenched fluorescence of ssDNA-CDs. Under optimized conditions, the increase in fluorescence intensity was proportional to the concentration of adenosine with a linear range of 10–500 nM and allowed a limit of detection as low as 4.2 nM. In addition, this method was successfully applied to adenosine determination in human serum samples with satisfactory results.
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JOURNAL OF SEPARATION SCIENCE
·
2016
·Vol. 39
·期 7
·1347-1356
·
IF 2.741
Ting Cheng,Shuqiang Zhu,Bin Zhu,Xiaoyan Liu,Haixia Zhang
The nucleoside or modified nucleoside level in biological fluids reflects the pathological or physiological state of the body. Boronate affinity absorbents are widely used to selectively extract nucleosides from complex samples. In this work, a novel functionalized absorbent was synthesized by attaching 4-mercaptophenylboronic acid to gold nanoparticles on modified attapulgite. The surface of the attapulgite was modified by poly(acryloyloxyethyltrimethyl ammonium chloride) by atom transfer radical polymerization, creating many polymer brushes on the surface. The resultant material exhibited superior binding capacity (30.83 mg/g) for adenosine and was able to capture cis -diol nucleosides from 1000-fold interferences. Finally, to demonstrate its potential for biomolecule extraction, this boronate affinity material was used to preconcentrate nucleosides from human urine and plasma.
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RSC Advances
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2016
·Vol. 6
·期 34
·28470-28476
·
IF 3.289
Li Gao,Chaozhan Wang,Yinmao Wei
In this work, polyethyleneimine-modified boronate affinity fibrous cotton with good selectivity and higher binding capacity for cis-diols was developed for in-pipette-tip solid-phase extraction (SPE). The introduction of polyethyleneimine for the modification of cotton fiber provided abundant binding sites for adsorption of cis-diols, resulting in higher binding capacities up to 300 μg g−1 for catechol, 450 μg g−1 for dopamine and 700 μg g−1 for adenosine, respectively. The adsorbent could still show recognition ability towards cis-diols even with a 1000-fold amount of interferences in the solution. Several extraction parameters were optimized, including adsorbent dose, pipette times, washing and elution solvents. Under optimal extraction conditions, the proposed in-pipette-tip SPE method coupled with reversed-phase liquid chromatography was successfully used to extract nucleosides in urine. The limit of detection was 3.5–4.7 ng mL−1 and the recoveries were in the range of 89–102% with relative standard deviations of less than 9.9%. In conclusion, combination of the specific adsorption performance of the prepared boronate affinity fibrous material and in-pipette-tip SPE provided a fast pretreatment method of trace cis-diols in complex real samples.
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TALANTA
·
2016
·
IF 4.035
Huihui Li,Ting Cheng,Shuxia Wang,Xinyue Zhu,Haixia Zhang
Boronate affinity materials have been widely used for selective capture of cis-diol-containing molecules, but most do not have sufficient extraction efficiency. We have prepared boronic acid-functionalized attapulgite, and then it was coated with imidazolium-based ionic liquid , 1-dodecyl-3-methylimidazolium bromide (C 12 mimBr), via physical self-assembly process. The extraction efficiency of the material increased dramatically after coated with C 12 mimBr, and its enrichment ratios for nucleosides increased by 9- to 282-fold. Besides, the C 12 mimBr-coated adsorbent did not lose selectivity and was able to capture cis-diols in the presence of a 100-fold excess of interferences. C 12 mimBr-coated material was applied to selective enrichment of nucleosides from human urine. The limits of detection and the limits of quantification were in the range of 0.06–0.46 ng mL −1 and 0.20–1.53 ng mL −1 , respectively. Reproducibility of the method was determined with relative standard deviations≤9.9%. The recoveries of the target nucleosides from spiked human urine were in the range of 87.8–109.6%. In our preception, self-assembly ionic liquid layer can serve as a promising alternative to improve the extraction efficiency of boronate affinity materials.
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JOURNAL OF CHROMATOGRAPHY A
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2017
·
IF 3.981
Chusheng Liu,Haibin Li,Qiqin Wang,Jacques Crommen,Haibo Zhou,Zhengjin Jiang
The quest for higher column efficiency is one of the major research areas in polymer-based monolithic column fabrication. In this research, two novel polymer-based HILIC monolithic columns with 400 μm I.D. × 800 μm O.D. were prepared based on the thermally initiated co-polymerization of N,N -dimethyl- N -(3-methacrylamidopropyl)- N -(3-sulfopropyl) ammonium betaine (SPP) and ethylene glycol dimethacrylate (EDMA) or N,N’ -methylenebisacrylamide (MBA). In order to obtain a satisfactory performance in terms of column permeability, mechanical stability, efficiency and selectivity, the polymerization parameters were systematically optimized. Column efficiencies as high as 142, 000 plates/m and 120, 000 plates/m were observed for the analysis of neutral compounds at 0.6 mm/s on the poly(SPP- co -MBA) and poly(SPP- co -EDMA) monoliths, respectively. Furthermore, the Van Deemter plots for thiourea on the two monoliths were compared with that on a commercial silica based ZIC-HILIC column (3.5 μm, 200 Å, 150 mm × 300 μm I.D.) using ACN/H 2 O (90/10, v/v) as the mobile phase at room temperature. It was noticeable that the Van Deemter curves for both monoliths, particularly the poly(SPP- co -MBA) monolith, are significantly flatter than that obtained for the ZIC-HILIC column, which indicates that in spite of their larger internal diameters, they yield better overall efficiency, with less peak dispersion, across a much wider range of usable linear velocities. A clearly better separation performance was also observed for nucleobases, nucleosides, nucleotides and small peptides on the poly(SPP- co -MBA) monolith compared to the ZIC-HILIC column. It is particularly worth mentioning that these 400 μm I.D. polymer-based HILIC monolithic columns exhibit enhanced mechanical strength owing to the thicker capillary wall of the fused-silica capillaries.
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TALANTA
·
2017
·
IF 4.162
Shuxia Wang,Huihui Li,Xiujuan Guan,Ting Cheng,Haixia Zhang
Boronic acid modified materials have been widely used to adsorb nucleosides , but their adsorption capacities require further improvement. Most cis -diol containing biomolecules are in very low abundance along with interfering components in real samples, and need to be enriched specially. In this study, we synthesize a kind of silica absorbent modified with boronic acid derivative, using amorphous silica as raw material and obtaining high adsorption capacity for adenosine. In addition, the adsorption equilibrium can be completed within 10 s and 1 min for the desorption. Finally, the material was successfully applied to enrich nucleosides from cells and the spiked recoveries were found between 82.21% and 118.9%. The results showed that the prepared adsorbent has potential to effectively enrich cis-diol substances from cell samples.
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ACS Applied Materials & Interfaces
·
2017
·
IF 7.504
Hao Liang,Feifei Lin,Zijie Zhang,Biwu Liu,Shuhui Jiang,Qipeng Yuan,Juewen Liu
Using nanomaterials to achieve functional enzyme mimics (nanozymes) is attractive for both applied and fundamental research. Laccases are multicopper oxidases highly important for biotechnology and environmental remediation. In this work, we report an exceptionally simple yet functional laccase mimic based on guanosine monophosphate (GMP) coordinated copper. It forms an amorphous metal–organic framework (MOF) material. The ratio of copper and GMP is 3:4 as determined by isothermal titration calorimetry. It has excellent laccase-like activity and converts a diverse range of phenol containing substrates such as hydroquinone, naphthol, catechol and epinephrine. Comparative work shows that the activity is originated from guanosine coordination instead of phosphate binding in GMP. Cu2+ is required and cannot be substituted by other metal ions. At the same mass concentration, the Cu/GMP nanozyme has a higher Vmax and similar Km compared to the protein laccase. To achieve the same catalytic efficiency, the cost of the Gu/GMP is ∼2400-fold lower than that of laccase. The Cu/GMP is much more stable at extreme pH, high salt, high temperature and for long-term storage. This is one of the first laccase-mimicking nanozymes, which will find important applications in analytical chemistry, environmental protection, and biotechnology.
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JOURNAL OF CHROMATOGRAPHY A
·
2017
·
IF 3.981
Chen Zhao,Yan Yang,Linfang Wei,Qinghua Guo,Hao Fang,Shaolin Chen,Qiang Hua
Yarrowia lipolytica is an oleaginous yeast with promise in producing terpenoids such as lycopene . Though methods for analyzing primary metabolic intermediates have been established, further work is needed to better analyze nucleotides and coenzymes . Here, we presented an optimized method for the separation of nucleotides and coenzymes in Y. lipolytica using the capillary electrophoresis. The separation of twelve metabolites including four coenzymes, five nucleotides and three nucleosides was achieved within 32 min using a voltage of 15 kV and 70 mM sodium carbonate/hydrogencarbonate buffer with 1.0% β -CD at pH 10. The results show that the concentrations of adenosine triphosphate and nicotinamide adenine dinucleotide phosphate changed significantly between lycopene producing strain and the control, indicating that these two metabolites may be closely related with lycopene production. The optimized method provides a useful approach for future metabolic analysis of fermentation process as well as industrial strain improvement.
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JOURNAL OF PHARMACEUTICAL AND BIOMEDICAL ANALYSIS
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2017
·
IF 3.255
Yang Huang,Tingting Zhang,Yumei Zhao,Haibo Zhou,Guangyun Tang,Marianne Fillet,Jacques Crommen,Zhengjin Jiang
Nucleobases, nucleosides and ginsenosides, which have a significant impact on the physiological activity of organisms, are reported to be the active components of ginseng, while they are less present in ginseng extracts. Few analytical methods have been developed so far to simultaneously analyze these three classes of compounds with different polarities present in ginseng extracts. In the present study, a simple and efficient analytical method was successfully developed for the simultaneous separation of 17 nucleobases, nucleosides and ginsenosides in ginseng extracts using supercritical fluid chromatography coupled with single quadrupole mass spectrometry (SFC-MS). The effect of various experimental factors on the separation performance, such as the column type, temperature and backpressure, the type of modifier and additive, and the concentration of make-up solvent were systematically investigated. Under the selected conditions, the developed method was successfully applied to the quality evaluation of 14 batches of ginseng extracts from different origins. The results obtained for the different batches indicate that this method could be employed for the quality assessment of ginseng extracts.
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BIOMACROMOLECULES
·
2025
·
IF 5.4
Huan Liu,Ronger Ai,Bizhi Liu,Li He
Diabetic wound healing remains a significant challenge due to complex pathological mechanisms, including prolonged inflammation, excessive reactive oxygen species (ROS) accumulation, angiogenesis dysfunction, and increased susceptibility to bacterial infection. In this study, we developed a dual ROS/glucose-responsive quercetin-loaded supramolecular hydrogel (GPQ hydrogel) for treating diabetic wounds. The hydrogel was fabricated by incorporating quercetin (QUE) into a guanosine–phenylboronic acid (GP) hydrogel network through dynamic borate ester bonds. Structural characterization revealed the formation of a typical G-quadruplex structure in the GPQ hydrogel. The dual responsiveness to ROS and glucose enabled the controlled release of QUE, effectively addressing the abnormal wound microenvironment in diabetes. In vitro studies demonstrated the excellent antibacterial, antioxidant, anti-inflammatory, and pro-angiogenic properties of the GPQ hydrogel. Furthermore, the in vivo diabetic wound healing study using a full-thickness wound model in streptozotocin-induced diabetic rats showed that the GPQ hydrogel significantly accelerated wound closure, enhanced re-epithelialization and collagen deposition, and promoted angiogenesis compared to the control and GP hydrogel groups. Immunofluorescence analysis confirmed the superior antioxidant and pro-angiogenic effects of the GPQ hydrogel in the wound microenvironment. This study presents a promising multifunctional biomaterial for effectively managing diabetic wounds.
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ANALYTICAL LETTERS
·
2017
·
IF 1.15
Xiuping He,Jiangtao Wang,Xiaoqi Mei
A multitemplate molecularly imprinted polymer was synthesized using fragments similar to gonyautoxins 1 and 4 including 2,4,6-triaminopyrimidine, 4-hydroxy-2-butanone, and imidazole as dummy templates by bulk polymerization. Scanning electron microscopy and infrared spectroscopy showed a porous structure and the formation of organic groups in the imprinting process of the polymer. One millilitre of 0.1 mol L−1 acetic acid and 1 mL of 95% methanol were the optimized washing and eluting solutions during the molecularly imprinted solid-phase extraction. The adsorption capacity of the multitemplate molecularly imprinted polymer was lower than for the monotemplate molecularly imprinted polymer prepared in a previous study in seawater in which Alexandrium tamarense and Alexandrium minutum were cultivated. This result may due to the inappropriate combination of the dummy template fragments in the synthesis resulting in the unfitness of the imprinting sites for gonyautoxins 1 and 4. In general, it is inappropriate to use fragments with the similar parts to the analyte as the dummy templates. However, this work indicated the optimal molecularly imprinted polymer for the selective extraction of gonyautoxins 1 and 4.
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