NEW JOURNAL OF CHEMISTRY
·
2021
·Vol. 46
·期 3
·1120-1126
·
IF 3.591
Wenwen Liu,Qing Kang,Pengcheng Wang,Feimeng Zhou
The ratiometric fluorescence immunoassay is known as a spectrofluorimetric variant for the sensitive and quantitative analyses of biomarkers. However, there are few comparative studies between it and the traditional, single-wavelength-based immunoassay. In this work, a ratiometric fluorescence immunoassay was designed via fluorescence resonance energy transfer (FRET) in a system comprising MnO2 nanosheets, o-phenylenediamine (OPD), and fluorescent carbon nanodots (FCNs). The MnO2 nanosheet oxidizes OPD, producing a fluorescence peak at 580 nm, while FCNs exhibit a fluorescence peak at 490 nm. Under the effect of FRET, the fluorescence at 580 nm increases significantly while the fluorescence at 490 nm is reduced. The FRET effect was confirmed by our fluorescence lifetime measurements. We optimized the experimental conditions that include solution pH, OPD concentration, and reaction time. By electrostatically coating the MnO2 nanosheets with antibody molecules and using the resultant materials as a detection probe, the ratiometric fluorescence sensing was extended to the detection of alpha fetoprotein (AFP) in human serum samples on a 96-well titer plate. Our ratiometric fluorescence immunoassay possesses a good dynamic range (from 0.14 to 130.43 pM). The detection limit was estimated to be 0.13 pM (0.009 ng mL−1), which is 7.6-fold lower than that of the single-wavelength-based immunoassay. The measurement results of serum samples from healthy and patient donors are highly comparable to those measured by chemiluminescence for the same donors, demonstrating the viability for serological assays of important cancer markers.
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JOURNAL OF MOLECULAR LIQUIDS
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2021
·
IF 6.165
Hang Li,Qing-Sheng Zhao,Sen-Lin Chang,Tan-Ran Chang,Ming-Hui Tan,Bing Zhao
Industrial hemp is an important economic crop. The ethanol extract of its leaf is also known as cannabidiol full-spectrum oil (CFSO) and has a lot of health benefits. But its applications in many fields are limited owing to the poor thermal stability and low aqueous solubility. In this study, 2, 6-di-O-methyl-β-cyclodextrin (DM-β-CD) was used to prepare inclusion complex (IC) of CFSO to enhance its thermal stability and water solubility. Phase solubility study indicated that CFSO formed ICs with DM-β-CD at a 1:1 stoichiometric ratio. The complexation rate of CFSO/DM-β-CD IC was 91.5%. The results of SEM, FT-IR, DSC, PXRD, NMR, and molecular docking revealed that the bioactive components of CFSO were embedded into DM-β-CD cavities. After complexation, the aqueous solubility of CFSO in CFSO/DM-β-CD IC was increased from 0.046 to 12.4 μg/mL. The DPPH and ABTS EC 50 values of CFSO/DM-β-CD IC were 130.5 and 12.0 μg/mL respectively, which indicated that the antioxidant ability of CFSO/DM-β-CD IC was stronger than that of CFSO. The MICs of CFSO/DM-β-CD IC were around 6.25–12.5 μg/mL for Escherichia coli and 12.5–25 μg/mL for Bacillus subtilis . The data showed that the antibacterial activity of CFSO was nearly not influenced by complexation. The thermal stability of CFSO was also improved after inclusion. The findings could promote the use of CFSO and the development of the industrial hemp industry.
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ACS Omega
·
2021
·
IF 3.512
Xu Chen,Xingyu Ouyang,Jiayi Li,Yi-Lei Zhao
Laccase–mediator systems (LMSs) have been intensively investigated in lignin degradation. Although only natural metabolites are available for fungal lignin degradation, mediator molecules from metabolites have received substantially less attention than artificial organic–synthetic compounds. It remains unclear which metabolites can accelerate laccase-catalyzed reactions and how those natural mediators influence lignin degradation. In this work, we evaluated Trametes versicolor laccase-catalyzed reaction kinetics on a lignin guaiacyl subunit model (guaiacylglycerol-β-guaiacyl ether, G-β-GE) in the presence of a group of lignin syringyl subunit molecules: syringaldehyde, acetosyringone, and methyl syringate. We then compare their performance to a well-known synthetic mediator ABTS, 2,2′-azino-bis(3-ethylbenzothiazoline-6-sulfonic acid). Time-resolved UPLC-TOF-MS revealed that the syringyl mediators were more effective in accelerating the β-O-4 cleavage and Cα-oxidation of G-β-GE than ABTS under laccase-catalysis, despite the syringyl compounds possessing slower individual oxidation rates. In addition, the product profile of polymerization was also promoted dramatically, compared to that of the ABTS/laccase system. The LMS kinetic modeling suggested that mediator–substrate aggregation played a critical role in the laccase–mediator system; in which, the lignin syringyl and guaiacyl subunits likely form a π–π stacking van der Waals complex that can be oxidized faster than the syringyl or guaiacyl monomers by themselves. This syringyl–guaiacyl aggregation hypothesis postulates that the weak interactions in lignin biopolymers are able to accelerate the laccase-catalyzed biodegradation.
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NEW JOURNAL OF CHEMISTRY
·
2021
·Vol. 45
·期 24
·10959-10970
·
IF 3.591
Sethupathi Shanmugasundaram,Hairus Abdullah,Noto Susanto Gultom,Hardy Shuwanto,Dong-Hau Kuo
Hydrogen is an inevitable energy source to replace fossil fuels in the future. Herein, we report Ni-doped ZnIn2(O,S)4/In(OH)3 heterojunction composites with different sulfur contents to support green hydrogen gas evolution. A simple one-step hydrothermal preparation process was carried out by simultaneously adding all chemical precursors during the synthesis of composites. The as-prepared composites were carefully characterized by XRD, FE-SEM, TEM, XPS, DRS, TPC, MS, EIS and CV techniques, which confirmed their performance in the hydrogen evolution reaction (HER) under visible-light illumination. With increasing sulfur content, XRD analysis indicated the gradual formation of Ni-doped ZnIn2(O,S)4 co-existing with the In(OH)3 phase. The highest hydrogen evolution rate of 2100 μmol g−1 h−1 under visible-light illumination was achieved in the presence of the Ni-doped ZnIn2(O,S)4/In(OH)3 composite. Its excellent photocatalytic performance is related to the good separation of photocarriers. XPS analysis suggests the formation of positively and negatively charged defects on catalyst surfaces which attract the photogenerated electrons and holes, respectively, thus leading to an extended photocarrier lifetime. Furthermore, the coupling effect with In(OH)3 provides a more positive conduction band (CB) relative to that of the Ni-doped ZnIn2(O,S)4 phase for facile electron transfer. A plausible HER mechanism based on the experimental data is proposed in this work.
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ANALYTICAL CHEMISTRY
·
2021
·
IF 6.986
Siyuan Kong,Quanqing Zhang,Lujie Yang,Yuanyu Huang,Mingqi Liu,Guoquan Yan,Huanhuan Zhao,Mengxi Wu,Xiangmin Zhang,Pengyuan Yang,Weiqian Cao
The heterogeneity and low abundance of protein glycosylation present challenging barriers to the analysis of intact glycopeptides, which is key to comprehensively understanding the role of glycosylation in an organism. Efficient and specific enrichment of intact glycopeptides could help greatly with this problem. Here, we propose a new enrichment strategy using a boronic acid (BA)-functionalized mesoporous graphene–silica composite (denoted as GO@mSiO2–GLYMO–APB) for isolating intact glycopeptides from complex biological samples. The merits of this composite, including high surface area and synergistic effect from size exclusion functionality of mesoporous material, hydrophilic interaction of silica, and the reversible covalent binding with BA, enable the effective and specific enrichment of both intact N- and O-glycopeptides. The results from the enrichment performance of the strategy evaluated by standard glycoproteins and the application to global N- and O-glycosylation analyses in human serum indicate the robustness and potential of the strategy for intact glycopeptide analysis.
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BIOCHEMICAL ENGINEERING JOURNAL
·
2020
·
IF 3.475
Hong-Yan Wang,Yu-Li Xie,Xin Shi,Hong-Ling Shi,Jian-He Xu,Cun-Duo Tang,Lun-Guang Yao,Yun-Chao Kan
Halogenated mandelate and its derivatives are important scaffolds in chemical industry. However, the natural D -mandelate dehydrogenase (DMDH) showed relatively low catalytic activity toward D -o-chloromandelic acid, which largely limits the efficiency of dehydrogenation processes. To improve catalytic activity of Lactobacillus brevis D -mandelate dehydrogenase ( Lb DMDH) toward halogenated substrate, a D -mandelate dehydrogenase mutant Lb DMDH N253S with higher catalytic activity toward D -o-chloromandelic acid was successfully obtained by directed evolution, which was about 29 times of Lb DMDH. In addition, the temperature optimum of Lb DMDH N253S is 50 °C, and closer to the optimal growth temperature for Escherichia coli , indicating that it may be more advantageous in whole cell catalysis using living cells as catalysts. Meanwhile, the K cat value toward D -o-chloromandelic acid of Lb DMDH N253S is 2.08 s −1 , which is significantly higher than the one (0.09 s −1 ) of Lb DMDH, indicating that Lb DMDH N253S displayed higher catalytic efficiency toward D -o-chloromandelic acid. Then, we preliminarily explained the molecular basis for its catalytic performance by in silico design methods. All of these results established a solid foundation for molecular modification of DMDHs and the other industrial enzymes.
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MICROCHIMICA ACTA
·
2020
·Vol. 187
·期 11
·1-11
·
IF 6.232
Zou Jiao,Lan Xi-Wen,Zhao Guo-Qing,Huang Zhao-Ning,Liu Yi-Ping,Yu Jin-Gang
A novel chiral sensing platform, 6-O-α-maltosyl-β-cyclodextrin (Mal-βCD)-based film, is proposed for selective electrochemical recognition of tyrosine ( Tyr ) enantiomers. Black phosphorus nanosheets (BP NSs) and Mal-βCD modified glassy carbon electrode (Mal-βCD/BP NSs/GCE) were prepared by a layer-to-layer drop-casting method, and the platform was easy to fabricate and facile to operate. It is proposed that the amino and hydroxyl groups of the Tyr enantiomers and the chiral hydroxyl groups of Mal-βCD selectively form intermolecular hydrogen bonds to dominate effective chiral recognition. Two linear equations of Ip (μA) = 11.40 C L-Tyr (mM) + 0.28 ( R 2 = 0.99147) and Ip (μA) = 7.96 C D-Tyr (mM) + 0.22 ( R 2 = 0.99583) in the concentration range 0.01–1.00 mM have been obtained. The limits of detection (S/N=3) for L- Tyr and D- Tyr were 4.81 and 6.89 µM, respectively. An interesting phenomenon was that the value of I L- Tyr /I D- Tyr (1.51) in this work was slightly higher than the value of I L- Trp /I D- Trp (1.49) reported in our previous study, where tryptophan ( Trp ) enantiomers were electrochemically recognized by Nafion (NF)-stabilized BPNSs-G2-β-CD composite. The two similar sensors fabricated by different methods showed different recognition ability toward either Tyr or Trp enantiomers, and the underlying mechanism was discussed in detail. More importantly, the proposed chiral sensor enables prediction of the percentages of D- Tyr in racemic Tyr mixtures. The chiral sensor may provide a novel approach for the fabrication of novel chiral platforms in the practical detection of L- or D- enantiomer in racemic Tyr mixtures. Graphical abstract
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Frontiers in Chemistry
·
2020
·
IF 3.693
Zhang Qianchun,Liang Junyi,Zhao Li,Wang Yan,Zheng Yuguo,Wu Yun,Jiang Li
A novel carbon quantum dots (CQDs) were successfully synthesized by one-step hydrothermal reaction using Rosa roxburghii as a biomass-based precursor. The CQDs have an average size of 2.5 nm and a narrow size distribution. They display strong blue fluorescence with a quantum yield of 24.8% and good biocompatibility. Notably, these CQDs were capable of detecting trace o-nitrophenol in surface water and sewage with high sensitivity and specificity. The linear range is 0.08–40 μmol/L, and the limit of detection is 15.2 nmol/L. Furthermore, this CQDs was successfully applied for o-nitrophenol analysis in river water and sewage samples. Additionally, Hep3B cells, a human hepatocellular carcinoma cell line, can be easily imaged with high resolution using the as-prepared CQDs as nanoprobes. These results reveal that the as-prepared CQDs have potential applications for detecting o-nitrophenol and cell imaging.
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CRYSTAL GROWTH & DESIGN
·
2020
·
IF 4.089
H. Liu,X. Yang,S. Cao,F. Yu,S. Long,J. Chen,M. Zhang,S. Parkin,T. Li,Z. Yang
A series of N-phenyl-2-hydroxynicotinanilides (PHNAs) have been synthesized, and their crystal structures have been investigated. The identity of these compounds is revealed to be the tautomer of PHNAs, i.e., 2-oxo-1,2-dihydropyridine-3-carboxylic acid phenylamides, compounds with both amide and lactam functionalities. Among these compounds, those with no or negligible steric hindrance take a near planar conformation and form lactam–lactam dimers, not the widely observed amide NH···O═C hydrogen bond chains, while those with steric hindrance take a twisted conformation and form an amide NH···O═C (lactam) hydrogen bond. A succinct theoretic study combining conformational analysis and molecular electrostatic potential surfaces (MEPS) survey provided a reasonable explanation of the formation of these two different hydrogen bond motifs.
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Small
·
2019
·Vol. 16
·期 4
·1905700
·
IF 10.856
Bo Yan,Chun Du,Guowei Yang
Codoping of N and O in ultrathin graphitic carbon nitride (g-C 3 N 4 ) nanosheets leads to an inner electric field. This field restrains the recombination of photogenerated carriers and, thus, enhances hydrogen evolution. The layered structure of codoped g-C 3 N 4 nanosheets (N-O-CNNS) not only provides abundant sites of contact with the reaction medium, but also decreases the distance over which the photogenerated electron–hole pairs are transported to the reaction interface. Quantum confinement in the ultrathin structure results in an increased bandgap and makes the photocatalytic reaction more favorable than bulk g-C 3 N 4 . Under visible light irradiation, N-O-CNNS with 3 wt% Pt achieves a hydrogen evolution rate of 9.2 mmol g −1 h −1 and a value of 46.9 mmol g −1 h −1 under AM1.5 with 5 wt% Pt. Thus, this work paves the way for designing efficient nanostructures with increased separation/transfer efficiency of photogenerated carriers and, hence, increased photocatalytic activities.
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FOOD CHEMISTRY
·
2023
·
IF 8.8
Chenlu Ma,Youfa Xie,Xin Huang,Lu Zhang,David Julian McClements,Liqiang Zou,Wei Liu
A novel phospholipid-based nanovesicle (PBN) was developed to encapsulate (-)-epigallocatechin gallate (EGCG), a major polyphenol in green tea, to mask its bitter taste and expand its application in food products. The PBN was formed using W/O emulsion-transfer methods and showed a multilayer membrane nanovesicle structure (around 200 nm) observed with TEM. The PBN possessed a high encapsulation efficiency (92.1%) for EGCG. The bitterness of EGCG was significantly reduced to 1/12 after encapsulation. Fourier transform infrared spectroscopy (FTIR) indicated the EGCG mainly interacted with the upper chain/glycerol/head group region of the lipid bilayer in PBN. Quartz crystal microbalance with dissipation (QCM-D) showed the addition of γ-cyclodextrin in PBN enhanced EGCG's adsorption with phospholipids and allowed for its good sustained release. Encapsulating EGCG in PBN inhibited its complexation with mucin, reducing bitterness and astringency. This provides a new method to improve EGCG's flavor, potentially expanding its application in the food industry.
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ENVIRONMENTAL RESEARCH
·
2023
·
IF 8.3
Zhengquan Yan,Xuemei Zhou,Lingmin Kong,Wenjing Xu,Junkai Hao,Shuo Sun,Jing Feng,Huitian Zhi,Xiao Zhu,Lei Hu
To effectively differentiate toxic aminophenol isomers, a kind of spindle-shaped Cu-Ru bimetal mesoporous nanozyme (Cu-Ru MPNZ) with high specific surface was developed by one-pot homogeneous reduction method, directed by hexadecyl trimethyl ammonium bromide (CTAB) in this work. By virtue of the distinctive microstructure, Cu-Ru MPNZ expressed superior bi-functional oxidase- and peroxidase-mimic activity to catalyze the oxidation of 3,3′,5,5,’-tetramethylbenzidine (TMB) and 2,2′-azinobis (3-ethylbenzothiazoline-6- sulfonic acid) ammonium salt (ABTS) with low Michaelis-Menten constants and quick reaction rates. Especially, toxic aminophenol isomers could exclusively react with the oxydates of TMB or ABTS to express differentiable signals in color. Under the optimal conditions, Cu-Ru MPNZ was successfully applied for visual differentiation of toxic aminophenol isomers in real aqueous, juices and medicinal samples with low detection limits (1.60 × 10 −8 mol/L for o -aminophenol and 3.25 × 10 −8 mol/L for m -aminophenol) and satisfactory recoveries (96.6–103.5%). The different recognition mechanisms of Cu-Ru MPNZ to toxic o - and m -aminophenol isomers were proposed for the first time as far as we known. This work will provide a potential way to monitor different organic isomer pollution in future.
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