ANALYTICAL AND BIOANALYTICAL CHEMISTRY
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2016
·Vol. 408
·期 29
·8317-8323
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IF 3.125
Yan Zequn,Xue Min,He Qian,Lu Wei,Meng Zihui,Yan Dan,Qiu Lili,Zhou Lijun,Yu Yingjie
A novel polymerized crystalline colloidal array (PCCA) sensing material for the detection of urine glucose was developed by embedding a two-dimensional (2-D) polystyrene crystalline colloidal array (CCA) in 3-acrylamidophenylboronic acid (3-APBA)-functionalized hydrogel. After adjusting the cross-linker concentration, this material showed significant sensitivity for glucose under lab conditions, the particle spacing of the PCCA changed from 917 to 824 nm (93 nm) within 3 min as the glucose concentration increased from 0 to 10 mM, and the structural color of the PCCA changed from red through orange, to green, and finally, to cyan. In further experiments, this material was used to semi-quantitatively detect glucose in 20 human urine (HU) samples. Compared with the traditional dry-chemistry method, which was applied widely in clinical diagnosis, the PCCA method was more accurate and cost-effective. Moreover, this method can efficiently avoid the errors induced by most of the urine-interfering elements like vitamin C and ketone body. With a homemade portable optical detector, this low-cost intelligent sensing material can provide a more convenient and efficient strategy for the urine glucose detection in clinical diagnosis and point-of-care monitoring.
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Analytical Methods
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2024
·
IF 2.7
Wu Bing,Sun Xiaoyu,Shao Zeman,Sen Liu,Zhongmei Yang,Qiuyang Zhang,Yanchun Wei
Mercury ions (Hg2+)are highly toxic heavy metal ions, posing serious health risks to humans when present above safe concentrations1–3. Therefore, the development of a rapid and effective Hg2+ detection method is of significant importance. In this study, based on surface plasmon resonance (SPR) technology integrated with COMSOL simulation analysis, a highly sensitive and selective Hg2+ sensing system is constructed. Initially, the gold nanoparticles and the surface of the fiber optic gold film are modified by sodium sulfide (Na2S). In the presence of Hg2+, the modified sulfur ions specifically bind to Hg2+, forming a composite structure Au/S-Hg2+-S/AuNPS. Due to the strong electromagnetic coupling between gold nanoparticles and the gold film, a significant SPR wavelength shift occurs. Experimental results demonstrate the high sensitivity of the sensor to Hg2+. The fiber optic SPR transducer exhibits enhanced selectivity towards Hg2+ ions and high recovery rates in real environmental samples. This sensing system provides an alternative method for rapid and accurate determination of mercury content.
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PROCESS BIOCHEMISTRY
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2024
·
IF 3.7
Puhong Yi,Yue Xu,Hanlin Liu,Yuhua Hao,Mengdan Liu,Zhiqiang Liu,Yaping Xue,Liqun Jin,Yuguo Zheng
2-oxo-4-[(hydroxy)(methyl)phosphinoyl]butyric acid (PPO) is a valuable prochiral keto acid for the asymmetric synthesis of the important herbicide L-phosphinothricin (L-PPT). Developing an efficient biocatalytic pathway to meet the increasing demand for PPO is highly attractive. In this study, a robust D-amino acid aminotransferase from Cytobacillus firmus ( Cf DAAT) was screened, which exhibited excellent tolerability to D,L-PPT and showed remarkable specific activity and affinity toward pyruvate (61.9 U/mg, Km = 7.4 mM). A designed co-substrate regeneration system was then introduced to shift the reaction equilibrium forward by coupling with D-amino acid oxidase (DAAO) and catalase (CAT). An efficient whole-cell biocatalyst was obtained by fine-tuning RBS intensity to coordinate the co-expression of the three enzymes. Moreover, the optimum conditions to promote overall conversion efficiency were identified by response surface methodology. Consequently, with only a catalytic amount of pyruvate (3.33 mol%) added in a 1 L reaction system, 200 mM D-PPT (400 mM D,L-PPT) was completely converted in 10 h, resulting in a PPO productivity of 3.33 g⋅L −1 ⋅h −1 , and a notable conversion rate of >99% at 300 mM D-PPT in 16 h. It demonstrated a considerable catalytic level and provided a competitive route for industrial PPO production from D,L-PPT.
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JOURNAL OF BIOLOGICAL CHEMISTRY
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2024
·
IF 4
Chunxiu Liu,Kailiang Ma,Li Jiang,Xumei Liu,Yang Tong,Sen Yang,Xinghua Jin,Yifeng Wei,Yan Zhang
The sulfite-reducing bacterium Bilophila wadsworthia , a common human intestinal pathobiont, is unique in its ability to metabolize a wide variety of sulfonates to generate sulfite as a terminal electron acceptor (TEA). The resulting formation of H 2 S is implicated in inflammation and colon cancer. l -cysteate, an oxidation product of l -cysteine, is among the sulfonates metabolized by B. wadsworthia , although the enzymes involved remain unknown. Here we report a pathway for l -cysteate dissimilation in B. wadsworthia RZATAU, involving isomerization of l -cysteate to d -cysteate by a cysteate racemase ( Bw CuyB), followed by cleavage into pyruvate, ammonia and sulfite by a d -cysteate sulfo-lyase ( Bw CuyA). The strong selectivity of Bw CuyA for d -cysteate over l -cysteate was rationalized by protein structural modeling. A homolog of Bw CuyA in the marine bacterium Silicibacter pomeroyi ( Sp CuyA) was previously reported to be a l -cysteate sulfo-lyase, but our experiments confirm that Sp CuyA too displays a strong selectivity for d -cysteate. Growth of B. wadsworthia with cysteate as the electron acceptor is accompanied by production of H 2 S and induction of Bw CuyA. Close homologs of Bw CuyA and Bw CuyB are present in diverse bacteria, including many sulfate- and sulfite-reducing bacteria, suggesting their involvement in cysteate degradation in different biological environments.
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Soft Matter
·
2011
·Vol. 7
·期 14
·6451-6456
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IF 4.457
Shengtong Sun,Peiyi Wu
Near infrared spectroscopy in combination with two-dimensional correlation spectroscopy (2Dcos) and perturbation correlation moving window (PCMW) technique is employed to illustrate the gelation microdynamic mechanism of hydrogelator N-octyl-D-gluconamide (8-GA), which can rapidly self-agglomerate into helical bilayer micellar fibers upon cooling from spherical micelles. Boltzmann fitting and PCMW easily determined the gelation temperature to be ca. 72 °C and the transition temperature range to be 70–75 °C. Moreover, band shifting and splitting phenomena can be observed for CH-related overtones, indicating the formation of much ordered and tight hydrophobic core from octyl tails. On the other hand, 2Dcos was used to discern the sequential orders during the gelation process and concluded that all the group motions have a continuous transfer from the octyl tail to the chiral carbohydrate head followed by the final immobilization of the solvent, which meanwhile, is actually a continuous dehydration process from the hydrophobic core to the outer hydrophilic chiral head. The driving force of the gelation process in microdynamics can only be the dehydration process of hydrophobic octyl chains, but with final helical superstructures being stabilized by amide-associated hydrogen bonding and the “chiral bilayer effect” of carbohydrate heads.
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RSC Advances
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2017
·Vol. 7
·期 15
·8823-8831
·
IF 3.108
Tsogzolmaa Ganbold,Gerile Gerile,Hai Xiao,Huricha Baigude
RNA interference (RNAi) has shown great potential for clinical treatment of a variety of diseases. As an effective post-transcriptional regulation, RNAi induces degradation of specific target mRNA, leading to a decreased level of disease related gene product, which could be resistant to conventional small molecule therapeutics. Because of the relatively small size of short interfering RNA (siRNA) as well as it's robustness in the design of efficient 20–22 nucleotide sequences targeting any known gene, delivery of siRNA in vitro and in vivo has achieved tremendous success by the design and fabrication of various carrier materials including peptides, lipids, and polymers. While siRNA delivery efficiency of these materials proved to be appreciable, their tissue specificity, biocompatibility and cytotoxicity still need much improvement. We report a novel siRNA delivery material designed by optimization of our previously reported peptidomimetic based lipoplex. The novel lipoplex, which bears a D-amino acid based dipeptide head group, possesses an ideal balance of increased stability in a tissue environment, and enhanced efficiency of tissue specific delivery as well as minimized cytotoxicity. The novel lipoplex carrying siRNA efficiently targeted mouse liver, initiated RNAi and knocked down the apoB dose dependently, which is confirmed by both RT-qPCR and Western blotting. Moreover, the novel lipoplex does not induce any apparent cytotoxicity, as confirmed by the measurement of liver enzyme levels in serum.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2025
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IF 21.1
Yisong Zhou,Jiawei Xie,Yushuang Huang,Chang-an Zhou,Chao Wang,Lei Song,Kui Ma,Hairong Yue,Ji-Jun Zou,Bin Liang
The hydrogenative rearrangement of biomass-derived furfural offers a sustainable pathway to produce cyclopentanol (CPL) and cyclopentanone (CPO), which are traditionally obtained from fossil resources. Achieving selective synthesis of either product requires precise control over catalyst electronic structure and adsorption behavior, yet it still remains challenging. Herein, we report that both doping and tuning the spatial distance between Pt clusters effectively regulate the d -band center of active sites, enabling selective synthesis of CPO and CPL with high yields of 97.2 % and 96.0 %, respectively. Mechanistic studies suggest that reducing the spatial distance between Pt nanoclusters elevates the d -band center, thereby reducing the occupancy of antibonding states and strengthening the Pt-O bond between Pt and CPO, thus favoring CPL formation. By contrast, doping Pt with NiP lowers the d -band center, thus weakening CPO adsorption and promoting its selective synthesis. These results highlight d -band center regulation as a promising strategy for achieving selective hydrogenation.
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Materials Science & Engineering C-Materials for Biological Applications
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2013
·
IF 2.404
Ming Zhang,De-Jun Chen,Rui-Zhi Wang,Jiu-Ju Feng,Zhengyu Bai,Ai-Jun Wang
Single crystalline flower-like Bi 2 S 3 nanostructures were successfully synthesized via a simple, facile and green hydrothermal method, with the assistance of D -penicillamine. The products were characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM), and transmission electron microscopy (TEM), and found their morphologies mainly depend on the ratios of Bi 3 + to D -penicillamine, as well as the reaction temperature and time. And the possible growth mechanism has been discussed in some detail. In addition, the as-prepared Bi 2 S 3 nanoflowers show good hydrogen storage ability. This strategy can be potentially expanded to prepare other metal chalcogenides materials.
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BIOORGANIC CHEMISTRY
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2025
·
IF 4.7
Ruobin Sun,Qipeng Yan,Wenhao Deng,Pengcheng Chen,Dan Wu,Pu Zheng
Achieving enzyme catalysis at high substrate concentrations is a substantial challenge in industrial biocatalysis, and the role of glycosylation in post-translational modifications that modulate enzyme substrate inhibition remains poorly understood. This study provides insights into the role of N -glycosylation in substrate inhibition by comparing the catalytic properties of d -lactonohydrolase ( d -Lac) derived from Fusarium moniliforme expressed in prokaryotic and eukaryotic hosts. Experimental evidence indicates that recombinant d -Lac expressed in Pichia pastoris ( Pp Lac-WT) exhibits higher hydrolysis rates at a substrate concentration of 400 g/L, with reduced substrate inhibition and enhanced stability compared to the recombinant d -Lac expressed in Escherichia coli ( Ec Lac-WT). Mutant Pp Lac-M1 achieves a conversion rate of 40 % at a substrate concentration of 400 g/L, with a space–time yield of d -pantoic acid reaching 91.1 g/L/h. Proteomics analysis reveals that residues N29 and N278, located approximately 10–20 Å from the active site undergo N -glycosylation in Pp Lac-WT. Using microsecond-scale molecular dynamics simulations and Markov state models, we elucidate the effects of glycosylation on the conformational flexibility of two key loops at the entrance of the binding pocket. Specifically, the loops in Pp Lac-WT can transition between open and closed states, whereas those in Ec Lac-WT tend to remain open. In high substrate concentration conditions, the open state causes congestion, leading to substrate inhibition. Shortest-path map analysis confirms that substrate entry is dynamically controlled by residue N29 on the loops surrounding the active site. Our findings enhance the understanding of the effects of glycosylation on enzyme conformational dynamics and provide insights into mitigating inhibition at high substrate concentrations.
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Scientific Reports
·
2016
·Vol. 6
·期 1
·1-10
·
IF 5.228
Liang Chaoning,Zhang Yi,Jia Yan,Wenzhao Wang,Li Youhai,Lu Shikun,Jin Jian-Ming,Tang Shuang-Yan
Glycodiversification broadens the scope of natural product-derived drug discovery. The acceptor substrate promiscuity of glucosyltransferase-D (GTF-D), a carbohydrate-processing enzyme from Streptococcus mutans , was expanded by protein engineering. Mutants in a site-saturation mutagenesis library were screened on the fluorescent substrate 4-methylumbelliferone to identify derivatives with improved transglycosylation efficiency. In comparison to the wild-type GTF-D enzyme, mutant M4 exhibited increased transglycosylation capabilities on flavonoid substrates including catechin, genistein, daidzein and silybin, using the glucosyl donor sucrose. This study demonstrated the feasibility of developing natural product glycosyltransferases by engineering transglycosidases that use donor substrates cheaper than NDP-sugars, and gave rise to a series of α-glucosylated natural products that are novel to the natural product reservoir. The solubility of the α-glucoside of genistein and the anti-oxidant capability of the α-glucoside of catechin were also studied.
研究领域:
生物化学
·
药物开发
·
合成生物学
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APPLIED SURFACE SCIENCE
·
2022
·
IF 7.392
Xiaojie Liu,Yong Zhao,Yahui Du,Quanliang Wang,Xin Jing,Liangmin Yu,Mingliang Sun
Conjugated donor (D)–acceptor (A) polymer heterojunctions have developed as attractive photocatalysts. However, it is a great difficulty in precisely keeping the batch-to-batch reproducibility of polymers and controlling the related photocatalytic activity . Herein, three ladder-like small molecules BTx (BT2F, BTORCAE, and BTORIC2Cl) are synthesized via molecular engineering and the corresponding BTx/g-C 3 N 4 heterojunctions are developed as photocatalysts for sterilization and contaminant degradation. It is demonstrated that employing another A unit into the D–A–D backbones of the small molecule could promote its intramolecular charge transfer and also improve the intermolecular charge transfer. Notably, BTORIC2Cl employing 2-(5,6-Dichloro-3-oxo-2,3 dihydro-1H-inden-1-ylidene)malononitrile as A 1 unit in its symmetric A 1 –D–A 2 –D–A 1 structure displays near-infrared absorption and extends the absorption edge of BTORIC2Cl/g-C 3 N 4 to 850 nm. With the synergy of efficient intermolecular charge transfer, BTORIC2Cl/g-C 3 N 4 contributes the champion photocatalytic activity of 98.9 % and 99.6 % antibacterial rates for Staphylococcus aureus and Escherichia coli . Moreover, the highest degradation reaction rate constant for Rhodamine B obtained by BTORIC2Cl/g-C 3 N 4 is 5.7 times that of g-C 3 N 4 . This study proposes new ideas of fabricating small molecules/g-C 3 N 4 OSHJs as photocatalysts via rational molecular engineering.
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JOURNAL OF CHEMICAL THERMODYNAMICS
·
2016
·
IF 2.196
Dandan Han,Yumin Liu,Xiaona Li,Teng Zhang,Zhenfang Li,Shichao Du,Mingxia Guo,Shijie Xu,Bo Yu,Baohong Hou,Junbo Gong
The solubility of calcium d -pantothenate in (water + methanol) mixtures and the effect of β -alanine on the solubility of calcium d -pantothenate in a constant mole ratio of methanol and water was measured from 263.15 K to 303.15 K by the HPLC analysis method ( P = 0.1 MPa). The solubility of calcium d -pantothenate increased with increasing temperature in all the mixtures at constant composition. Besides, it also increased with mole fraction of water in (water + methanol) mixtures at a constant temperature. Additionally, the solubility of calcium d -pantothenate was enhanced by β -alanine at a given temperature. The experimental solubility in (water + methanol) mixtures was correlated by the modified Apelblat equation, the ternary NRTL equation and Solubility-Polarity Model. The Apelblat equation, the quaternary NRTL equation and the Cohn equation were adopted to correlate the experimental solubility in the (water + methanol + β -alanine) mixtures. Worthwhile, the quaternary NRTL equation was first applied to correlating the quaternary solid-liquid equilibrium. It turned out that all the selected models give good performance on solubility prediction.
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