ACS Sustainable Chemistry & Engineering
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2018
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IF 6.14
Mengjie Wu,Hui Ma,Zhongyi Ma,Yufang Jin,Chunyan Chen,Xiaoya Guo,Yan Qiao,Christian Marcus Pedersen,Xianglin Hou,Yingxiong Wang
Deep eutectic solvents (DESs) exhibit similar physicochemical properties to the ionic liquids. They are inexpensive, renewable, nontoxic, and environmentally benign solvents and have gradually attracted attention in several fields, for example, biorefinery. Here choline chloride-based DESs have been used as solvents and catalysts for the preparation of deoxyfructosazine (DOF) through a self-condensation reaction of d-glucosamine (GlcNH2). The catalytic performances of a “green cocatalyst”, amino acids, and the reaction mechanism were also studied. The results displayed that choline chloride/urea was capable to convert GlcNH2 efficiently, with a 13.5% yield of DOF at low temperature and with a short reaction time (100 °C, 150 min). Among the screened amino acids, arginine showed the highest activity and gave the highest yield of DOF (30.1%) under the optimized reaction conditions. Nuclear magnetic resonance (NMR) studies revealed a strong hydrogen bond interaction between GlcNH2 and arginine. Moreover, a detectable intermediate, namely dihydrofructosazine, in the condensation of GlcNH2 to DOF/fructosazine (FZ) was captured by in situ NMR technique.
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BIOMACROMOLECULES
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2015
·
IF 5.75
Piming Ma,Long Jiang,Pengwu Xu,Weifu Dong,Mingqing Chen,Piet J. Lemstra
In this work we report the in situ preparation of fully biobased stereocomplex poly(lactide) (SC-PLA) nanocomposites grafted onto nanocrystalline cellulose (NCC). The stereocomplexation rate by compounding high-molar-mass poly(d-lactide) (PDLA) with comb-like NCC grafted poly(l-lactide) is rather high in comparison with mixtures of PDLA and PLLA. The rapid stereocomplexation was evidenced by a high stereocomplexation temperature (Tc-sc = 145 °C) and a high SC crystallinity (Xc-sc = 38%) upon fast cooling (50 °C/min) from the melt (250 °C for 2 min), which are higher than currently reported values. Moreover, the half-life crystallization time (175–190 °C) of the SC-PLA was shortened by 84–92% in comparison with the PDLA/PLLA blends. The high(er) stereocomplexation rate and the melt stability of the SC in the nanocomposites were ascribed to the nucleation effect of the chemically bonded NCC and the “memory effect” of molecular pairs in the stereocomplex melt because of the confined freedom of the grafted PLLA chains.
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BIOCHEMICAL AND BIOPHYSICAL RESEARCH COMMUNICATIONS
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2015
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IF 2.297
Li Ma,Xia Gong,Ge Kuang,Rong Jiang,Rongchun Chen,Jingyuan Wan
Sesamin has been described to exert anti-oxidant and anti-inflammatory properties. In present study, we investigated the potential effects and mechanisms of sesamin on lipopolysaccharide (LPS)-induced fulminant hepatic failure (FHF) in d -galactosamine (D-GalN)-sensitized mice. Our results showed that pretreatment with sesamin dose-dependently improved LPS/D-GalN-induced mortality and liver injury as indicated by reduced serum levels of aminotransferases and alleviated pathological damage as well as hepatocyte apoptosis in mice. Additionally, sesamin markedly attenuated LPS/D-GalN-induced adhesion molecules expression, and decreased neutrophils recruitment. Furthermore, sesamin inhibited LPS-induced tumor necrosis factor-alpha (TNF-α) production, p38 mitogen-activated protein kinases (MAPK) and NF-κB activation, and Toll like receptor (TLR) 4 expression in mice and in RAW264.7 macrophage cells. In summary, these results demonstrate that sesamin protects mice from LPS-induced FHF and the molecular mechanisms may down-regulate the expression of TLR4, block MAPK and NF-κB activation, decrease the production of TNF-α.
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Chemical Biology & Drug Design
·
2015
·Vol. 87
·期 4
·499-507
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IF 2.485
Xuebao Wang,Di Chen,Shufang Yu,Zaikui Zhang,Yu Wang,Xiaolu Qi,Weitao Fu,Zixin Xie,Faqing Ye
A series of tetrahydrobenzothieno[2,3-d]pyrimidine derivatives were designed, synthesized, and evaluated as inhibitors of FGFR1. These analogs were synthesized via Gewald's reaction under mild conditions. The structures of the synthesized compounds were characterized by spectroscopic data (IR, 1 H NMR and MS). Their antitumor activities were evaluated against H460, A549 and U251 cell lines in vitro . Results revealed that the tested compounds showed moderate antitumor activities. Structure–activity relationship analyses indicated that compounds with an aromatic ring substituted in the C-2 position or with larger molecules such as 3g , 4c , and 7 were more effective than others. The compound, 3g (78.8% FGFR1 inhibition at 10 μ m ), was identified to have the most potent antitumor activities, with IC 50 values of 7.7, 18.9, and 13.3 μ m against the H460, A549, and U251 cell lines, respectively. Together, the results suggested that tetrahydrobenzothieno[2,3-d]pyrimidine derivatives may serve as a potential agent for the treatment of FGFR1-mediated cancers.
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Journal of Physical Chemistry C
·
2015
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IF 4.772
Yongxin Tao,Xiaogang Gu,Linhong Deng,Yong Qin,Huaiguo Xue,Yong Kong
We report a Cu2+-modified β-cyclodextrin, Cu2-β-CD, that was self-assembled on poly(l-glutamic acid) (P-l-Glu) for chiral recognition of d-tryptophan (d-Trp). Cu2+ formed binuclear hydroxy-bridge (Cu(OH)2Cu) at the wider opening of the cavity of β-CD and acted as a cap to prevent high-energy water molecules from being released while forcing Trp isomers to enter through its narrower opening. Because H-bonds were favored to form between the high-energy water molecules and the amino groups of d-Trp inside the cavity of β-CD, d-Trp was thus recognized. The recognition capability of the Cu2-β-CD appeared to depend on the way the Cu2-β-CD self-assembled onto P-l-Glu, preferring via H-bonds rather than via electrostatic interactions, because electrostatic interactions between P-l-Glu and Cu(OH)2Cu could alter the configuration of the Cu2-β-CD cavity, resulting in weakened H-bonds between high-energy water molecules and d-Trp.
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Nanoscale
·
2016
·Vol. 8
·期 18
·9764-9770
·
IF 7.76
Tengfei Long,Yanjia Guo,Min Lin,Mengke Yuan,Zhongde Liu,Chengzhi Huang
Despite a significant surge in the number of investigations into both optically active Au and Ag nanostructures, there is currently only limited knowledge about optically active Cu nanoclusters (CuNCs) and their potential applications. Here, we have succeeded in preparing a pair of optically active red-emitting CuNCs on the basis of complexation and redox reaction between copper(II) and penicillamine (Pen) enantiomers, in which Pen serves as both a reducing agent and a stabilizing ligand. Significantly, the CuNCs feature unique aggregation induced emission (AIE) characteristics and therefore can serve as pH stimuli-responsive functional materials. Impressively, the ligand chirality plays a dramatic role for the creation of brightly emissive CuNCs, attributed to the conformation of racemic Pen being unfavorable for the electrostatic interaction, and thus suppressing the formation of cluster aggregates. In addition, the clusters display potential toward cytoplasmic staining and labelling due to the high photoluminescence (PL) quantum yields (QYs) and remarkable cellular uptake, in spite that no chirality-dependent effects in autophagy and subcellular localization are observed in the application of chiral cluster enantiomer-based cell imaging.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2016
·
IF 2.567
Binglin Li,Jiao Wang,Xiaoli Zhang,Binxia Zhao
Phospholipase D (PLD) was immobilized in a simple and effective way by adsorption and precipitation of the enzyme, followed by chemical cross-linking to form an “enzyme net” covering the surface of nonporous silicon dioxide nanoparticles. For catalyzing transphosphatidylation to produce phosphatidylethanolamine (PE), at pH 6.0 and 35 °C (the optimum operational conditions), the specific activity of immobilized PLD reached 15872 U/gprotein, which was approximately 1.15 times higher than the maximum value of specific activity of free PLD (13813 U/gprotein). A kinetic study demonstrates immobilized PLD had increases in catalytic activity and enzyme–substrate affinity. In addition, the thermostability and pH tolerance were significantly enhanced compared with free PLD. The half-life of immobilized PLD was significantly increased from 30 to 70 days at 4 °C (approximately 2.3 times). This novel method has been proven to be suitable for the production of robust biocatalysts.
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JOURNAL OF PHARMACEUTICAL AND BIOMEDICAL ANALYSIS
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2024
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IF 3.1
Wenchan Deng,Rongrong Huang,Yuanjiang Pan,Cuirong Sun
The metabolism process of amino acids is closely related to the growth of normal and cancer cells. It is still not clear how L/D-configuration amino acids participate in the metabolism of colorectal cell. Herein, intra- and extra-cellular metabolic distribution of L/D-amino acids in colorectal cell (HCT116) and human normal intestinal epithelial cell (NCM460) were profiled utilizing HPLC-MS/MS coupled with a chiral probe. The results displayed the differential metabolic portrayal for the two cell lines. Compared with NCM460 cell, 13 kinds of significant differential amino acids were founded in a lower concentration within HCT116 cell, and L-Gln was even not detected for intra-cell; as for extra-cell culture medium, the HCT116 cell consumed more L-Gln, D-Phe and D-Leu, while L-Met was low ingested in HCT116 cell. L-Ala and Gly were excretion in both two cell lines, excepted L-Cit which was uptake in HCT116 and excretion in NCM460 cell. Furthermore, the dynamic changes of chiral amino acids displayed that phenylalanine, tyrosine and tryptophan biosynthesis and arginine biosynthesis is the major pathway for intra-cellular metabolites and extra-cellular metabolites, respectively. Moreover, with additional D-amino acids in culture medium, the results exhibited that high concentration of D-amino acids have no significant effect on the proliferation of NCM460 cell, but could influence the profiling of amino acids metabolites, and further affect the proliferation of HCT116 cell. This present work enhances the understanding of these differential amino acids metabolic network and depicts a dynamic process of metabolic dysregulation of HCT116 and NCM460 cell.
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ELECTROCHIMICA ACTA
·
2025
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IF 5.6
Hongdi Zheng,Liuyan Zhang,Yingying Li,Binkai Yuan,Shixuan Wang,Zeyi Guan,Gengzhe Shen,Guibin Tan,Yanmei Zhang
A honeycomb-like porous self-supporting Ni-Al(G) electrode was successfully prepared by low-pressure cold spraying combined with heat treatment. The main components of the electrode were Ni and NiAl. Graphene was uniformly dispersed throughout the electrode, exhibiting a 3-D distribution, which increased the active site of electrode and improved the electron exchange rate. The electrochemical properties of the Ni-Al(G) electrode were characterized using 6 M KOH. As a result, the Ni-Al(G) electrode requires only an overpotential of 130 mV to achieve a current density of 100 mA cm −2 , and a Tafel slope of 35.5 mV dec −1 . In addition, the electrode exhibited excellent stability. The addition of graphene and the honeycomb-like porous structure of the Ni-Al(G) electrode resulted in an excellent hydrogen evolution activity. This study provides a simple and rapid technique for building high-performance, low-cost, and industrially available electrodes for the efficient alkaline HER.
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INTERNATIONAL JOURNAL OF MOLECULAR SCIENCES
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2025
·Vol. 26
·期 4
·1558
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IF 4.9
Jiabin Huang,Haotian Wu,Ranran Gao,Lan Wu,Mengyue Wang,Yang Chu,Yuhua Shi,Li Xiang,Qinggang Yin
L-ascorbic acid (vitamin C, AA) is widely present in plants, but humans lack the ability to synthesize it independently. As a potent reducing agent, AA is susceptible to oxidation, making the enhancement of its stability crucial. 2-O-β-D-glucopyranosyl-L-ascorbic acid (AA-2βG) is a stable natural derivative of AA with glycosylation, initially discovered in the fruits ofLycium barbarum. Understanding the biosynthesis of AA-2βG is crucial for enhancing its production inL. barbarum. While the established biosynthesis pathway of AA constitutes the upstream of AA-2βG biosynthesis, the conclusive step of β-glycosylation remains unclear. We identified aL. barbarumcultivar by UPLC, ZN01, with a high content of AA-2βG, and compared its leaves, immature fruits, and mature fruits to a normal AA-2βG contentL. barbarumcultivar for metabolomic and transcriptomic analysis. The RNA-seq and RT-qPCR analysis revealed that the expression levels of genes involved in the AA biosynthesis pathway did not consistently correlate with AA-2βG content, suggesting that the final glycosylation step may be a key determinant of AA-2βG accumulation. Subsequently, utilizing phylogenetic and co-expression analysis, we identified ten UDP-glycosyltransferases (UGTs) and three β-glucosidases (BGLUs) which may be involved in the crucial step of the conversion from AA to AA-2βG, and the UGTs’ activities were predicted through molecular docking. Lastly, we speculated that the presence of the glycosylation process of AA might have a crucial role in maintaining AA homeostasis inL. barbarum, and deliberated on potential correlations between AA, carotenoids, and anthocyanins. Our integrated multi-omics analysis provides valuable insights into AA-2βG biosynthesis inL. barbarum, identifying thirteen candidate genes and highlighting the complex interplay between AA, carotenoids, and anthocyanins. These findings have implications for improving AA-2βG content inL. barbarum.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
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2024
·
IF 7.7
Xiaolong Sun,Jiahuan Hu,Yufeng Zhou,Xiangyu Zi,Huayue Zhu,Xi Luo,Yongqian Fu
In this study, we endeavored to catalyze the biosynthesis of D -phenyllactic (D-PLA) from L-Phenylalanine (L-Phe) through a one-pot method. However, the crucial enzymes for the biosynthesis of phenylpyruvate (PPA), amino acid oxidase (L-AAD), is a membrane-bound protein. Herein, we proposed a novel co-immobilization strategy of whole cells and enzymes, integrating them into ZIF-90 to achieve efficient biosynthesis of D-PLA. Consequently, we embarked on integrating both enzyme and E. coli into ZIF-90, ultimately obtaining the novel biocatalyst E. coli /LDH@ZIF-90. This achievement facilitated the cascade reaction between LDH and E. coli , enabling a streamlined one-pot bioconversion process. The morphology and structure of E. coli /LDH@ZIF-90 were thoroughly characterized using a range of methods, including XRD, SEM, FT-IR, CLSM, and XPS, which confirmed that the material had been successfully synthesized. Further activity experiments revealed that E. coli /LDH@ZIF-90 exhibited good stability even under harsh conditions. Additionally, the biocatalyst retained 76 % of its initial catalytic activity after completing six cycles. Moreover, when utilized for the biosynthesis of D-PLA, this system demonstrated an impressive conversion rate of 85.2 % after 12 h. The successful cascade catalysis from L-Phe to D-PLA underscored the potential of the enzyme-cell cascade catalytic system, offering valuable insights for its potential industrial applications.
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ACS Catalysis
·
2025
·
IF 13.1
Ren Ma,Yujing Zhang,Feiyang Yu,Shilong Wei,Yang Xing,Chengfang Qiao,Zhengqiang Xia,Qi Yang,Gang Xie,Sanping Chen
High energy level difference between electron donor (D) and electron acceptor (A) and low energy loss during charge transfer are prerequisites for the construction of efficient D–A-type covalent-organic framework (COF) photocatalysts. However, the spatial structure characteristics of the building blocks inevitably lead to the torsion of the D–A COF skeleton during the construction process and thus prevent effective charge migration. Herein, with the high-energy-level triphenylamine (TPA) as a model electron donor, the formyl positional isomers of tris(3-formylbiphenyl) amine (NDC) and tri(4-formylbiphenyl) amine (NBC) react with an acceptor 1,3,5-tris(4-aminophenyl) triazine (TTA), producing both D–A COFs for photocatalytic CO2 reduction and benzylamine coupling reactions. Structural investigations evidence that the formyl positional isomerism imparts the dihedral angle of TPA single arm reducing from 51.09 to 2.12°, the interlayer spacing from 3.89 to 3.55 Å, and the exciton binding energy from 97.25 to 85.86 meV in TTA-COFs. Such the “near-flat” TTA-NDC structure with confined clover-like channels dramatically accelerates the intralayer and interlayer charge migration efficiency and improves CO2 adsorption and oxygen activation ability (O2•– concentration of 48.01 μmol·L–1 in 3 h). To the best of our knowledge, TTA-NDC exhibits the highest benzylamine coupling efficiency with a turnover frequency value of 518.4 h–1 among the pristine COF photocatalysts, and its electron consumption rate for photocatalytic CO2 reduction reaches 1632.2 μmol·g–1·h–1, 3.85-fold higher than TTA-NBC, far surpassing most COF-based photocatalysts. Parallelly, the protonated H-TTA-NDC shows high CO2 reduction to CH4 yield (310.1 μmol·g–1·h–1) and selectivity (85.1%) due to the improved proton conductivity (σ = 1.07 × 10–2 S·cm–1). Additionally, the durability, stability, and possible photocatalytic mechanisms of TTA-NDC were systematically investigated.
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