MICROCHIMICA ACTA
·
2016
·Vol. 183
·期 5
·1779-1786
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IF 4.831
Li Huihui,Zhu Shuqiang,Cheng Ting,Wang Shuxia,Zhu Bin,Liu Xiaoyan,Zhang Haixia
Boronate affinity materials have been widely used for selective capture of cis-diols such as nucleosides. Adsorbents with features of low binding pH and high adsorption capacity are highly desired. However, most reported materials only possess one of the two features. We have synthesized a 1,3,5-triazine-containing binary boronic acid by reacting cyanuric chloride with 3-aminophenylboronic acid, and the product was then grafted onto attapulgite (a fibrous aluminum-magnesium silicate). The resulting functionalized attapulgite exhibit low binding pH (5.0) and display high adsorption capacity (19.5 ± 1.1 mg⋅g −1 for adenosine). The material exhibits high selectivity for cis-diols even in the presence of a 1000-fold excess of interferences. It was applied to the selective extraction of nucleosides from human urine. Typical features of the method include (a) limits of detection in the range from 4 to 17 ng⋅mL −1 , (b) limits of quantification between 13 and 57 ng⋅mL −1 , (c) relative standard deviations of ≤9.1 %, and (d) recoveries of nucleosides from spiked human urine between 85.0 and 112.9 %. In our perception, the material and method offer a promising strategy for selective capture of cis-diols in the areas of proteomics, metabolomics and glycomics.
We have prepared 1,3,5-triazine-containing binary boronic acid-functionalized attapulgite. The material exhibited low binding pH (5.0) and high adsorption capacity (19.5 ± 1.1 mg⋅g‾ 1 for adenosine).
研究领域:
生物化学
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分析化学
·
材料科学
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DOI
高影响因子
ACS Applied Polymer Materials
·
2024
·
IF 4.4
Weicheng Tang,Jianqiong Mou,Yujuan Chen,Yunli Yu,Xiaoyang Yu,Qiaolian Cheng,Zihao Wan,Wenfeng Tan,Mingming Liu
The quality of microcystin-LR (MC-LR) standards is frequently low and varies considerably due to the quite complex and challenging isolation and purification of MC-LR from Microcystis aeruginosa lysates. To streamline the way of standard acquisition, we describe an approach that combines rational design and directed chemical evolution for discovering synthetic hydrogel copolymers, which are potential abiotic affinity materials for MC-LR. A small focused polymer library was engineered by incorporating various combinations and ratios of candidate N-acryloyl-(l)-amino acid monomers, including N-acryloyl-glycine (AGly), N-acryloyl-l-phenylalanine (APhe), and N-acryloyl-l-glutamic acid (AGlu), that were selected based on the analysis of structural and physicochemical properties of MC-LR. A hydrogel copolymer AGlu-NP13 (58% AGlu, 40% TBAm, and 2% BIS) that had a high and specific affinity to MC-LR was screened from the polymer library. The hydrogen bond interaction may dominate the AGlu-NP13–MC-LR binding. The external conditions that influence the hydrogen bond interaction, including pH and solvation environments, controlled the catch and release of MC-LR on AGlu-NP13. The uptake of MC-LR is maximum under a saturated ethyl acetate (10%, v/v) solution at pH 3. The bound MC-LR can be completely desorbed from the hydrogel copolymer with a pH 9.5 and 70% methanol aqueous solution. The screened polymer affinity ligand was successfully applied for the isolation and purification of MC-LR from the lyophilized cell extracts of M. aeruginosa 905, providing a potential application of this material in standard preparation, sample pretreatment, and adsorption removal of MC-LR in complicated environmental and biological samples.
研究领域:
环境科学
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生物化学
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材料科学
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DOI
高影响因子
TALANTA
·
2020
·
IF 5.339
Muhammad Mujahid Ali,Dilshad Hussain,Yan Tang,Xuechun Sun,Zhengchao Shen,Fengxia Zhang,Zhenxia Du
Boronic acid-based affinity materials have gained tremendous attention for the selective separation and recognition of cis-diol containing biomolecules. But often, these boronate affinity materials are stuck to some serious issues like high binding pH and weak affinity, especially in the case of glycoproteins . Here in this study, we used 5-boronoisophthlic acid as a novel affinity ligand for the selective capture and release of glycoproteins. The pKa value of 5-boronoisophthalic acid is investigated to be 7.8 which is just closed to physiological pH and is ideally suitable for the fast binding and elution kinetics of glycoproteins to avoid their degradation and deactivation. The affinity ligand is attached to the surface of polymer support using branched polyethyleneimine (PEI) which enhances the binding strength as it has multiple amine groups available for the attachment of 5-boronoisophthalic for synergistic interactions. The resulting affinity material is characterized and packed in a micropipette-tip using hydrophilic melamine foam as a frit to make the separation process smooth, simple, reliable, and robust. This boronic acid-based affinity tip exhibits binding constants for model glycoproteins in the range of 10 −6 –10 −7 M, binding capacities in the range of 0.662 μM/g, and selectivity up to 1:1000 (HRP to BSA) under optimized extraction conditions. Finally, the boronic-based affinity tip is successfully applied to selectively capture the glycoproteins from the human milk sample, especially lactoferrin which is highly important in dairy manufacture.
研究领域:
生物化学
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分离科学
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蛋白质组学
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DOI
PubMed
高影响因子
MICROCHIMICA ACTA
·
2018
·Vol. 185
·期 3
·1-8
·
IF 5.705
Deng Ya’nan,Gao Qin,Ma Juan,Wang Chaozhan,Wei Yinmao
Poly(3-acrylamidophenylboronic acid) (PAAPBA) was grafted onto polydopamine-coated magnetic graphene oxide via surface-initiated atom transfer radical polymerization to obtain a new kind of boronate affinity material (BAM). The BAM possesses good water dispersity and adsorption capacities as high as 154, 357, 588 and 1111 μmol·g −1 for adenosine, salbutamol, dopamine and catechol, respectively. For the molecules without nitrogen atoms, the BAM can selectively capture the cis -diols under the interference of non- cis -diols. For molecules containing nitrogen, the non- cis -diols are also retained, but much less than the cis -diols. The selectivity can be improved by adding salts to facilitate complexation and to suppress the electrostatic interaction between cis -diols and the boronic acid ligand. The BAM was successfully employed to the enrichment of catecholamines from real urine samples. Results indicate that it is a promising material for the pretreatment of real samples.
Schematic of the preparation of an ultrahigh capacity boronate affinity material by grafting polymer brush from polydopamine coated magnetic graphene oxide. The material has good selectivity to cis -diol-containing molecules and can be applied to enrich catecholamines in urine samples.
研究领域:
分析化学
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材料科学
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生物医学
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产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2019
·
IF 8.355
Ningning Zhao,Zhiqiang Liu,Junpeng Xing,Zhong Zheng,Fengrui Song,Shu Liu
Boronate-functionalized materials have been widely used for the selective separation and enrichment of glycoproteins and glycans. However, emerging boronic acid materials either use expensive boronic acid compounds containing electron-withdrawing groups combined with a graft structure or explore only simple methods for the synthesis of boronic acid structures with improved electron-withdrawing groups. In this study, polyethyleneimine (PEI)-assisted teamed boronate affinity (TBA)-functionalized magnetic nanoparticles (MNPs) (Fe 3 O 4 @PEI@TBA NPs) were designed to specifically capture trace ginsenosides from rat plasma under neutral conditions without requiring protein precipitation. The synergistic effect of the Fe 3 O 4 @PEI@TBA NPs exhibited higher affinity for ginsenosides (45.64 mg g −1 ) based on PEI dendrimer-assisted multivalent binding, the low p K a value of TBA and specific recognition sites. Additionally, the captured ginsenosides were quickly detected and characterized using ultra-high-performance liquid chromatography coupled with high-resolution mass spectrometry (UHPLC-MS) and an enriched in-house library. Compared to the 37 compounds identified using the methanol method, 63 ginsenoside prototypes and metabolites were successfully detected and identified in rat plasma by applying this novel integrated strategy. The strategy exhibited selectivity and identified more types and quantities of ginsenosides. Our study provided in-depth insight into the synergistic development of specific functional materials in combination with advanced analytical platforms for the selective capture and characterization of trace glycoconjugate families in analytical, engineering and biomedical fields under neutral conditions.
研究领域:
分析化学
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生物医学
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材料科学
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产品关联
DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2022
·Vol. 46
·期 27
·13207-13212
·
IF 3.925
Baoyue Zhang,Xue Chen,Jianghua He,Bailin Guo,Sheng Bi,Feng Zhang,Miaomiao Tian
Glycoproteins play an important role in biological processes such as protein folding, information transmission, nerve conduction, and molecular recognition. Therefore, designing and developing an adsorbent with high adsorption capacity for glycoproteins are of great importance. In this study, a novel boronate affinity material (Zr-MOF@S-S@B) has been prepared by combining a Zr-MOF, a disulfide covalent bond (–S–S–), and 4-mercaptophenylboronic acid (4-MPBA) for the selective enrichment and elution of glycoproteins at physiological pH. The affinity between boronic acid and cis-diol leads to a high adsorption capacity of 625.5 mg g−1 to the composite material for ovalbumin (OVA). At the same time, Zr-MOF@S-S@B is reusable and has a large specific surface area. Furthermore, the material contains disulfide bonds that can release surface-binding glycoproteins specifically under physiological pH conditions, thus effectively avoiding the reduction of glycoprotein activity. The method is successfully used for the enrichment of OVA in egg white samples and protein powder, which has broad application prospects in the study of glycoproteins.
研究领域:
材料科学
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生物化学
·
分析化学
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产品关联
DOI
高影响因子
Energy Storage Materials
·
2025
·
IF 20.2
Siyu Fang,Tiansheng Bai,Jialin Liao,Shuai Zhang,Jiaxian Wang,Funian Mo,Wei Zhai,Zhenglin Hu,Jingyu Lu,Kwun Nam Hui,Lijie Ci,Deping Li
Lithium metal anodes hold the potential for high-energy-density batteries due to their substantial theoretical capacity, but their practical application is hindered by issues such as dendrite growth, poor cycling stability, and safety concerns. This study presents the development of a three-dimensional Li-Si composite alloy anode (Ag@Cu@Li-Si), combining a porous copper scaffold with a lithiophilic silver (Ag) layer and a lithium-silicon (Li-Si) alloy. The Ag@Cu@Li-Si composite demonstrates significant improvements in dendrite suppression, cycling stability, and electrochemical performance. The composite anode exhibits a critical current density of 15 mA cm −2 and over 900 hours of stable operation at 1.0 mA cm −2 in symmetric cells. When integrated into a full cell with a commercial LiFePO 4 cathode, it maintains excellent cycling stability, delivering over 600 cycles with a rate capability of 1.0 C. This study provides valuable insights into the design of lithium metal anodes, highlighting the importance of lithiophilic materials and 3D frameworks for high-performance lithium-metal batteries.
研究领域:
储能
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材料科学
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电化学
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纳米技术
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电池技术
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产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2017
·
IF 7.504
Qing-Shan Liu,Ran Deng,Qing-Fang Yan,Lin Cheng,Yongming Luo,Keqin Li,Xiaoying Yin,Xiaoyan Qin
In order to efficiently screen and isolate β-tubulin inhibitors, β-tubulin was immobilized on core–shell PMMA/CS (poly(methyl methacrylate)/Chitosan) nanoparticles to produce a new type of immobilized affinity material named β-tubulin-immobilized nanoparticles (β-TIN). The selectivity and adsorption performance of β-TIN were characterized using various control drugs. The β-TIN, the paclitaxel molecularly imprinted ploymers (MIP), and the C18 adsorbing material were compared for selectivity and enrichment ratio. Microtubule-targeting antitumor compounds were screened and isolated from a typical Chinese medicine, Chloranthus multistachys, by β-TIN. Three active compounds (curcolnol, zedoarofuran, and codonolactone) in Chloranthus multistachys extract were captured successfully. Microscale thermophoresis demonstrated that these three compounds strongly bind to β-tubulin, and the dissociation constants (Kd) between the three active compounds and β-tubulin were 1820 ± 0.68 nM, 1640 ± 0.52 nM, and 284 ± 1.00 nM, respectively. Moreover, the binding affinity between codonolactone and β-tubulin was greater than that between paclitaxel and β-tubulin. The antitumor activities of the three compounds were confirmed by the microtubule inhibition model, and the results showed a similar antitumor mechanism as paclitaxel. Molecular dynamics simulations were performed to preliminarily investigate the potential binding sites and the structure–activity relationship between the three active molecules and β-tubulin. Our study is the first to report the use of this novel material which is highly efficient in capturing low-content β-tubulin inhibitors from a complex mixture. The three screened compounds exhibited potential antineoplastic activity, and these lead compounds utilize a new mechanism of action with promising development prospects. Because β-TIN is easily prepared, displays excellent adsorption and selectivity for targets, and can effectively maintain the steric conformation and activities of target proteins, it will be very useful in the screening of lead compounds for different drug target proteins.
研究领域:
药学
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纳米技术
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生物技术
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癌症研究
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药物发现
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产品关联
DOI
PubMed
高影响因子
ACS Applied Materials & Interfaces
·
2021
·
IF 9.229
Xue Ma,Jinghua Zhang,Chong Zhang,Xiaoqing Yang,Ajuan Yu,Yanjie Huang,Shusheng Zhang,Gangfeng Ouyang
Aminothiols are closely related to chronic kidney disease, but little is known regarding levels of related aminothiols in the urine of immunoglobulin A vasculitis with nephritis (IgAVN) patients. Herein, a well-defined core–shell Zr-based metal–organic framework (Zr-MOF) composite SiO2@50Benz-Cys was constructed as a mercury ion affinity material via a solvent-assisted ligand exchange strategy for the selective extraction and enrichment of low-concentration aminothiols in IgAVN patient urine. SiO2@50Benz-Cys was competent to enrich the total glutathione (GSH) and total homocysteine (Hcy) in virtue of the excellent affinity after chelation with mercury ions. The extraction efficiencies were closely related to the pH, dithiothreitol amount, and the dose of functional Zr-MOF. Coupled with HPLC–MS/MS in optimized conditions, GSH and Hcy were determined with low detection limits of 0.5 and 1 nmol L–1, respectively. The recoveries of GSH and Hcy for the urine sample at three spiked levels were in the range of 85.3–105% and 79.5–103%, which showed good precision and accuracy. Benefiting from the matrix interference elimination in the process of extraction, the simultaneous detection of aminothiols in the urine of the healthy group and immunoglobulin A vasculitis (IgAV) and IgAVN patients was successfully carried out, suggesting that the Zr-MOF and the robust method together provided a potential application in the analysis of urinary biomolecules. The analysis of variance (ANOVA) showed that the levels of GSH and Hcy had significant differences between the patients and the control. This work is very valuable as it provides a better understanding of concentration alterations of GSH and Hcy in urine involved with IgAVN for clinical research.
研究领域:
分析化学
·
临床化学
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肾病学
·
生物标志物分析
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产品关联
DOI
PubMed
高影响因子
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