Polymers
·
2022
·Vol. 14
·期 19
·4133
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IF 4.967
Lianming Zhang,Kui Luo,Jingxia Gao,Jianping Li
A new chiral molecularly imprinted polymer (MIP) sensor with dual recognition ability was developed for the highly selective separation of enantiomers with toxic side effects in drugs. The sensor contains double-stranded deoxyribonucleic acid (dsDNA) as the element that immobilizes the chiral molecular conformation: the dsDNA enables the imprinted cavities to match the three-dimensional structure and functional groups from the chiral molecule. By embedding the spatial orientation of dsDNA in MIPs, one can accurately capture and immobilize the molecular conformation, eliminating the influence of interfering analogues. Herein, L-penicillamine (L-Pen) was selected as the chiral template molecule and embedded into dsDNA to form dsDNA-L-Pen complex, which was then embedded into the MIPs by electropolymerization. After elution, the stereo-selective imprinted cavities were obtained. The ATATATATATAT-TATATATATATA base sequence showed a high affinity for the embedded L-Pen, which endowed the imprinted cavities with a larger number of sites and improved the selectivity toward Pen enantiomers. Under the optimal working conditions, the current response of the MIP/dsDNA sensor exhibited a positive linear relationship with the logarithm of the L-Pen concentration in the range of 3.0 × 10−16to 3.0 × 10−13mol/L, and the detection limit was 2.48 × 10−16mol/L. After the introduction of dsDNA into the MIP, the selectivity of the sensor toward D-Pen increased by 6.4 times, and the sensor was successfully applied in the analysis of L-Pen in penicillamine tablets.Keywords:molecularly imprint;sensor;dsDNA;chiral;L-Pen
研究领域:
分析化学
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生物医学工程
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PubMed
高影响因子
Analytical Methods
·
2018
·Vol. 10
·期 19
·2263-2271
·
IF 2.073
Yunmei Huang,Jidong Yang,Haiyan Yuan,Yuan Guo,Xiaoqing Zeng,Jiawei Cheng,Yuhui Zhang
D-Penicillamine (D-PA), as the dominant enantiomer, is usually used in many clinical drugs, but the other enantiomer, L-penicillamine (L-PA) is a toxic enantiomer. Therefore, it is of great significance to analyze and detect L-PA in biomedical or environmental samples. CdTe quantum dots (CdTe QDs) were modified by N-acetyl-L-cysteine (NALC) as novel fluorescent probes and were successfully utilized for the determination of L-penicillamine. The fluorescence of the CdTe QDs decreased significantly in the presence of cupric ions (Cu2+) due to the binding of Cu2+ to NALC on the surface of the CdTe QDs, but the addition of L-PA immediately resulted in efficient fluorescence recovery of the modulated CdTe QDs. The experimental results showed that the pH of the buffer solution and the concentration of Cu2+ affected the fluorescence intensity upon adding L-PA. Under the optimum conditions, the recovered fluorescence intensity was linearly proportional to the increasing L-PA concentration in the range of 2 × 10−7 to 4 × 10−6 mol L−1, with correlation coefficient R2 = 0.9980. So, a new, simple and rapid method for the determination of L-PA has been developed and its potential has been demonstrated in human serum samples and environmental samples with satisfactory results.
研究领域:
分析化学
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生物医学
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环境科学
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高影响因子
JOURNAL OF HAZARDOUS MATERIALS
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2022
·
IF 14.224
Jiajia Lian,Pei Liu,Qingyun Liu
Realizing the high value-added utilization of cheap minerals in environmental catalysis has important practical significance. Herein, four nano-scale minerals, namely halloysite (Hal) nanotubes , palygorskite (Pal) nanorods , and montmorillonite (Mon) and hydrotalcite (LDH) nanosheets , were selected for in-situ supporting CeO 2 nanoparticles (NPs) by a facile one-pot hydrothermal method. Among various nanocomposites (NCs), CeO 2 /Pal behaves the highest peroxidase-like activity, attributing to larger surface area for uniformly dispersing CeO 2 NPs and more exposed active oxygen vacancy (O vac ) defects. A novel off-on colorimetric strategy was constructed for detecting toxic L -penicillamine (LPA) and Cu 2+ ion with limit of detections (LODs) of 8.37 and 9.80 μM, respectively. Density functional theory (DFT) calculations show that the O vac defect on CeO 2 (111) surface can catalyze the heterolytic cleavage of H 2 O 2 into H 2 O and oxygen radical (•O), instead of being two hydroxyl radicals (•OH) on clean surface. It can also act as trapping site for O 2 and H 2 O adsorption, improving the oxygen affinity and hydrophilicity of CeO 2 /Pal. This study provides a feasible strategy for designing mineral-based nanozymes and an insight into the possible catalytic mechanism.
研究领域:
环境催化
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材料科学
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生物分析化学
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PubMed
高影响因子
SCIENCE OF THE TOTAL ENVIRONMENT
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2022
·
IF 10.753
Kangling Tang,Yu Chen,Sisi Tang,Xiaodan Wu,Pengfei Zhao,Jinli Fu,Huibin Lei,Zhaoxia Yang,Zhaohui Zhang
Establishment of a rapid, sensitive, visual, accurate and low-cost fluorescence detection system to detect multiple targets was of great significance in food safety evaluation, ecological environment monitoring and human health monitoring. In this work, a smartphone-assisted down/up-conversion dual-mode ratiometric fluorescence sensor was proposed based on metal-organic framework (NH 2 -MIL-101(Fe)) and CdTe quantum dots (CdTe QDs) for visual detection of mercury ions (Hg 2+ ) and L-penicillamine (L-PA), in which NH 2 -MIL-101(Fe) was used as the reference signal and CdTe QDs was used as the response signal. The down-conversion fluorescence system at excitation wavelength of 300 nm (ex: 330 nm) was used to detect Hg 2+ and L-PA, in which the detection limit of Hg 2+ was 0.053 nM with the fluorescence color changed from green to blue, and the detection limit of L-PA was 1.10 nM with the fluorescence color changed from blue to green. Meanwhile, the up-conversion fluorescence system at excitation wavelength of 700 nm (ex: 700 nm) was used to detect Hg 2+ and L-PA. The detection limits of Hg 2+ and L-PA were 0.11 nM and 2.93 nM, respectively. The detection of Hg 2+ and L-PA were also carried out based on the color extraction RGB values identified by the smartphone with a detection limit of 0.091 nM for Hg 2+ and 8.97 nM for L-PA. In addition, the concentrations of Hg 2+ and L-PA were evaluated by three-dimensional dynamic analysis in complex environments. The smartphone-assisted down/up-conversion dual-mode ratiometric fluorescence sensor system provides a new strategy for detection Hg 2+ and L-PA in food safety evaluation, environmental monitoring and human health monitoring.
研究领域:
食品安全评价
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环境监测
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人类健康监测
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生物传感技术
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PubMed
高影响因子
ANALYTICAL CHEMISTRY
·
2024
·
IF 6.7
Xuwen Gao,Zhijian Tian,Xiaoxuan Ren,Yaojia Ai,Bin Zhang,Guizheng Zou
The commercialized electrochemiluminescence (ECL) immunoassay is carried out by holding luminophore Ru(bpy)32+ at a given potential. Designing an electrochemiluminophore with a narrow triggering potential window is strongly anticipated to decrease the electrochemical cross-talk and improve the flux of the commercialized ECL immunoassay in a potential-resolved way. Herein, L-penicillamine-capped silver nanoclusters (LPA-AgNCs) are facilely synthesized and utilized as tags to perform the ECL immunoassay with a sole and narrow triggering potential window of 0.24 V by employing hydrazine (N2H4) as a coreactant. The maximum ECL emission of the LPA-AgNCs/N2H4 system is located ca. +1.27 V. Upon immobilizing LPA-AgNCs onto the electrode surface via forming a sandwich immunocomplex, the ECL of LPA-AgNCs/N2H4 can be utilized to sensitively and selectively determine human carcinoembryonic antigen from 0.5 to 1000 pg/mL with a low limit of detection of 0.1 pg/mL (S/N = 3). This work might open a way to screen electrochemiluminophores for the multiple ECL immunoassay in a potential-resolved way.
研究领域:
分析化学
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生物化学
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生物医学工程
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高影响因子
SENSORS AND ACTUATORS B-CHEMICAL
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2021
·
IF 7.46
Qian Han,Cun Wang,Pingkun Liu,Gui Zhang,Li Song,Yingzi Fu
Since the sensing methods in drug detection are commonly hampered by signal capacity limitations and sole analysis information, dual-mode sensors with high accuracy and flexibility have become more popular. Herein, we present a two-dimensional porphyrin-based metal-organic framework (ZnTCPP MOF) as a unique electrochemiluminescent (ECL) and electrochemical (EC) dual-signal indicator, combined with L-penicillamine-capped Au nanoparticles (L-Pen-Au NPs) as a specific selector, to construct an innovative dual-mode drug sensing platform. Inspired by the optical and electrocatalytic activity of 5,10,15,20-tetrakis-(4-carboxyphenyl)porphyrin (TCPP), a series of ZnTCPP MOFs have been synthesized through a facile bottom-up method. Among them, the “oval-like” ZnTCPP MOF generates higher ECL responses than TCPP monomer when acting as a near-infrared luminophore and outputs stronger EC signals when acting as a redox active probe. In addition, the ZnTCPP MOF, when employed as a nanocarrier, can load many L - Pen-Au NPs. Using L-Pen-Au NPs as selectors, synergistically enhanced dual-mode sensors for detection of the anti-inflammatory drug S-naproxen (S-NAP) exhibit versatile and superior performance and a wide linear range with an ultralow limit of detection. We believe that the applications of this dual-mode sensor can be readily expanded to become a universal platform for sensitive detection of different types of drugs by changing the selector.
研究领域:
分析化学
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材料科学
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生物医学工程
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DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
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2021
·
IF 10.588
Yan Zhang,Hai-Yan Wang,Xi-Wen He,Wen-You Li,Yu-Kui Zhang
In this work, we innovatively synthesized homochiral fluorescence nano molecularly imprinted polymers (D-MIP) with dual affinity (metal ion affinity and homochiral affinity) for the specific separation and detection of L-penicillamine (L-PA), which is a core-shell structure with a SiO 2 -covered CDs core and an imprinted layer with L-PA cavities. A switch for fluorescence response was built by chelating grafted Cu 2+ , what's more, the imprinted L-PA was pre immobilized by Cu 2+ to form the directional imprinting with predetermined spatial structure. More importantly, the homochiral affinity of D-galactose in homochiral molecularly imprinted polymers (D-MIP) greatly enhanced the selective adsorption of L-PA, and D-MIP showed a high selectivity factor (α) of 3.45, which is 1.9 times that of the non-homochiral molecularly imprinted polymers (MIP). Meanwhile, D-MIP exhibited a high enantiomeric excess (ee) value of 56% for separation of racemic PA. Additionally, a high sensitive and selective method was established for the detection of L-PA.
研究领域:
材料科学
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分析化学
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纳米技术
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生物技术
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DOI
高影响因子
SENSORS AND ACTUATORS B-CHEMICAL
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2022
·
IF 9.221
Xiao-Fan Wu,Qingmei Ge,Nan Jiang,Mao Liu,Hang Cong,Zhu Tao
Utilizing a novel concept of chiral amplification induced by host-guest interactions, a new macrocyclic compound , benzo[3]uril (BU[3]), was formed in a chiral microenvironment via the encapsulation of L -cysteine∙H + (L-Cys∙H), and the electrochemiluminescence properties of BU[3] were sensibilized with the formation of a supramolecular complex . Based on this principle, an ultra-sensitive chiral electrochemiluminescence sensor was constructed to recognize the enantiomer of penicillamine (PA). This sensor exhibited high selectivity and sensitivity for L -PA compared to other reported values, with a detection limit of 10 -12 mol·L -1 within a linear range of 10 -5 –10 -10 mol·L -1 , and no obvious electrochemiluminescence response to D -PA. The sensor presents high stability, good reproducibility, strong anti-interference ability, and acceptable recovery, which suggests an ability to quantitatively detect L -PA in an aqueous environment.
研究领域:
分析化学
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材料科学
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电化学
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手性和超分子化学
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DOI
高影响因子
ANALYTICA CHIMICA ACTA
·
2021
·
IF 6.558
Shutong Yang,Fangling Wu,Fanzhen Yu,Liancheng Gu,Huanhuan Wang,Yiyi Liu,Yanqiu Chu,Fengyan Wang,Xiang Fang,Chuan-Fan Ding
Penicillamine (Pen) is a common chiral drug that is obtained from penicillin. Between the two enantiomers of Pen, only D-Pen can be used to treat cystinuria and rheumatoid arthritis while L-Pen is toxic. Therefore, it requires great efforts for the research of the rigorous analysis and distinction of the two enantiomers. The non-covalent combination of chiral molecules and chiral selectors (CSs) has been proved as a unique strategy for chiral distinction by ion mobility spectrometry in coupling with -mss spectrometry (IM-MS). Here, we developed a simple method to distinguish D, L-Pen by using special CSs for IM-MS separation. The CSs utilized here include cyclodextrins (CD) and linear chain oligosaccharides plus metal ions . We found that non-covalent complexes [Pen+β-CD + Li] + could be easily formed by electrospray ionization of the mixture of the solution, and the chirality of Pen could be effectively recognized by measuring their mobilities due to the different collision cross collision sections of [D-Pen+β-CD + Li] + and [L-Pen+β-CD + Li] + . A detailed analysis of [Pen+β-CD + Li] + was then conducted by the optical rotation measurements and NMR experiments to reveal their structural differences. Furthermore, DFT calculation showed the differences of molecular conformation between the complexes. The results provide a new powerful method for fast analysis and recognition of chirality of Pen compounds by IM-MS.
研究领域:
分析化学
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质谱
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手性
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药物分析
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PubMed
高影响因子
LANGMUIR
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2023
·
IF 3.9
Jing Fu,Yujin Miao,Di Zhang,Yongjie Zhang,Luyao Meng,Xinrui Ni,Jinglin Shen,Wei Qi
The construction of macroscopic chiral luminescent aggregates with well-defined structures not only contributes to the development of functional materials but also has significant implications for analyzing chiral transfer and amplification in biological systems and self-assembly systems. Meanwhile, achieving water-soluble chiral metal nanoclusters (NCs) with high photoluminescence (PL) intensity through a convenient method remains a challenge. Herein, we reported the enhanced luminescence of gold nanoclusters stabilized by D-/L-penicillamine (D-/L-AuNCs) induced by poly(allylamine hydrochloride) (PAH) through supramolecular self-assembly strategies. FT-IR spectra and zeta potential measurements revealed that supramolecular assembly was driven by the synergistic effect of hydrogen bonds and electrostatic interactions, which effectively limited the intramolecular vibration and rotation of the ligand and reduced nonradiative relaxation, thus improving the luminescence properties of nanoclusters. Interestingly, during the slow solvent evaporation process, chiral entanglement of assemblies was enhanced, forming macroscopic wheat-shaped superstructures. This study enriches the understanding of the self-assembly mechanism of nanoclusters and provides a pathway for constructing NC-based chiroptical materials.
研究领域:
材料科学
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纳米技术
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物理化学
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光学
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PubMed
高影响因子
Science Advances
·
2024
·Vol. 10
·期 42
·
IF 11.7
Jun Zhang,Kai Wu,Xiaoqing Gao,Min Zhang,Xin Zhou,Florian Bertram,Chen Shen,Yunlong Zhou
Chiral structures and functions are essential natural components in biominerals and biological crystals. Chiral molecules direct inorganics through chiral growth of facets or screw dislocation of crystal clusters. As chirality promoters, they initiate an asymmetric hierarchical self-assembly in a quasi-thermodynamic steady state. However, achieving chiral assembly requires a delicate balance between intricate interactions. This complexity causes the roles of achiral-chiral and inorganic components in crystallization to remain ambiguous. Here, we elucidate a definitive mechanism using an achiral-chiral ligand strategy to assemble inorganics into hierarchical, self-organized superstructures. Achiral ligands cluster inorganic building blocks, while chiral ligands impart chiral rotation. Achiral and chiral ligands can flexibly modulate the chirality of superstructures by fully using their competition in coordination chemistry. This dual-ligand strategy offers a versatile framework for engineering chiroptical nanomaterials tailored to optical devices and metamaterials with optical activities across a broad wavelength range, with applications in imaging, detection, catalysis, and sensing.
研究领域:
材料科学
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纳米技术
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化学
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光学
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PubMed
高影响因子
JOURNAL OF CHROMATOGRAPHY A
·
2024
·
IF 3.8
Ting Tao,Yuyu Cao,Liping Zhang,Dayi Xu,Kaiyuan Pang,Yanli Li,Xiaobao Wei,Zengxian Sun
Thiol amino acids, with great physiological significance, are unstable, and have small molecular weights, as well as very low endogenous concentrations. Therefore, to quantitatively and directly analyze them using liquid chromatography-tandem mass spectrometry is difficult. To overcome these problems, we aimed to prepare a thiol-free amino acid plasm matrix as blank sample to reduce the background for the first time. Using compounds with maleimide group that react with classical thiols to generate water-insoluble products. Reducing agents Tris(2-carboxyethyl)phosphine (TCEP) was applied to cooperate with bismaleimide (DM) for elimination of thiol amino acids from plasma 10 min at room temperature and pH 7. Further, the residual TCEP from plasma were removed using an anion exchange resin within 10 min. Methodological validation analysis revealed good performance in linearity, precision, extraction recovery (≥ 82 %), and stability (except oxidized glutathione). This quantitative analysis was successfully applied to blood samples of 9 people in good health. This study provides a foundation for the development of accurate and rigorous quantitative analysis methods targeting thiol amino acids in different body fluids or tissues. Moreover, it paves the way toward realizing several clinical applications.
研究领域:
生物化学
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临床医学
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PubMed
高影响因子
危险品化学品经营许可证（带存储）