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Selective SERS Identification and Quantification of Glucose Enantiomers on Homochiral MOFs Based Enzyme-Free Nanoreactors

CHEMICAL ENGINEERING JOURNAL(2023)

Northeastern Univ

Cited 8|Views21
Abstract
Enantiomeric identification plays a critical role in diverse fields ranging from pharmaceutics, biologics, and stereoselective synthesis to daily life. In this study, an enantioselective surface-enhanced Raman scattering (SERS) substrate was developed by integrating homochiral MIL-101(Fe) with oxidase (GOx)-mimicking Au nanoparticles (Au/Chiral-MIL-101(Fe)) for identification and quantification of chiral molecules. Using L/D- glucose (Glu) as the model enantiomers, the homochiral environment of Au/Chiral-MIL-101(Fe) exhibited se-lective recognition abilities for Glu enantiomers. The captured Glu was further oxidized to hydrogen peroxide (H2O2) by GOx-like activity of Au nanoparticles. The generated H2O2 molecules reduced Fe(III) nodes in MIL-101 (Fe) to Fe(II) for the growth of Prussian blue (PB) on site. Benefitting from the pre-concentrated feature and confinement effect of the porous metal-organic frameworks (MOFs) structure, the Au/Chiral-MIL-101(Fe) hybrid based nanoreactors exhibited high catalytic performance for H2O2 generation and further PB growth, resulting in an excellent sensitivity for Glu quantification. The enantioselective discrimination between L-Glu and D-Glu was directly determined from the intensity of PB signals at 2150 cm-1. Using this sensing strategy, Glu enantiomers could be quantified with a limit of detection (LOD) of 0.09 mu M for L-Glu and 0.08 mu M for D-Glu. Owing to its enzyme-free nature and universal characteristic for the discrimination of other monosaccharide enantiomers, this design provides an attractive substrate for sensing chiral molecules by Raman technology.
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Key words
surface-enhanced Raman scattering,Metal -organic frameworks,Enantiomeric identification,Nanozyme,Glucose sensing
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要点】:本研究开发了一种手性选择性表面增强拉曼散射(SERS)基底,通过将同手性MIL-101(Fe)与过氧化酶(GOx)模拟的金纳米颗粒(Au/Chiral-MIL-101(Fe))结合,用于识别和量化手性分子,其创新点在于实现了对葡萄糖对映体的选择性识别和量化。

方法】:通过整合手性MIL-101(Fe)和氧化酶模拟的Au纳米颗粒,开发了一种手性选择性SERS基底。

实验】:使用L/D-葡萄糖作为手性模型分子,在Au/Chiral-MIL-101(Fe)上表现出对葡萄糖对映体的选择性识别能力。实验中,L-葡萄糖和D-葡萄糖被分别氧化成过氧化氢(H2O2),然后过氧化氢分子将MIL-101(Fe)中的Fe(III)节点还原为Fe(II),促进了普鲁士蓝(PB)的生长。借助多孔金属有机框架(MOFs)结构的预浓缩特性和限制效应,Au/Chiral-MIL-101(Fe)杂化基底纳米反应器显示出高效催化过氧化氢生成和PB生长的性能,从而实现了对葡萄糖的高灵敏度量化。对L-Glu和D-Glu的对映选择性区分直接由2150 cm-1处PB信号的强度确定。采用这一传感策略,L-Glu和D-Glu的对映体可以分别以0.09 μM和0.08 μM的检测限进行量化。由于其无酶性质和对其他单糖对映体的普遍区分能力,该设计为通过拉曼技术检测手性分子提供了一种有吸引力的基底。