Molecular-Sieving Label-Free Surface-Enhanced Raman Spectroscopy for Sensitive Detection of Trace Small-Molecule Biomarkers in Clinical Samples.

IF 11.3 1区化学 Q1 CHEMISTRY, PHYSICAL

ACS Catalysis Pub Date : 2024-09-18 Epub Date: 2024-09-05 DOI:10.1021/acs.nanolett.4c02890

Mingyang Chen, Yangcenzi Xie, Ming Li

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引用次数: 0

Abstract

Small-molecule biomarkers are ubiquitous in biological fluids with pathological implications, but major challenges persist in their quantitative analysis directly in complex clinical samples. Herein, a molecular-sieving label-free surface-enhanced Raman spectroscopy (SERS) biosensor is reported for selective quantitative analysis of trace small-molecule trimetazidine (TMZ) in clinical samples. Our biosensor is fabricated by decorating a superhydrophobic monolayer of microporous metal-organic frameworks (MOF) shell-coated Au nanostar nanoparticles on a silicon substrate. The design strategy principally combines the hydrophobic surface-enabled physical confinement and preconcentration, MOF-assisted molecular enrichment and sieving of small molecules, and sensitive SERS detection. Our biosensor utilizes such a "molecular confinement-and-sieving" strategy to achieve a five orders-of-magnitude dynamic detection range and a limit of detection of ≈0.5 nM for TMZ detection in either urine or whole blood. We further demonstrate the applicability of our biosensing platform for longitudinal label-free SERS detection of the TMZ level directly in clinical samples in a mouse model.

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用于灵敏检测临床样本中痕量小分子生物标记物的无标签分子筛表面增强拉曼光谱。

小分子生物标记物在具有病理影响的生物液体中无处不在，但在复杂的临床样本中直接对其进行定量分析仍面临重大挑战。本文报告了一种分子筛分无标记表面增强拉曼光谱（SERS）生物传感器，用于选择性定量分析临床样本中的痕量小分子曲美他嗪（TMZ）。我们的生物传感器是通过在硅基底上装饰微孔金属有机框架（MOF）外壳包覆金纳米柱纳米粒子的超疏水单层而制成的。设计策略主要结合了疏水表面的物理限制和预浓缩、MOF 辅助的分子富集和小分子筛分以及灵敏的 SERS 检测。我们的生物传感器利用这种 "分子限制和筛分 "策略，在尿液或全血中检测 TMZ 的动态检测范围达到了五个数量级，检测限≈0.5 nM。我们还进一步证明了我们的生物传感平台的适用性，它可以在小鼠模型中直接对临床样本中的 TMZ 水平进行纵向无标记 SERS 检测。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

ACS Catalysis CHEMISTRY, PHYSICAL-

CiteScore

20.80

自引率

6.20%

发文量

1253

审稿时长

1.5 months

期刊介绍： ACS Catalysis is an esteemed journal that publishes original research in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. It offers broad coverage across diverse areas such as life sciences, organometallics and synthesis, photochemistry and electrochemistry, drug discovery and synthesis, materials science, environmental protection, polymer discovery and synthesis, and energy and fuels. The scope of the journal is to showcase innovative work in various aspects of catalysis. This includes new reactions and novel synthetic approaches utilizing known catalysts, the discovery or modification of new catalysts, elucidation of catalytic mechanisms through cutting-edge investigations, practical enhancements of existing processes, as well as conceptual advances in the field. Contributions to ACS Catalysis can encompass both experimental and theoretical research focused on catalytic molecules, macromolecules, and materials that exhibit catalytic turnover.