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

IF 9.1 1区材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Nano Letters 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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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。

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来源期刊

Nano Letters 工程技术-材料科学：综合

CiteScore

16.80

自引率

2.80%

发文量

1182

审稿时长

1.4 months

期刊介绍： Nano Letters serves as a dynamic platform for promptly disseminating original results in fundamental, applied, and emerging research across all facets of nanoscience and nanotechnology. A pivotal criterion for inclusion within Nano Letters is the convergence of at least two different areas or disciplines, ensuring a rich interdisciplinary scope. The journal is dedicated to fostering exploration in diverse areas, including: - Experimental and theoretical findings on physical, chemical, and biological phenomena at the nanoscale - Synthesis, characterization, and processing of organic, inorganic, polymer, and hybrid nanomaterials through physical, chemical, and biological methodologies - Modeling and simulation of synthetic, assembly, and interaction processes - Realization of integrated nanostructures and nano-engineered devices exhibiting advanced performance - Applications of nanoscale materials in living and environmental systems Nano Letters is committed to advancing and showcasing groundbreaking research that intersects various domains, fostering innovation and collaboration in the ever-evolving field of nanoscience and nanotechnology.