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基于微观-宏观 SERS 策略的痕量分子检测高灵敏度纸基微流控芯片

Micro-macro SERS strategy for highly sensitive paper cartridge with trace-level molecular detection.

机构信息

School of Life Science and Technology, Xidian University, Xi'an, Shaanxi, 710126, China.

School of Life Science and Technology, Xidian University, Xi'an, Shaanxi, 710126, China; School of Mathematics and Physics, Hebei University of Engineering, Handan, Hebei, 056038, China; Xi'an Intelligent Precision Diagnosis and Treatment International Science and Technology Cooperation Base, Xidian University, Xi'an, Shaanxi, 710126, China.

出版信息

Biosens Bioelectron. 2024 Nov 15;264:116665. doi: 10.1016/j.bios.2024.116665. Epub 2024 Aug 12.

DOI:10.1016/j.bios.2024.116665
PMID:39173336
Abstract

Surface-enhanced Raman Scattering (SERS) has become a powerful spectroscopic technology for highly sensitive detection. However, SERS is still limited in the lab because it either requires complicated preparation or is limited to specific compounds, causing poor applicability for practical applications. Herein, a micro-macro SERS strategy, synergizing polymer-assisted printed process with paper-tip enrichment process, is proposed to fabricate highly sensitive paper cartridges for sensitive practical applications. The polymer-assisted printed process finely aggregates nanoparticles with a discrete degree of 1.77, and SERS results are matched with theoretical enhancement, indicating small cluster-dominated hotspots at the micro-scale and thus 41-fold SERS increase compared to other aggregation methods. The paper-tip enrichment process moves molecules in a fluid into small tips filled with plasmonic clusters, and molecular localization at hotspots is achieved by the simulation and optimization of fluidic velocity at the macro-scale, generating a 39.5-fold SERS sensibility increase in comparison with other flow methods. A highly sensitive paper cartridge contains a paper-tip and a 3D-printed cartridge, which is simple, easy-to-operate, and costs around 2 US dollars. With a detection limit of 10  M for probe molecules, the application of real samples and multiple analytes achieves single-molecule level sensitivity and reliable repeatability with a 30-min standardized procedure. The micro-macro SERS strategy demonstrates its potential in practical applications that require point-of-care detection.

摘要

表面增强拉曼散射(SERS)已成为一种用于高灵敏度检测的强大光谱技术。然而,SERS 在实验室中仍然受到限制,因为它要么需要复杂的制备,要么仅限于特定的化合物,导致实际应用的适用性较差。在此,提出了一种微-宏 SERS 策略,将聚合物辅助印刷工艺与纸尖富集工艺相结合,用于制造用于敏感实际应用的高灵敏度纸匣。聚合物辅助印刷工艺精细地聚集纳米颗粒,离散度为 1.77,并且 SERS 结果与理论增强相匹配,表明在微尺度上存在以小团簇为主的热点,与其他聚集方法相比,SERS 增强了 41 倍。纸尖富集工艺将流体中的分子移动到充满等离子体簇的小尖端中,通过对宏观尺度上流体速度的模拟和优化,实现分子在热点处的定位,与其他流动方法相比,SERS 灵敏度提高了 39.5 倍。一个高灵敏度的纸匣包含一个纸尖和一个 3D 打印的匣,它简单、易于操作,成本约为 2 美元。对于探针分子,检测限为 10  M,应用于真实样品和多种分析物,在 30 分钟的标准化程序下实现了单分子级别的灵敏度和可靠的可重复性。微-宏 SERS 策略在需要即时检测的实际应用中显示出了其潜力。

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