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含硫化铜纳米颗粒的石墨烯混合太赫兹超表面对菌血症的快速早期检测及原位消除

Rapid and Early Detection of Bacteremia and In Situ Elimination by Graphene Hybrid Terahertz Metasurfaces with CuS Nanoparticles.

作者信息

Ma Jiali, Wang Junju, He Hong, Ling Fang, Huang Yingzhou, Wu Xiaoxiao, Li Shunbo, Xu Yi, Wang Li, Yang Xiang

机构信息

Key Laboratory of Optoelectronic Technology and Systems (Ministry of Education), School of Optoelectronics Engineering, Chongqing University, Chongqing 40133l, China.

Chongqing Key Laboratory of Interface Physics in Energy Conversion, College of Physics, Chongqing University, Chongqing 400044, China.

出版信息

ACS Nano. 2025 Aug 12;19(31):28588-28601. doi: 10.1021/acsnano.5c07889. Epub 2025 Aug 1.

DOI:10.1021/acsnano.5c07889
PMID:40749043
Abstract

Currently, clinical culture methods for bacterial detection suffer from a long detection time and low sensitivity, which are insufficient to satisfy the requirements for rapid diagnosis of bacteremia. Here, we fabricated terahertz metal-graphene hybrid metasurfaces (THz MGHM) coupled with polyethylenimine-modified CuS nanoparticles (PEI@CuS NPs) for ultrasensitive detection and in situ inactivation of pathogenic bacteria. To obtain a strong light localization effect based on the bound state in the continuum (BIC), the MGHM consists of a symmetry-broken complementary metal elliptical hole array and a monolayer of graphene covering the surface. Both experimental and simulation approaches were employed to investigate the feasibility and enhancement mechanisms of PEI@CuS NPs in MGHM biosensing. The intense electron transfer between the PEI@CuS NPs and MGHM triggered obvious changes in the graphene's conductivity, which led to a significant change in the quasi-BIC (QBIC) resonance. With the assistance of this THz signal amplifier, the boronic-acid-group-functionalized MGHM was embedded into a poly(methylpentene) (TPX) microfluidic device, which achieved selective capture and sensitive detection of bacteria with limits of detection (LODs) between 11 and 14 CFU/mL for different species. Subsequently, the system accomplished in situ inactivation of bacteria through the synergistic effect of the dual photothermal effect and the generation of reactive oxygen species (ROS). Notably, the THz MGHM platform exhibited time-to-positivity (TTP) for bacteremia patients earlier than traditional blood culture did by an average of 5 h and enabled timely sterilization, which provides a strategy for rapid warning of bacteremia and prevention of dissemination risk for potential clinical applications.

摘要

目前,用于细菌检测的临床培养方法存在检测时间长和灵敏度低的问题,不足以满足菌血症快速诊断的要求。在此,我们制备了太赫兹金属-石墨烯混合超表面(THz MGHM),并将其与聚乙烯亚胺修饰的硫化铜纳米颗粒(PEI@CuS NPs)相结合,用于病原菌的超灵敏检测和原位灭活。为了基于连续统中的束缚态(BIC)获得强烈的光局域化效应,MGHM由一个对称破缺的互补金属椭圆孔阵列和覆盖在表面的单层石墨烯组成。采用实验和模拟方法研究了PEI@CuS NPs在MGHM生物传感中的可行性和增强机制。PEI@CuS NPs与MGHM之间强烈的电子转移引发了石墨烯电导率的明显变化,进而导致准BIC(QBIC)共振发生显著变化。借助这种太赫兹信号放大器,将硼酸基团功能化的MGHM嵌入聚(甲基戊烯)(TPX)微流控装置中,实现了对细菌的选择性捕获和灵敏检测,不同菌种的检测限(LOD)在11至14 CFU/mL之间。随后,该系统通过双光热效应和活性氧(ROS)生成的协同作用实现了细菌的原位灭活。值得注意的是,THz MGHM平台对菌血症患者的阳性检测时间(TTP)比传统血培养平均早5小时,并能及时杀菌,为菌血症的快速预警和预防潜在临床应用中的传播风险提供了一种策略。

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