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高活性刷状纳米碳微电极的电化学微流控多重生物分析。

Electrochemical Microfluidic Multiplexed Bioanalysis by a Highly Active Bottlebrush-like Nanocarbon Microelectrode.

机构信息

Key Laboratory of Material Chemistry for Energy Conversion and Storage, Ministry of Education, School of Chemistry and Chemical Engineering, Huazhong University of Science and Technology, Wuhan 430074, China.

Union Hospital, Tongji Medical College, Huazhong University of Science & Technology, Wuhan 430022, China.

出版信息

Anal Chem. 2022 Mar 15;94(10):4463-4473. doi: 10.1021/acs.analchem.1c05544. Epub 2022 Feb 24.

Abstract

We present a highly efficient multichannel microfluidic electrochemical sensor integrated with an electroactive nanocarbon microelectrode for sensitive and selective detection of multiple biomarkers in different biological samples. Our results have shown that ionic liquid-assisted wet spinning followed by tailored growth of metal-organic frameworks and pyrolysis treatment led to structural and molecular engineering of mechanically robust all-carbon microfibers for excellent electrochemical activities. The flexible bottlebrush-like nanocarbon microelectrode features a "stem" of freestanding N, B-codoped graphene fiber and high-density "bristles" of Co, N-codoped carbon nanotube arrays, leading to promoted electrocatalytic mechanism that has been substantiated by density functional theory calculations. The structural characteristics, high catalytic activities, and favorable biocompatibility of the bottlebrush nanocarbon electrodes provide opportunities for multichannel, microfluidic detection of redox-active biomolecules, including hydrogen sulfide (HS), dopamine (DA), uric acid (UA), and ascorbic acid (AA), and have been applied to on-chip monitoring of HS and DA released from live cancer cells or neuroblastoma cells and DA, UA, and AA in trace amounts of body fluids such as sweat, finger blood, tears, saliva, and urine, which is of great significance for clinical diagnosis and prognosis in point-of-care testing.

摘要

我们提出了一种高效的多通道微流控电化学传感器,该传感器与电活性纳米碳微电极集成在一起,用于在不同的生物样品中灵敏和选择性地检测多种生物标志物。我们的研究结果表明,离子液体辅助湿法纺丝,随后进行金属有机框架的定制生长和热解处理,导致了机械坚固的全碳微纤维的结构和分子工程,从而具有优异的电化学活性。灵活的瓶刷状纳米碳微电极具有独立的 N、B 共掺杂石墨烯纤维“茎”和高密度的 Co、N 共掺杂碳纳米管阵列“刷毛”,从而促进了电催化机制,这已通过密度泛函理论计算得到证实。瓶刷纳米碳电极的结构特征、高催化活性和良好的生物相容性为氧化还原活性生物分子的多通道、微流控检测提供了机会,包括硫化氢 (HS)、多巴胺 (DA)、尿酸 (UA) 和抗坏血酸 (AA),并已应用于从活癌细胞或神经母细胞瘤细胞中释放的 HS 和 DA 以及汗液、指尖血、眼泪、唾液和尿液等微量体液中的 DA、UA 和 AA 的芯片上监测,这对于即时护理测试中的临床诊断和预后具有重要意义。

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