Channel-Splitting Photoassisted Enzyme Biofuel Cells: A High-Confluent and Self-Powered Platform for Electrochemistry-Photoelectrochemistry-Coupled Ratiometric Bioassays.

IF 6.7 1区化学 Q1 CHEMISTRY, ANALYTICAL

Analytical Chemistry Pub Date : 2025-10-23 DOI:10.1021/acs.analchem.5c04991

Cui Wang,Yang Lei,Zhuo Xing,Qihan Sun,Xuefei Zhang,Rong-Bin Song,Zhaohui Li

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引用次数: 0

Abstract

The integration of photoelectrochemical (PEC) and electrochemical (EC) signals is attractive for ratiometric EC bioassays. However, their different signal acquisition patterns will bring additional deviations and different magnitude values for weakening the self-calibration reliability. Herein, we present a photoassisted enzyme biofuel cell (PA-EBFC) as the self-powered and high-confluent system for PEC-EC-coupled ratiometric bioassays. The target can trigger the introduction of Au nanoparticle-decorated TiO2 nanospheres (TiO2@Au NSs) onto an anode, which can provide steric hindrance for suppressing the glucose oxidation over Au nanobowls while endowing photoresponsive ability. Moreover, the contributions of photoresponsive ability and steric hindrance to the open-circuit voltage (EOCV) of PA-EBFC have been counteracted by optimizing the Au content of TiO2@Au NSs, generating a constant EOCV under illumination (ElightOCV) and a target-related decrease in EOCV without illumination (EdarkOCV). Using microRNA-486-5p (miR-486-5p) as a model analyte, the entropy-driven DNA circuit has also been integrated for improving the sensitivity. The developed platform has displayed a good negative correlation between the EdarkOCV/ElightOCV and the logarithm of miR-486-5p concentration, along with a limited detection of 0.48 fM. This study demonstrates that splitting the nonillumination to illumination channels of PA-EBFC could be a promising strategy to upgrade EC-PEC-coupled ratiometric assays.

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通道分裂光辅助酶生物燃料电池：电化学-光电化学-耦合比率生物测定的高融合和自供电平台。

光电化学（PEC）和电化学（EC）信号的集成对比率电化学生物测定具有吸引力。然而，它们不同的信号采集方式会带来额外的偏差和不同幅度的值，从而削弱了自校准的可靠性。在此，我们提出了一种光辅助酶生物燃料电池（PA-EBFC）作为自供电和高汇合系统，用于pec - ec偶联的比例生物测定。该目标可以触发在阳极上引入金纳米粒子修饰的TiO2纳米球（TiO2@Au NSs），该纳米球可以提供空间位阻来抑制金纳米碗上的葡萄糖氧化，同时赋予光响应能力。此外，通过优化TiO2@Au NSs的Au含量，可以抵消PA-EBFC的光响应能力和空间位阻对开路电压（EOCV）的影响，在光照下产生恒定的EOCV (ElightOCV)，而在没有光照的情况下产生与靶标相关的EOCV降低（EdarkOCV）。使用microRNA-486-5p （miR-486-5p）作为模型分析物，熵驱动的DNA电路也被集成以提高灵敏度。开发的平台显示EdarkOCV/ElightOCV与miR-486-5p浓度的对数呈良好的负相关，并且检测到0.48 fM的有限。该研究表明，将PA-EBFC的非照明通道拆分为照明通道可能是升级ec - pec耦合比率测定的一种有前途的策略。

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

Analytical Chemistry 化学-分析化学

CiteScore

12.10

自引率

12.20%

发文量

1949

审稿时长

1.4 months

期刊介绍： Analytical Chemistry, a peer-reviewed research journal, focuses on disseminating new and original knowledge across all branches of analytical chemistry. Fundamental articles may explore general principles of chemical measurement science and need not directly address existing or potential analytical methodology. They can be entirely theoretical or report experimental results. Contributions may cover various phases of analytical operations, including sampling, bioanalysis, electrochemistry, mass spectrometry, microscale and nanoscale systems, environmental analysis, separations, spectroscopy, chemical reactions and selectivity, instrumentation, imaging, surface analysis, and data processing. Papers discussing known analytical methods should present a significant, original application of the method, a notable improvement, or results on an important analyte.