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<p>Owing to the protease-free and hairpin DNA primers-free design of entropy-powered catalysis (EPC), nanobiosensors constructed from this amplification protocol show promising potential for detecting tumor biomarkers in live biosystems. Nevertheless, EPC’s single-round signal enhancement and perpetual activation during bio-delivery severally restrict its sensitivity and precision in responding to low-concentration analytes. To overcome these&#xa0;restrictions, this study first links together fuel strands produced by two separate EPC modules, thus establishing an ultrasensitive nanobiosensor that implements an exceptional crosslinked bientropy-powered catalysis with more powerful two-round amplification capacity. Following that, one DNA segment is embedded with a photocleavable bond to block the analyte’s recognition site, whereby a near-infrared light (NIR)-regulated strategy facilitated by upconversion luminescence is utilized to precisely activate the biosensing operation. Our conceptual proof is validated by determining&#xa0; microRNA-21, a low-abundance biomarker inclined to be overexpressed in various malignant tumors. In addition to ultra-high sensitivity (with a remarkably low limit of detection of 32.44 fM) and satisfactory specificity (discriminating even single-nucleotide mutations) in buffered environments, this bientropy-powered catalysis crosslinked nanobiosensor enables reliable imaging assays in both live cells and animals, offering a potent toolbox for cancer diagnostics.</p> Graphical Abstract <p></p>

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Bientropy-powered catalysis crosslinked ultrasensitive nanobiosensor for precise NIR light-regulated imaging of tumor biomarkers

  • 期刊论文

  • 发表日期：

    2025年9月26日

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  • Lejing Yao,
  • Xiaoming Sun,
  • Qing Tang,
  • Jingwei Qiu,
  • Da Liu,
  • Cheng-Yu Li

摘要

Owing to the protease-free and hairpin DNA primers-free design of entropy-powered catalysis (EPC), nanobiosensors constructed from this amplification protocol show promising potential for detecting tumor biomarkers in live biosystems. Nevertheless, EPC’s single-round signal enhancement and perpetual activation during bio-delivery severally restrict its sensitivity and precision in responding to low-concentration analytes. To overcome these restrictions, this study first links together fuel strands produced by two separate EPC modules, thus establishing an ultrasensitive nanobiosensor that implements an exceptional crosslinked bientropy-powered catalysis with more powerful two-round amplification capacity. Following that, one DNA segment is embedded with a photocleavable bond to block the analyte’s recognition site, whereby a near-infrared light (NIR)-regulated strategy facilitated by upconversion luminescence is utilized to precisely activate the biosensing operation. Our conceptual proof is validated by determining  microRNA-21, a low-abundance biomarker inclined to be overexpressed in various malignant tumors. In addition to ultra-high sensitivity (with a remarkably low limit of detection of 32.44 fM) and satisfactory specificity (discriminating even single-nucleotide mutations) in buffered environments, this bientropy-powered catalysis crosslinked nanobiosensor enables reliable imaging assays in both live cells and animals, offering a potent toolbox for cancer diagnostics.

Graphical Abstract