Deep-Learning-Decoded Spatial Electrochemiluminescence from Potentiostat-Free, Button-Battery-Driven Microneedle Arrays for Multiplexed microRNA Imaging

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Abstract
Electrochemiluminescence (ECL) bioassays are essential for rapid intracerebral hemorrhage (ICH) diagnosis, while conventional approaches require bulky instrumentation and complex readout electronics that hinder point-of-care (POC) use. To address this limitation, we developed a battery-driven catalysis-initiated ECL imaging platform for multiplexed detection of ICH-associated microRNAs. The device integrated a gold film-modified copper microneedle array (Au film/Cu MNA), polydimethylsiloxane (PDMS) dual-chamber microcells, and button-battery excitation. Heterogeneous catalysis at the Au film/Cu MNA generated reactive oxygen species (ROS) that amplified ECL and sustained luminescence propagation across 168 μm. A competitive hybridization assay using ferrocene-modified linker DNA (Fc-LDNA) on microneedle tips enabled simultaneous miRNA-126 and miRNA-21 detection with detection limits of 4.6 and 0.8 pM, respectively. A hybrid convolutional neural network (CNN) model decoded spatial emission patterns, extending the linear ranges to 1.28 ∼ 32 fM and 0.59 ∼ 32 fM, beyond those achieved by pixel averaging. Preliminary clinical validation (n = 35 ICH, n = 25 healthy controls) revealed an inverse miRNA expression correlation and dual-target diagnostic accuracy (AUC = 0.993), exceeding single-biomarker performance (miRNA-126: AUC = 0.945; miRNA-21: AUC = 0.964). This strategy advances ECL bioanalysis toward portable, multiplexed biomarker quantification in neurological and inflammatory diseases.
Funding Information
  • Natural Science Foundation of Zhejiang Province (2023R5242)
  • Natural Science Foundation of Zhejiang Province (LY24B050004)
  • National Natural Science Foundation of China (NSFC) (22474128)
  • National Natural Science Foundation of China (NSFC) (22674176)

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