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<p>The rapid and sensitive detection of biomarkers such as interleukin-6 (IL-6) is crucial for managing sepsis. However, conventional diagnostic assays are often slow and difficult to adapt to rapid decentralized testing. Although microneedle (MN) biosensors offer a promising route toward minimally invasive and potentially point-of-care biomarker detection, challenges related to fabrication, sensitivity, and surface functionalization limit their broader applicability. In this study, we developed a polymer-based nanoporous MN array platform to address these limitations. A 3D printed master mold and a polydimethylsiloxane (PDMS) negative mold were employed to cast a polymer solution containing ethoxylated trimethylolpropane triacrylate (ETPTA) with 2-hydroxy-2-methylpropiophenone (HMPP) and poly(ethylene glycol) (PEG) as a porogen. Nanoporous MN arrays were fabricated with pores of 35 ± 1&#xa0;nm and a surface area of 34.5&#xa0;m²/g using 30% porogen concentration, while maintaining sufficient fracture force (&gt; 0.71&#xa0;N/needle) for reliable skin penetration. Surface amine functionalization was achieved via air plasma activation followed by silanization with 1% (3-aminopropyl)triethoxysilane (APTES) in toluene and subsequent N-(3-dimethylaminopropyl)-N′-ethylcarbodiimide (EDC) / N-hydroxysuccinimide (NHS) coupling, allowing stable antibody conjugation with an N 1s atomic percentage &gt; 4%. In comparison with nonporous MN controls, the nanoporous MN arrays exhibited a 4.5-fold increase in antibody loading capability, and over 95% of the conjugated antibodies remained intact during gelatin phantom insertion for at least 30&#xa0;min. The optimized platform showed a linear response (R² = 0.9834) for IL-6 in the range of 0.5 ~ 100 ng/mL in skin-mimicking phantoms, with a detection limit of 141 pg/mL, and exhibited excellent specificity for IgE, IP-10, and procalcitonin. These results demonstrate that nanoporous surface engineering can enhance antibody immobilization and phantom-based IL-6 sensing performance in polymer MN arrays, supporting their potential as minimally invasive biomarker sensing interfaces.</p>

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Surface engineering of polymer microneedle arrays for enhanced sensitivity

  • 期刊论文

  • 发表日期：

    2026年7月6日

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  • Ju-Hong Yang,
  • Young Ki Hahn

摘要

The rapid and sensitive detection of biomarkers such as interleukin-6 (IL-6) is crucial for managing sepsis. However, conventional diagnostic assays are often slow and difficult to adapt to rapid decentralized testing. Although microneedle (MN) biosensors offer a promising route toward minimally invasive and potentially point-of-care biomarker detection, challenges related to fabrication, sensitivity, and surface functionalization limit their broader applicability. In this study, we developed a polymer-based nanoporous MN array platform to address these limitations. A 3D printed master mold and a polydimethylsiloxane (PDMS) negative mold were employed to cast a polymer solution containing ethoxylated trimethylolpropane triacrylate (ETPTA) with 2-hydroxy-2-methylpropiophenone (HMPP) and poly(ethylene glycol) (PEG) as a porogen. Nanoporous MN arrays were fabricated with pores of 35 ± 1 nm and a surface area of 34.5 m²/g using 30% porogen concentration, while maintaining sufficient fracture force (> 0.71 N/needle) for reliable skin penetration. Surface amine functionalization was achieved via air plasma activation followed by silanization with 1% (3-aminopropyl)triethoxysilane (APTES) in toluene and subsequent N-(3-dimethylaminopropyl)-N′-ethylcarbodiimide (EDC) / N-hydroxysuccinimide (NHS) coupling, allowing stable antibody conjugation with an N 1s atomic percentage > 4%. In comparison with nonporous MN controls, the nanoporous MN arrays exhibited a 4.5-fold increase in antibody loading capability, and over 95% of the conjugated antibodies remained intact during gelatin phantom insertion for at least 30 min. The optimized platform showed a linear response (R² = 0.9834) for IL-6 in the range of 0.5 ~ 100 ng/mL in skin-mimicking phantoms, with a detection limit of 141 pg/mL, and exhibited excellent specificity for IgE, IP-10, and procalcitonin. These results demonstrate that nanoporous surface engineering can enhance antibody immobilization and phantom-based IL-6 sensing performance in polymer MN arrays, supporting their potential as minimally invasive biomarker sensing interfaces.