Wearable microneedle-based array patches for continuous electrochemical monitoring and drug delivery: toward a closed-loop system for methotrexate treatment

Marc Parrilla*, Usanee Detamornrat, Juan Domínguez-Robles, Sensu Tunca, Ryan F. Donnelly*, Karolien De Wael*

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

26 Citations (Scopus)

Abstract

Wearable devices based on microneedle (MN) technology have recently emerged as tools for in situ transdermal sensing or delivery in interstitial fluid (ISF). Particularly, MN-based electrochemical sensors allow the continuous monitoring of analytes in a minimally invasive manner through ISF. Exogenous small molecules found in ISF such as therapeutic drugs are ideal candidates for MN sensors due to their correlation with blood levels and their relevance for the optimal management of personalized therapies. Herein, a hollow MN array patch is modified with conductive pastes and functionalized with cross-linked chitosan to develop an MN-based voltammetric sensor for continuous monitoring of methotrexate (MTX). Interestingly, the chitosan coating avoids biofouling while enabling the adsorption of MTX at the electrode’s surface for sensitive analysis. The MN sensor exhibits excellent analytical performance in vitro with protein-enriched artificial ISF and ex vivo under a Franz diffusion cell configuration. The MN sensor shows a linear range from 25 to 400 μM, which fits within the therapeutic range of high-dose MTX treatment for cancer patients and an excellent continuous operation for more than two days. Moreover, an iontophoretic hollow MN array patch is developed with the integration of both the anode and cathode in the single MN array patch. The ex vivo characterization demonstrates the transdermal on-demand drug delivery of MTX. Overall, the combination of both MN patches represents impactful progress in closed-loop systems for therapeutic drug management in disorders such as cancer, rheumatoid arthritis, or psoriasis.
Original languageEnglish
Pages (from-to)4161-4170
Number of pages10
JournalACS Sensors
Volume8
Issue number11
Early online date19 Oct 2023
DOIs
Publication statusPublished - 24 Nov 2023

Keywords

  • Fluid Flow and Transfer Processes
  • Process Chemistry and Technology
  • Instrumentation
  • Bioengineering

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