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Additively Manufactured 3D Micro-bioelectrodes for Enhanced Bioelectrocatalytic Operation

Jodeiri, Keyvan; Foerster, Aleksandra; Trindade, Gustavo F.; Im, Jisun; Carballares, Diego; Fernández-Lafuente, Roberto; Pita, Marcos; De Lacey, Antonio L.; Parmenter, Christopher D; Tuck, Christopher

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Authors

Keyvan Jodeiri

Aleksandra Foerster

Gustavo F. Trindade

Jisun Im

Diego Carballares

Roberto Fernández-Lafuente

Marcos Pita

Antonio L. De Lacey

CHRISTOPHER TUCK CHRISTOPHER.TUCK@NOTTINGHAM.AC.UK
Professor of Materials Engineering



Abstract

The drive toward miniaturization of enzyme-based bioelectronics established a need for three-dimensional (3D) microstructured electrodes, which are difficult to implement using conventional manufacturing processes. Additive manufacturing coupled with electroless metal plating enables the production of 3D conductive microarchitectures with high surface area for potential applications in such devices. However, interfacial delamination between the metal layer and the polymer structure is a major reliability concern, which leads to device performance degradation and eventually device failure. This work demonstrates a method to produce a highly conductive and robust metal layer on a 3D printed polymer microstructure with strong adhesion by introducing an interfacial adhesion layer. Prior to 3D printing, multifunctional acrylate monomers with alkoxysilane (−Si-(OCH3)3) were synthesized via the thiol-Michael addition reaction between pentaerythritol tetraacrylate (PETA) and 3-mercaptopropyltrimethoxysilane (MPTMS) with a 1:1 stoichiometric ratio. Alkoxysilane functionality remains intact during photopolymerization in a projection micro-stereolithography (PμSLA) system and is utilized for the sol-gel reaction with MPTMS during postfunctionalization of the 3D printed microstructure to build an interfacial adhesion layer. This leads to the implementation of abundant thiol functional groups on the surface of the 3D printed microstructure, which can act as a strong binding site for gold during electroless plating to improve interfacial adhesion. The 3D conductive microelectrode prepared by this technique exhibited excellent conductivity of 2.2 × 107 S/m (53% of bulk gold) with strong adhesion between a gold layer and a polymer structure even after harsh sonication and an adhesion tape test. As a proof-of-concept, we examined the 3D gold diamond lattice microelectrode modified with glucose oxidase as a bioanode for a single enzymatic biofuel cell. The lattice-structured enzymatic electrode with high catalytic surface area was able to generate a current density of 2.5 μA/cm2 at 0.35 V, which is an about 10 times increase in current output compared to a cube-shaped microelectrode.

Citation

Jodeiri, K., Foerster, A., Trindade, G. F., Im, J., Carballares, D., Fernández-Lafuente, R., …Tuck, C. (2023). Additively Manufactured 3D Micro-bioelectrodes for Enhanced Bioelectrocatalytic Operation. ACS Applied Materials and Interfaces, 15(11), 14914–14924. https://doi.org/10.1021/acsami.2c20262

Journal Article Type Article
Acceptance Date Mar 2, 2023
Online Publication Date Mar 10, 2023
Publication Date Mar 22, 2023
Deposit Date May 3, 2023
Publicly Available Date Mar 29, 2024
Journal ACS Applied Materials and Interfaces
Print ISSN 1944-8244
Electronic ISSN 1944-8252
Publisher American Chemical Society (ACS)
Peer Reviewed Peer Reviewed
Volume 15
Issue 11
Pages 14914–14924
DOI https://doi.org/10.1021/acsami.2c20262
Keywords 3D printing, Electrodes, Gold, Polymers, Surface interactions
Public URL https://nottingham-repository.worktribe.com/output/18529304
Publisher URL https://pubs.acs.org/doi/10.1021/acsami.2c20262

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