Recycling 3D Printed Residues for the Development of Disposable Paper-Based Electrochemical Sensors

ACS Appl Mater Interfaces. 2023 Mar 8. doi: 10.1021/acsami.3c00370. Online ahead of print.

Abstract

Here, we propose a recyclable approach using acrylonitrile-butadiene-styrene (ABS) residues from additive manufacturing in combination with low-cost and accessible graphite flakes as a novel and potential mixture for creating a conductive paste. The graphite particles were successfully incorporated in the recycled thermoplastic composite when solubilized with acetone and the mixture demonstrated greater adherence to different substrates, among which cellulose-based material made possible the construction of a paper-based electrochemical sensor (PES). The morphological, structural, and electrochemical characterizations of the recycled electrode material were demonstrated to be similar to those of the traditional carbon-based surfaces. Faradaic responses based on redox probe activity ([Fe(CN)6]3-/4-) exhibited well-defined peak currents and diffusional mass transfer as a quasi-reversible system (96 ± 5 mV) with a fast heterogeneous rate constant value of 2 × 10-3 cm s-1. To improve the electrode electrochemical properties, both the PES and the classical 3D-printed electrode surfaces were modified with a combination of multiwalled carbon nanotubes (MWCNTs), graphene oxide (GO), and copper. Both electrode surfaces demonstrated the suitable oxidation of nitrite at 0.6 and 0.5 V vs Ag, respectively. The calculated analytical sensitivities for PES and 3D-printed electrodes were 0.005 and 0.002 μA/(μmol L-1), respectively. The proposed PES was applied for the indirect amperometric analysis of S-nitroso-cysteine (CysNO) in serum samples via nitrite quantitation, demonstrating a limit of detection of 4.1 μmol L-1, with statistically similar values when compared to quantitative analysis of the same samples by spectrophotometry (paired t test, 95% confidence limit). The evaluated electroanalytical approach exhibited linear behavior for nitrite in the concentration range between 10 and 125 μmol L-1, which is suitable for realizing clinical diagnosis involving Parkinson's disease, for example. This proof of concept shows the great promise of this recyclable strategy combining ABS residues and conductive particles in the context of green chemical protocols for constructing disposable sensors.

Keywords: 3D printing; S-nitroso-cysteine; carbon-based electrodes; complex thermoplastic waste; green chemical principles; stencil printing.