Microcrystalline Cellulose-Infused Additive Manufactured Filaments: A Sustainable Path to Enhancing Electrochemical Sensors

Ferreira, Bruno, Bernalte, Elena ORCID: https://orcid.org/0000-0002-0764-789X, Crapnell, Robert D ORCID: https://orcid.org/0000-0002-8701-3933, Augusto, Karen KL, Lomesh, Uday, Khan, Muhzamil A ORCID: https://orcid.org/0009-0001-3960-9310, Fatibello-Filho, Orlando, Paixão, Thiago RLC ORCID: https://orcid.org/0000-0003-0375-4513 and Banks, Craig E ORCID: https://orcid.org/0000-0002-0756-9764 (2025) Microcrystalline Cellulose-Infused Additive Manufactured Filaments: A Sustainable Path to Enhancing Electrochemical Sensors. ACS Applied Engineering Materials, 3 (6). pp. 1759-1769. ISSN 2771-9545

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Abstract

Additive manufacturing is an inherently low-waste manufacturing technology and the development of printable materials in a sustainable way is vital for the method to thrive and align with the United Nations Sustainable Development Goals. This study advances the field of additive manufacturing electrochemistry by uniquely producing an electrically conductive printable material, improving both sustainability and electrochemical performance. Through the innovative combination of microcrystalline cellulose, carbon black, biobased castor oil and recycled poly(lactic acid), a highly conductive, printable filament was produced. The incorporation of microcrystalline cellulose reduces the plastic content of the filament by 10 wt % while demonstrating a reduced resistance, making this filament a promising candidate for various applications that require conductivity. The additively manufactured electrodes with microcrystalline cellulose were electrochemically benchmarked against other additively manufactured electrodes without microcrystalline cellulose. The microcrystalline cellulose filament (20 wt % carbon black/10 wt % microcrystalline cellulose/10 wt % castor oil/60 wt % recycled poly(lactic acid)) produced a heterogeneous rate constant (kobs0) of 0.35 (±0.03) × 10–3 cm s–1 and a charge transfer resistance (Rct) of 207 ± 32 Ω, compared to kobs0 of 0.27 (±0.03) × 10–3 cm s–1 and Rct = 579 ± 32 Ω for the filament with no microcrystalline cellulose added. The microcrystalline cellulose filament was successfully used to create an eco-friendly electroanalytical sensing platform to detect dopamine, obtaining good values of linearity, ranging from 0.01 to 1 μM, a sensitivity of 7.943 μA μM–1, and a limit of detection (LOD) and quantification (LOQ) of 3 and 10 nM, respectively, before successfully being applied within a spiked human serum sample, obtaining recoveries of 102.4%. Overall, this work marks a significant advancement in the development of eco-friendly materials for additive manufacturing, contributing both to improved technological performance and the sustainability of the additive manufacturing industry.