Weerasinghe, U. A., Wu, T., Sugiarto, S., Li, K., Duong, P. K., Li, Z., Hashimoto, M., & Kai, D. (2026). Dual-functional polymerizable deep eutectic solvents for lignocellulose nanofibrillation and 3D printing. Chemical Engineering Journal, 544, 178887. https://doi.org/10.1016/j.cej.2026.178887
Abstract:
Lignocellulosic biomass, composed of natural biopolymers, holds significant potential for sustainable functional materials. However, conventional isolating methods of its constituents such as cellulose nanofibers and lignin often involve harsh chemical treatments and multistep processing. Herein, we introduce a one-pot strategy using a ternary polymerizable deep eutectic solvent (tPDES) system, comprising choline chloride, citric acid, and acrylic acid, to directly convert lignocellulosic biomass (pineapple leaf fibers, PALF) into nanocellulose-based eutectogels with 3D printing capabilities. The tPDES exhibits a dual function, enabling (1) cellulose modification through nanofibrillation and surface functionalization, and (2) UV-induced polymerization, generating stable eutectogels with reduced fiber size (average diameter: < 18 nm) and high crystallinity (91+%). The resulting dual-network structure, formed through dense chemical and physical crosslinks, imparts superior mechanical performance to the eutectogel, including a 9-fold increase in strength. Furthermore, the eutectogel demonstrates distinct multifunctional behaviors such as anti-freezing, self-healing, and strong adhesion, arising from the synergistic interactions within the dual-network matrix. The physical networks of cellulose nanofiber (CNF) facilitate the mechanical reinforcement and rheological performance, essential for direct ink writing (DIW). Moreover, we demonstrate liquid support medium-enabled 3D printing of eutectogels to fabricate tall and overhanging structures with enhanced fidelity. As a proof of concept, the 3D-printed eutectogel is applied as triboelectric nanogenerators (TENG) using various 3D-printed patterns, generating output currents up to 1.23 μA and voltages up to 91.8 V. This approach offers a sustainable and advanced manufacturing route for converting lignocellulosic biomass into functional materials for flexible energy harvesting applications.
License type:
Attribution-NonCommercial-NoDerivatives 4.0 International (CC BY-NC-ND 4.0)
Funding Info:
This research / project is supported by the Agency of Science, Technology and Research - Manufacturing, Trade, and Connectivity Individual Research Grants
Grant Reference no. : M22K2c0085
This research / project is supported by the Agency of Science, Technology and Research - Manufacturing, Trade, and Connectivity Programmatic Fund
Grant Reference no. : M25O2b0016