The increasing demand for functional materials and an efficient use of sustainable resources makes the search for new material systems an ever growing endeavor. With this respect, architected (meta-)materials attract considerable interest. Their fabrication at the micro- and nanoscale, however, remains a challenge, especially for composites with highly different phases and unmodified reinforcement fillers. This study demonstrates that it is possible to create a non-cytotoxic nanocomposite ink reinforced by a sustainable phase, cellulose nanocrystals (CNCs), to print and tune complex 3D architectures using two-photon polymerization, thus, advancing the state of knowledge toward the microscale. Micro-compression, high-res scanning electron microscopy, (polarised) Raman spectroscopy, and composite modeling are used to study the structure-property relationships. A 100% stiffness increase is observed already at 4.5 wt% CNC while reaching a high photo-polymerization degree of ≈80% for both neat polymers and CNC-composites. Polarized Raman and the Halpin-Tsai composite-model suggest a random CNC orientation within the polymer matrix. The microscale approach can be used to tune arbitrary small scale CNC-reinforced polymer-composites with comparable feature sizes. The new insights pave the way for future applications where the 3D printing of small structures is essential to improve performances of tissue-scaffolds, extend bio-electronics applications or tailor microscale energy-absorption devices.
Keywords: Halpin-Tsai composite model; cellulose nanocrystals (CNCs); degree of conversion; micromechanics; microscale 3D printing (two-photon polymerization); reinforced polymer nanocomposites; sustainable reinforcements.
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