Printed electronics (PE) have emerged as a rapidly growing technology owing to their potential for low-cost fabrication, flexibility, and scalable device manufacturing. The dependence on fossil-based components raises environmental concerns, leading the scientific community toward sustainable solutions, aiming to reduce the accumulation of electronic waste (e-waste) in the environment and the emission of toxic gases, as well as to offer a circular solution in the sector. This review presents an in-depth overview of biobased polymeric materials in printed and organic (bio-)electronics. Firstly, the principal printing techniques are presented in detail. The review proceeds by outlining the various biobased synthetic and natural polymers, along with their blends, that are employed in the fabrication of biobased substrates for printed devices. Finally, the review emphasizes the existing challenges and constraints in the field of PE, along with the promising opportunities for its future advancement.

A comprehensive investigation was conducted focusing on two series of poly(lactic acid) (PLA)-based nanocomposites filled with small amounts (0.5 and 1.0%) of metal (Ag/Cu) nanoparticles (NPs). Our work aimed to synthesize PLA/Ag nanocomposites via in situ ring-opening polymerization (ROP), and for comparison purposes, the same materials were also prepared via solution casting followed by melt mixing. PLA/Cu nanocomposites were also prepared via melt extrusion. Gel permeation chromatography (GPC) and intrinsic viscosity measurements [η] showed that the incorporation of Ag nanoparticles (AgNPs) resulted in a decrease in the molecular weight of the PLA matrix, indicating a direct effect of the AgNPs on its macromolecular structure. Fourier-transform infrared spectroscopy (FTIR) revealed no significant changes in the characteristic peaks of the nanocomposites, except for an in situ sample containing 1.0 wt% of AgNPs, where slight interactions in the C=O region were detected. Differential scanning calorimetry (DSC) analysis confirmed the semi-crystalline nature of the materials. Glass transition temperature was strongly affected by the presence of NPs in the case of the in situ-based samples. Melt crystallized studies suggested potential indirect polymer–NP interactions, while isothermal melt crystallization experiments confirmed the nucleation ability of the NPs. The mechanical performance was assessed via tensile and flexural measurements, revealing that the in situ-based samples exhibited remarkable flexibility. Moreover, during the three-point bending tests, none of the in situ nanocomposite samples broke. In this context, next-generation PLA-based nanocomposites have been proposed for advanced applications, including flexible printed electronics.

The synthesis of two series of poly(lactic acid) (PLA)-based polymer nanocomposites (PNCs) filled with small amounts (0.5 and 1%) of Ag and Cu nanoparticles (NPs) was performed. Moreover, two methods for the PNC synthesis were performed, namely, ‘conventional mixing techniques’ and ‘in situ ring opening polymerization (ROP)’. The latter method was employed for the first time; moreover, it was found to be more effective in achieving very good NP dispersion in the polymer matrix as well as the formation of interfacial polymer–NP interactions. The in situ ROP for PLA/Cu was not productive due to the oxidation of Cu NPs being faster than the initiation of ROP. The presence of NPs resulted in suppression of the glass transition temperature, T_g (23–60 °C), with the effects being by far stronger in the case of ROP-based PNCs, e.g., exhibiting T_g decrease by tens of K. Due to that surprising result, the ROP-based PLA/Ag PNCs exhibited elevated ionic conductivity phenomena (at room temperature). This can be exploited in specific applications, e.g., mimicking the facilitated small molecules permeation. The effects of NPs on crystallinity (2–39%) were found opposite between the two series. Crystallinity was facilitated/suppressed in the mixing/ROP -based PNCs, respectively. The local and segmental molecular mobility map was constructed for these systems for the first time. Combining the overall data, a concluding scenario was employed, that involved the densification of the polymer close to the NPs’ surface and the free volume increase away from them. Finally, an exceptional effect was observed in PLA + 0.5% Ag (ROP). The crystallization involvement resulted in a severe suppression of T_g (−25 °C).