The functionalisation of limonene has enabled the synthesis of two renewably-sourced monomers for the formation of terpene-derived polyesters. Three methods for the synthesis of the novel hydroxy-acid 6 are reported and their green-credentials scrutinised through comparison of their sustainability-metrics. Step-growth homo-polymerisation of 6 is demonstrated to yield a low molecular weight (2.6 kDa) novel polyester with 100% of its carbon content originating from the terpene starting material. The corresponding diol 2 is shown to act as a co-monomer with a renewable diacid. The resultant polyesters display impressive M_ns of up to 30 kDa with T_gs between −6 and 24 °C. These materials have been shown to depolymerise under basic conditions for reclamation of the diol monomer 2.

The application of electrochemical reactions in natural product synthesis has burgeoned in recent years. We herein report a formal synthesis of the complex and dimeric natural product kingianin A, which employs an electrochemically-mediated radical cation Diels–Alder cycloaddition as the key step.

It is reported that efficient photoinitiators, suitable for two‐photon polymerization, can be obtained using the copper catalyzed azide/alkyne cycloaddition reaction. This click chemistry strategy provides a modular approach to the assembly of photoinitiators that enables the rapid variation of key fragments to produce photoinitiators with desirable properties. To assess the performance of the first‐in‐class photoinitiators generated by this approach, a screening method is developed to enable the rapid determination of polymerization and damage thresholds in numerous photoresists during two‐photon polymerization. The degree of consumption of vinyl groups (DC) and homogeneity of the polymerization are further assessed by micro‐Raman spectroscopy. Finally, more complex structures are fabricated to demonstrate that the efficient two‐photon polymerization of stable 3D microarchitectures can be achieved using triazole‐based photoinitiators.

Conductive hydrogel-based materials are attracting considerable interest for bioelectronic applications due to their ability to act as more compatible soft interfaces between biological and electrical systems. Despite significant advances that are being achieved in the manufacture of hydrogels, precise control over the topographies and architectures remains challenging. In this work, we present for the first time a strategy to manufacture structures with resolutions in the micro-/nanoscale based on hydrogels with enhanced electrical properties. Gelatine methacrylate (GelMa)-based inks were formulated for two-photon polymerisation (2PP). The electrical properties of this material were improved, compared to pristine GelMa, by dispersion of multi-walled carbon nanotubes (MWCNTs) acting as conductive nanofillers, which was confirmed by electrochemical impedance spectroscopy and cyclic voltammetry. This material was also confirmed to support human induced pluripotent stem cell-derived cardiomyocyte (hPSC-CMs) viability and growth. Ultra-thin film structures of 10 µm thickness and scaffolds were manufactured by 2PP, demonstrating the potential of this method in areas spanning tissue engineering and bioelectronics. Though further developments in the instrumentation are required to manufacture more complex structures, this work presents an innovative approach to the manufacture of conductive hydrogels in extremely low resolution.