A new synthesis of PDTBTBz-2F _anti was developed via DHAP using a partially biobased monomer. Two pathways were compared by DFT, experiments and OSC tests, benchmarked to Stille coupling, and preliminarily adapted to continuous-flow.

Mammalian neurons exhibit diverse structural and physiological properties: a heterogeneity not present in current neuromorphic systems. Recent advancements have led to bio‐realistic spiking systems which are based on the integration and long‐term operation of organic electrochemical transistors (OECTs) with anti‐ambipolar characteristics. However, the library of materials enabling anti‐ambipolarity (AA) is restricted by the lack of stable, fast, and scalable organic mixed ionic and electronic conductors (OMIECs) exhibiting this specific OFF‐ON‐OFF behavior. This complicates mimicking specialized neuron types. Blending semiconducting with insulating polymers is a classic organic and OMIEC electronics strategy to improve device performance and enable tunability, yet unexplored for improving anti‐ambipolar stability in non‐ladder‐type anti‐ambipolar materials. Here, the n‐type OMIEC, P(gNDI‐gT2), is blended with the insulating polymer, PMMA, yielding stable anti‐ambipolar characteristics. The miscibility in solution forms a mechanically stabilizing and ion‐permeable framework in the solid state that considerably reduces swelling‐induced structural damage, thus preventing dramatic failure after the first operation cycles without compromising the conductive polymer's electronic pathways. Modulating the polymer blend ratio enables low‐power, fast‐spiking Hodgkin–Huxley neurons with tunable and programmable dynamics, without optimized device geometries, demonstrating frequency deconvolution and reservoir computing. These two computing primitive building blocks are essential for designing efficient spiking neural networks.

There is growing demand for biosourced functional polymers, particularly in organic electronics, which continue to rely heavily on petroleum-derived materials. In this regard, platform chemicals obtained from biomass offer sustainable alternatives. However, the development of biosourced polymers prepared by metal-free methods remains limited. In this context, lignin-derived divanillin is an attractive renewable unit that can be incorporated into polymer backbones. This work discusses the synthesis and characterization of a new family of biosourced divanillin-based polymers prepared through metal-free aldol polycondensation. Divanillin was obtained from biosourced vanillin and converted into two dialdehyde monomers bearing either methyl or decyl substituents. These monomers were polymerized via aldol polycondensation, affording the following polymers: PDVMeCP, PDVMeCH, PDVMeIND, and PDVC10IND. The influence of the cyclic ketone unit and side-chain structure on their thermal and optical properties was investigated. The polymers were soluble in common organic solvents and also showed solubility in greener solvents such as ethyl L-lactate and p-cymene. Optical and electrochemical analyses showed absorption maxima between 357 and 391 nm and electronic bandgaps from 1.84 to 2.14 eV. Overall, the results demonstrate that divanillin is a promising renewable building block for the metal-free synthesis of sustainable polymers.