Carboxylating Elastomer Via Thiol-Ene Click Reaction to Improve Miscibility with Conjugated Polymers for Mechanically Robust Organic Solar Cells with Efficiency of 19%

Incorporating flexible insulating polymers is a straightforward strategy to enhance the mechanical properties of rigid conjugated polymers, enabling their use in flexible electronic devices. However, maintaining electronic characteristics simultaneously is challenging due to the poor miscibility between insulating polymers and conjugated polymers. This study introduces the carboxylation of insulating polymers as an effective strategy to enhance miscibility with conjugated polymers via surface energy modulation and hydrogen bonding. The carboxylated elastomer, synthesized via a thiol-ene click reaction, closely matches the surface energy of the conjugated polymer. This significantly improves the mechanical properties, achieving a high crack-onset strain of 21.48%, surpassing that (5.93%) of the unmodified elastomer:conjugated polymer blend. Upon incorporating the carboxylated elastomer into PM6:L8-BO-based organic solar cells, an impressive power conversion efficiency of 19.04% is attained, which top-performs among insulating polymer-incorporated devices and outperforms devices with unmodified elastomer or neat PM6:L8-BO. The superior efficiency is attributed to the optimized microstructures and enhanced crystallinity for efficient and balanced charge transport, and suppressed charge recombination. Furthermore, flexible devices with 5% carboxylated elastomer exhibit superior mechanical stability, retaining approximate to 88.9% of the initial efficiency after 40 000 bending cycles at a 1 mm radius, surpassing approximate to 83.5% for devices with 5% unmodified elastomer. An effective strategy to enhance the miscibility between the conjugated polymer PM6 and the insulating elastomer styrene-butadiene-styrene (SBS) has been developed by incorporating carboxyl groups into SBS (SBS-COOH), resulting in optimized mechanical properties and morphology of PM6. A remarkable power conversion efficiency of 19.04% is achieved for organic solar cells with 5% SBS-COOH (PM6:L8-BO system), outperforming devices of PM6:L8-BO without or with SBS. image