Intrinsically stretchable polymer semiconductors synergistically constructed by hydrogen bonds and metal coordination

Intrinsically stretchable semiconducting polymers play a vital role in the development of wearable electronics, featuring low-cost, large-area and high-density fabrication. Only single-stage dynamic chemical bond has been widely incorporated into polymer backbones to afford stretchability while multiple dynamic bonds have not been investigated, making a formidable challenge to achieve high stretchability without compromising charge transport properties. Herein, we synthesize a series of stretchable polymer semiconductors incorporating urethane and bipyridine units, which can provide dynamic interconnected polymer network by combination of hydrogen bonds with metal coordination, simultaneously obtaining excellent stretchability and carrier mobilities. Compared with single-stage hydrogen bonds, multiple dynamic chemical bonds constructed by 10% hydrogen bonds and 0.25 equiv. metal coordination endowed the polymer semiconductors with an 58% enhancement in carrier mobility and a two-fold increase in crack-onset strain. Notably, the polymer exhibited stable carrier mobilities parallel to the stretching direction, with 91% of initial values even under 150% strain, which is the unprecedented value for intrinsically stretchable semiconducting polymers without blending of elastomers. Therefore, the introduction of multiple dynamic bonds provides an effective and promising approach for intrinsically stretchable and high-performance polymer semiconductor.