Abstract
Flexible thermoelectric generators (FTEGs) based on polymeric materials can conform to irregular surfaces; however, they often suffer from limited performance and stretchability. To overcome these limitations, we developed an inorganic–organic synergy thermoelectric generator (iosTEG) that delivers superior output power, achieving 2.5 μW under a 40 K temperature gradient in a single-pair configuration, outperforming previous all-organic and hybrid FTEGs. The iosTEG was fabricated via tape-assisted exfoliation of high-crystallinity p - and n -type Bi 2 Te 3 flakes, aligned on a flexible, self-healing Ni-bpyPTD polymer. Specifically, the Ni-bpyPTD matrix, synthesized through the crosslinking polymerization of PTD and 4,4′-bis(hydroxymethyl)-2,2′-bipyridine, followed by Ni 2+ coordination, forms dynamic supramolecular networks that enable stretchability and self-repair via hydrogen bonding and metal–ligand interactions. Moreover, liquid eutectic gallium–indium (EGaIn) was employed as a deformable electrode to bridge the flakes and copper electrode terminals. Notably, the iosTEG retains its functionality upon deformation, maintaining an output voltage of 13.9 mV after stretching ( cf. 17.8 mV in the undeformed state, Δ T = 30 K). The iosTEG exhibits excellent mechanical durability, maintaining stable electrical resistance under cyclic deformation, including bending to a 1.0 mm radius and stretchability up to 150%, while autonomously restoring conductivity after damage. The self-healing behavior is further validated by the recovery of R after intentional cutting, highlighting the promise of inorganic–organic integration for stretchable, durable, and high-performance energy devices.