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There has been increasing interest in the emerging ionic thermoelectric materials with huge ionic thermopower. However, it’s challenging to selectively tune the thermopower of all-solid-state polymer materials because the transportation of ions in all-solid-state polymers is much more complex than those of liquid-dominated gels. Herein, this work provides all-solid-state polymer materials with a wide tunable thermopower range (+20~−6 mV K −1 ), which is different from previously reported gels. Moreover, the mechanism of  p - n  conversion in all-solid-state ionic thermoelectric polymer material at the atomic scale was presented based on the analysis of Eastman entropy changes by molecular dynamics simulation, which provides a general strategy for tuning ionic thermopower and is beneficial to understand the fundamental mechanism of the  p - n  conversion. Furthermore, a self-powered ionic thermoelectric thermal sensor fabricated by the developed  p - and  n -type polymers demonstrated high sensitivity and durability, extending the application of ionic thermoelectric materials.

Selectively tuning ionic thermopower in all-solid-state flexible polymer composites for thermal sensing