Giant and bidirectionally tunable thermopower in nonaqueous ionogels enabled by selective ion doping

Ionic thermoelectrics show great potential in thermal sensing owing to their ultrahigh thermopower, low cost, and ease in production. However, the lack of effective n-type ionic thermoelectric materials seriously hinders their applications. Here, we report giant and bidirectionally tunable thermopowers within an ultrawide range from −15 to +17 mV K⁻¹ in solid ionic liquid–based ionogels. Particularly, a record high negative thermopower of −15 mV K⁻¹ is achieved in the ternary ionogel, rendering it among the best n-type ionic thermoelectric materials under the same condition. A thermopower regulation strategy through ion doping to selectively induce ion aggregates to enhance ion-ion interactions is proposed. These selective ion interactions are found to be decisive in modulating the sign and magnitude of the thermopower in the ionogels. A prototype wearable device integrated with 12 p-n pairs is demonstrated with a total thermopower of 0.358 V K⁻¹, showing promise for ultrasensitive thermal detection.