Although ionic thermoelectric (iTE) materials can have very high thermopower, it is of great significance to develop novel methods to further improve the ionic thermopower and figure of merit (ZTi). Here, significant improvement in the thermopower and thus the ZTi value of an ionogel by cationic doping, is reported. Doping sodium dicyanamide (Na:DCA) into the ionogels of poly(vinylidene fluoride‐co‐hexafluoropropylene) (PVDF‐HFP) and 1‐ethyl‐3‐methylimidazolium dicyanamide (EMIM:DCA) that is an ionic liquid can greatly enhance the thermopower. This is attributed to the interactions between the doped Na+ cations and DCA– anions, thereby increasing the difference in the mobilities of EMIM+ cations and DCA– anions. Moreover, through the combination with the solid networks engineering by an anti‐solvent to PVDF‐HFP, the PVDF‐HFP/EMIM:DCA ionogel doped with 0.5 mol% Na+ with respect to EMIM+ exhibits an ionic thermopower of 43.8 ± 1.0 mV K–1, ionic conductivity of 19.4 ± 0.3 mS cm–1 and thermal conductivity of 0.183 W m–1 K–1 at the relative humidity of 85% and room temperature. The corresponding ZTi value thus reaches 6.1 ± 0.4, much higher than the previous ZTi records of iTE materials. These ionogels can be used in the iTE capacitors for the thermoelectric conversion.

Abundant heat is generated in household, industry and natural processes, and the majority of the heat is dissipated to environment as waste heat owing to the low heat utilization efficiency....

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