The rapid growth of wearable systems
demands sustainable, mechanically
adaptable, and eco-friendly energy-harvesting devices. Quasi-solid
ionic thermocells have demonstrated the capability of continuously
converting low-grade heat into electricity to power wearable electronics.
However, a trade-off between ion conductivity and mechanical properties
is one of the most challenging obstacles for developing high-performance
quasi-solid thermocells. Herein, the trade-off is overcome by designing
anisotropic polymer networks to produce aligned channels for ion-conducting
and hierarchically assembled crystalline nanofibrils for crack blunting.
The ionic conductivity of the anisotropic thermocell has a more than
400% increase, and the power density is comparable to the record of
state-of-the-art quasi-solid thermocells. Moreover, compared with
the existing quasi-solid thermocells with the optimal mechanical performance,
this material realizes biomimetic strain-stiffening and shows more
than 1100% and 300% increases in toughness and strength, respectively.
We believe this work provides a general method for developing high-performance,
cost-effective, and durable thermocells and also expands the applicability
of thermocells in wearable systems.