Soft energy harvesters capable of matching the intrinsic compliance of biological tissues are essential for the realization of imperceptible electronics. While piezoionic transduction in soft electrolyte networks offers ideal bio-integration, it produces voltage outputs that are much lower than those of rigid piezoelectrics due to thermodynamic constraints that limit charge separation and transport. Here, we address these challenges through a multiscale synergistic strategy that co-optimizes macroscopic, microstructural, and molecular asymmetries. Specifically, asymmetric electrodes with dissimilar work functions establish a built-in field that actively biases interfacial ionic charge separation. Acting in concert, a microcone array of soft ionic conductors concentrates mechanical stress to drive stress-induced ion dissociation and directional migration, while cation-π interactions within the polymer network function as a molecular kinetic trap to favor anion-dominated transport. This hierarchical coupling in soft ionotronic materials unlocks a colossal four-order-of-magnitude enhancement in voltage sensitivity (>104 mV kPa-1, 0.03-0.07 kPa) and delivers a peak power density of 135.1 µW cm-2. The strategy proves universal as it operates in both ionogels and hydrogels to offer complementary advantages in stability and ionic conductivity. Demonstrations including breathing-driven LED illumination, confirm the scalability. These results establish a generalizable materials framework for high-performance piezoionic energy harvesting and autonomous bio-interfaces.
Zhan et al. (Wed,) studied this question.
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