Amphicharge‐Storable Pyropolymers Containing Multitiered Nanopores

Abstract In this study, hierarchically nanoporous pyropolymers (HN‐PPs) including numerous redox‐active heteroatoms are fabricated from polyaniline nanotubes by heating with KOH. In the large operating voltage range 1.0–4.8 V versus Li⁺/Li, HN‐PPs store amphicharges by a pseudocapacitive manner of Li‐ion (mainly <3.0 V) and electrochemical double layer formation of anion (primarily >3.0 V). Through these surface‐driven charge storage behaviors, HN‐PPs achieve a significantly high specific capacity of ≈460 mA h g⁻¹ at 0.5 A g⁻¹, maintaining specific capacities of 140 mA h g⁻¹ at a high specific current of 30 A g⁻¹ and 305 mA h g⁻¹ after 2000 cycles at 3 A g⁻¹. Furthermore, asymmetric energy storage devices based on HN‐PPs deliver a high specific energy of 265 W h kg⁻¹ and high specific power of 5081 W kg⁻¹ with long‐term cycling performance.