Adv. Funct. Mater.  - Host-Guest All-in-One Supercapacitors Enabled by 3D-Printed Zwitterionic Gel Microlattices for Advanced Energy Storage

Jian Meng, Zhenjiang Tan, Yang Chen, Wei Fan*, Chao Zhang, Le Li*, and Tianxi Liu*

Adv. Funct. Mater. 2025, DOI: 10.1002/adfm.202520575

All-in-one supercapacitors (ASCs) are promising advanced energy storage devices for flexible and wearable electronics, owing to their high structural integration, superior mechanical stability, and simplified assembly process. However, conventional planar-integrated ASCs often suffer from limited electrode loading, prolonged ion diffusion pathways, and poor low-temperature tolerance. Herein, a customizable host-guest 3D-ASC is reported that effectively overcomes these limitations. A zwitterionic hydrogel electrolyte with a graded microlattice architecture is fabricated via direct ink writing 3D printing, enabling enlarged electrolyte-electrode interfacial area and enhanced structural integrity. This architecture enables high active material loading without compromising ion transport efficiency. Simultaneously, the synergistic combination of zwitterionic polymers and water-in-salt components imparts ultrahigh ionic conductivity to the electrolyte, maintaining excellent performance even at −60 °C. The rationally designed host framework also facilitates in situ polymerization of polyaniline as the guest electrode, forming a continuous, integrated electrode-electrolyte interface. As a result, the host-guest 3D-ASC achieves a 12-fold enhancement in areal capacitance and energy density compared to planar ASCs, along with excellent rate capability, exceptional low-temperature resilience, and long-term cycling stability. This work demonstrates a robust and versatile strategy for next-generation integrated energy storage devices with high energy density and environmental adaptability.

Link: https://doi.org/10.1002/adfm.202520575