Gravity-Driven Assembly of Janus-Structured Ceramic-Polymer Hybrid Electrolytes for Stabilized Flexible Energy Storage

초록

Developing polymer electrolytes that simultaneously possess high ionic conductivity and superior interfacial stability presents a formidable challenge for flexible zinc-air batteries (ZABs), as these properties typically entail antagonistic structural requirements. To resolve this dilemma, a gravity-driven self-stratification strategy is conceptualized by engineering a Janus-structured hybrid electrolyte. Through the spontaneous sedimentation of hollow mesoporous silicon carbide (SiC) nanospheres within a polyampholyte network, a functionally graded architecture is constructed. Crucially, this asymmetric design enables a spatial decoupling of functions. In the bulk phase, dispersed SiC nanospheres serve as ionic modulators, leveraging mesoporous confinement and surface hydroxyls to reconstruct the hydrogen-bonding network of water, thereby establishing high-speed conduction channels (163.2 mS cm-1); conversely, at the anode interface, the in situ formed dense SiC layer acts as a physicochemical buffer that homogenizes zincate flux and mitigates local alkalinity. Consequently, this synergistic regulation empowers the assembled flexible ZABs with a high peak power density (123.4 mW cm-2) and an ultralong lifespan of 172 h. This work conceptualizes a facile sedimentation-assisted structural engineering approach, offering a generalizable pathway to decouple mechanical robustness and electrochemical activity in advanced ceramic-polymer hybrid electrolytes.

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