Interfacial Storage for Next-Generation Batteries: Mechanisms, Advances, and Challenges

Modern battery systems confront inherent kinetic and durability limitations due to the simultaneous accommodation of electrons and ions within the bulk phase of electrode materials. A paradigm-shifting strategy, inspired by the “job-sharing” electrochemistry concept, addresses these challenges by decoupling electron and ion storage into distinct space charge regions at engineered heterointerfaces. Despite the considerable promise of interfacial storage mechanisms in advancing next-generation batteries, the field lacks a coherent theoretical framework and universal design principles to fully harness their potential across diverse material systems and device architectures. This review provides a fundamental understanding of interfacial storage mechanisms while elucidating their impacts on electrochemical performance. We critically analyze recent breakthroughs in nanocomposite/heterostructure electrodes and solid-state electrolytes, highlighting how rational interface engineering can enhance charge transfer kinetics, transcend intrinsic bulk storage limitations, improve structural stability, and mitigate space charge effects at electrode/electrolyte interfaces. Moreover, we discuss cutting-edge characterization methodologies essential for probing interfacial evolution and charge storage behavior. Finally, we identify pivotal challenges in interfacial stability control and scalable manufacturing, while proposing promising research directions, such as atomic-scale interface engineering and sustainable fabrication strategies, to advance carbon-neutral energy storage systems through innovative electrochemical approaches.