Dynamically Forming Interconnected Interfaces in Confined Heterostructures Enable High Capacity Conversion Chemistry

Abstract Heterostructures endow electrochemical hybrids with promising energy storage properties owing to synergistic effects and interfacial interaction. However, developing a facile but effective approach to maximize interface effects is crucial but challenging. Herein, a bimetallic selenide heterostructure is realized in a confined carbon network via an in situ electrochemical strategy to induce highly active and stable electrode architecture. The dynamically formed heterostructures upon repeated delithiation/lithiation process not only yield abundant interconnected SnSe₂/FeSe₂ heterojunctions with continuous channels for ion/electron transfer but maintain excellent conversion reversibility. Serving as anode for lithium storage, the SnSe₂/FeSe₂@C framework enables a high discharging capacity of 1781.9 mAh g⁻¹ at 0.5 A g⁻¹ after 500 cycles and superior cycling stability (no capacity fade after 1200 cycles at 2 A g⁻¹). This study can guide future design protocols for interface engineering through the formation of dynamic channels of conversion reaction kinetics for potential applications in high‐performance electrodes.