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

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 SnSe 2 /FeSe 2 heterojunctions with continuous channels for ion/electron transfer but maintain excellent conversion reversibility. Serving as anode for lithium storage, the SnSe 2 /FeSe 2 @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.