Boosting Potassium Storage via Multifunctional Interface with High Lattice‐Matching

Abstract Atomic‐scale interface engineering is a prominent strategy to address the large volume expansions and sluggish redox kinetics for reinforcing K‐storage. Here, to accelerate charge transport and lower the activation energy, dual carbon‐modified interfacial regions are synthesized with high lattice‐matching degree, which is formed from a CoSe 2 /FeSe 2 heterostructure coated onto hollow carbon fibers. State‐of‐the‐art characterization techniques and theoretical analysis, including ex‐situ soft X‐ray absorption spectroscopy, synchrotron X‐ray tomography, ultrasonic transmission mapping, and density functional theory, are conducted to probe local atomic structure evolution, mechanical degradation mechanisms, and ion/electron migration pathways. The results suggest that the heterostructure composed of the same crystal system and space group can sharply regulate the redox kinetics of transition metal selenium and dual carbon‐modified approach can tailor physicochemical degradation. Overall, this work presents the design of a stable heterojunction synergistic superior hollow carbon substrate, inspiring a pathway of interface engineering strategy toward high‐performance electrode.