Self‐Adaptive Interface Reconstruction over Black Phosphorus Complex for Wide‐Temperature and Fast‐Charging Potassium Ion Storage

Black phosphorus (BP), exhibiting a large spatial layer and high theoretical capacity, has been heralded as a promising candidate for K+ storage. Nevertheless, the unpredictability of the structural/interfacial reconstruction guides the arduous kinetics and poor stability, especially conferring to high current density and wide‐temperature operation. To address these challenges, self‐adaptive interface reconstruction with a multiple secondary bonds mediation (IRSM) strategy is adopted for amphipathic BP complex to improve kinetics and stability, wherein BP nanospheres encapsulated into a sacciform B‐doped carbon matrix (BC) are further grafted with polybromoisobutyryloxy benzenesulfonic (PBBS), which undergoes in situ polymerization and is transformed into metal‐organic bromoisobutyrylox supramolecular (PBS). Consequently, combining the flexibility/rigidity advantage of organic moiety and the stability advantage of inorganic moiety, BC@BP@PBS manifests excellent fast charging behaviors, a wide‐temperature operation from −70 °C to 80 °C, and an extended cycle life of up to 1300 cycles. This work builds an ingenious protocol for leveraging the trade‐off between fast charging, wide‐temperature operation, and long life span for high‐performance cell devices.