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Laser‐Manufactured Metastable Supranano SnOx for Efficient Electron/Ion Bridging in SnO2‐Graphene Heterostructure Boosting Lithium Storage

Robust anchoring of high‐capacity nanocrystals (NCs) on porous conductive substrates is of paramount importance but it is challenging for highly efficient energy storage to prevent the weak interfacial interactions, inevitable aggregation, and sluggish charge transfer, due to the technical hurdles of constructing heterostructures with firm electron/ion bridging. Herein, a facile and high‐efficiency liquid‐phase laser manufacturing strategy to guarantee the covalent bonding of ultrafine NCs on conductive substrates by predesigning metastable supranano (<10 nm) particles is proposed. The manufacturing of supranano SnO2 (≈3.4 nm) is demonstrated to tightly anchor on mesoporous walls of graphene with high loading (≈81.3%) and homogenous dispersion. Such a optimized heterostructure with unimpeded electron/ion transfer delivers extraordinary long‐term cycling stability (1132 mAh g–1 at 1.0 A g–1 after 1250 cycles) and impressive rate capability (275 mAh g–1 at 30.0 A g–1) as the anode for Li‐storage, which are some of the highest values among the reported SnO2‐based anodes. The study provides an important avenue for addressing the interfacial bridging in‐between heterostructures via creating active metastable supranano particles for intriguing electrochemical applications or even beyond, based on laser‐matter interactions.