High‐Crystallinity Wrinkled Hard Carbon via Molecular‐Level Anchoring Glucose Molecules with Cooperative‐Assembly of Intermolecular Hydrogen Bonds for Sodium‐Ion Batteries

Abstract Tuning of micro‐ and macro‐structures of hard carbon is important for expanding its properties. However, achieving controlled and integrated modulation of the micro‐ and macro‐structures of such materials remains a challenge. An intermolecular hydrogen bond‐driven interfacial cooperative‐assembly and then polymerization strategy is reported herein: micelles‐glucose molecules are used for the synthesis of wrinkled hard carbon spheres with precisely tunable crystallinity. As intermolecular hydrogen is positioned bonds to achieve an anchoring effect, which facilitates immobilization of glucose molecules at the molecular level during the assembly and subsequent dehydration‐aromatization. In virtue of controlling the micelle concentration, the density of intermolecular hydrogen bonding interactions is precisely regulated. As a result, the yielded hard carbon spheres exhibited excellent sodium‐ion storage performance because of their high crystallinity and exposed surfaces. By establishing a simple micelle–based interfacial reaction strategy, the study leverages optimized intermolecular hydrogen bond anchoring effects to tailor the properties of materials at a molecular level.