Pressure-Driven Topological Reconfiguration toward Fast-Charging Hard Carbon with Plateau-Capacity Retention

Abstract

Abstract Conventional carbonization of semi-coke induces excessive ordering of aromatic skeletons, producing dense graphitic structures that hinder Na+ intercalation and suppress low-potential plateau capacity. Here, we develop a rapid thermomechanical coupling sintering strategy using moderate pressure to drive π–π interactions and topological reconfiguration of aromatic units. This process suppresses excessive graphitization while constructing interconnected, twisted pseudo-graphitic domains with abundant closed nanopores. At 1000 mA g–1, PTR-HC reaches 80% SOC in ≈14.4 min and retains 90.1% of its plateau capacity, enabled by abundant Na+ storage sites and rapid diffusion pathways. Kinetic analyses reveal accelerated Na+ transport and a thin, NaF-rich solid-electrolyte interphase with fewer organic components. In situ XRD and Raman attribute slope capacity to surface/defect adsorption and intercalation and the plateau capacity to quasi-metallic Na clusters in closed pores. This work establishes pressure-driven topological engineering as a promising strategy for upgrading semi-coke into fast-charging hard carbon with high plateau-capacity retention.