Crumpled two-dimensional heterostructures for pseudocapacitive and interphase-stable fast-charging silicon anodes

In this study, a crumpled heterostructured composite composed of Si nanoparticles (NPs) combined with reduced graphene oxide (rGO), MoS₂, and Ti₃C₂T_x MXene (Si@rGO/MoS₂/MXene crumpled composite, SGMM-CC) is developed as a robust conductive matrix for stabilizing high-capacity Si anodes. Within this architecture, rGO serves as a lightweight and flexible backbone that enables long-range electron transport, MoS₂ provides a mechanically compliant layered interface that facilitates ion transport, and MXene offers a chemically active surface that stabilizes adjacent components while enhancing electrical conductivity and mechanical strength. The resulting three-dimensional structure establishes a continuous conductive network, accommodates volume changes, and strengthens interfacial interactions, thereby mitigating Si pulverization and suppressing the formation of an unstable solid-electrolyte interphase. Consequently, the SGMM-CC anode delivers an initial Coulombic efficiency of ∼84% and a high reversible capacity of ∼1350 mAh g^-1 at 6 A g^-1. In addition, it retains 74.6% of its capacity after 1100 cycles at 3 A g^-1, significantly outperforming the Si/rGO (10.0%) and Si/rGO/MoS₂ (24.6%) control electrodes. These results indicate that multi-2D crumpled heterostructures are effective in enabling durable and high-rate Si anodes for next-generation lithium-ion batteries.