Sustainable Recycling of Photovoltaic Silicon Waste into High‐Performance Anodes via Interface Engineering

Abstract Silicon‐based anodes are crucial for enhancing the energy density of lithium‐ion batteries, but the practical application is hindered by significant volume expansion and interfacial degradation. Here, a sustainable strategy is proposed to upcycle photovoltaic silicon waste (PV‐WSi) into high‐performance anode materials via interface‐engineered hierarchical structuring. The Si/TiO 2 constructed through sand milling achieves strong interfacial coupling, effectively dissipating stress and suppressing particle pulverization during cycling. A dual‐carbon network (carbon nanotubes (CNTs) integrated with polyvinylpyrrolidone (PVP)‐derived carbon shells) synergistically enhances electronic transport while isolating silicon from electrolyte corrosion. The large‐scale feasibility of this method is confirmed via COMSOL simulations and experiments. The optimized Si/TiO 2 /CNTs/C composite delivers ultralong cyclability (≈1100 mAh·g −1 after 2500 cycles at 1 A·g −1 ) and high‐rate capability (>1000 mAh·g −1 at 13 A·g −1 ). The assembled pouch‐type full cell (Si/TiO 2 /CNTs/C‐G//NCM811) achieves an energy density over 320 Wh·kg −1 and retains >500 mAh capacity with 77% retention after 500 cycles at 1 C. This work offers a scalable engineering strategy for the value‐added recycling of PV‐WSi and the development of advanced anode materials.