All-Process Catalysis from Low-Cost Scalable Synthesis to Activated Electrochemical Reaction of SiO x /Carbon Anodes

Abstract Silicon oxide (SiOx) is a promising anode for lithium-ion batteries, yet its practical application is hindered by multistep synthesis, hazardous silane-based routes, poor scalability, and sluggish electrochemical conversion. Herein, we report a low-cost and scalable strategy for constructing graphitic carbon-confined SiOx (SiOx@GC) anodes via all-process catalysis using waste-derived superabsorbent polymers and industrial by-product SiCl4 as carbon and silicon precursors, respectively. Ni species participate throughout by catalyzing carbon graphitization, mediating confined SiOx formation, and dynamically facilitating electrochemical conversion during cycling. This integrated Ni-enabled process promotes efficient SiOx formation and its deeper, more reversible conversion into electrochemically active silicon. Consequently, the SiOx@GC anode delivers 1147 mAh g–1 after 100 cycles at 0.1 A g–1, stable cycling over 1000 cycles at 5 A g–1, and a full-cell energy density of 353 Wh kg–1 after 250 cycles. This work establishes an all-process catalytic framework for coupling scalable SiOx synthesis with reversible electrochemical conversion.