Multilayer Si@SiOx@void@C anode materials synthesized via simultaneously carbonization and redox for Li-ion batteries

Abstract

In the development of high-performance lithium-ion batteries (LIBs), the composition and structure of electrode materials are of critical importance. Silicon has a theoretical specific capacity 10 times that of graphite, nonetheless, its application as an anode material confronts challenge as it undergoes huge volume change and pulverization amidst the alloying and dealloying processes. Herein, a novel method to prepare a multilayer Si-based anode was proposed. Three layers, SiO2, nickel and triethylene glycol (TEG), were coated successively on Si nanoparticles, which served respectively as the sources of SiOx, sacrificial templates and carbon. Nickel can not only serve as a hollow template, but also play a catalytic role, which makes carbonization and redox reactions occur synchronously under a mild condition. Amid the carbonization process of TEG at 450 °C, several-nm-thick SiO2 layer can react with the as-derived carbon to form a silicon suboxides (SiOx (0 < x < 2)) intermedium layer. After removing the nickel template, a micro-nano scaled Si@SiOx@void@C with conformal multilayer-structure can be obtained. The BET specific surface area and pore volume of powders were increased dramatically because of the derivation of abundant voids, which can not only buffer the swelling effect of silicon, but also provide richer ionic conductivity. The as-assembled half-cell with Si@SiOx@void@C as the anode material possesses high capacity (∼1000 mAh g−1 at 3 A g−1), long cycle life (300 cycles with 77% capacity retention) and good rate performance (558 mAh g−1 at 5 A g−1).