Interfacial Oxygen Stabilizes Composite Silicon Anodes

Silicon can store Li+ at a capacity 10 times that of graphite anodes. However, to harness this remarkable potential for electrical energy storage, one has to address the multifaceted challenge of volume change inherent to high capacity electrode materials. Here, we show that, solely by chemical tailoring of Si-carbon interface with atomic oxygen, the cycle life of Si/carbon matrix-composite electrodes can be substantially improved, by 300%, even at high mass loadings. The interface tailored electrodes simultaneously attain high areal capacity (3.86 mAh/cm(2)), high specific capacity (922 mAh/g based on the mass of the entire electrode), and excellent cyclability (80% retention of capacity after 160 cycles), which are among the highest reported. Even at a high rate of 1C, the areal capacity approaches 1.61 mAh/cm(2) at the 500th cycle. This remarkable electrochemical performance is directly correlated with significantly improved structural and electrical interconnections throughout the entire electrode due to chemical tailoring of the Si-carbon interface with atomic oxygen. Our results demonstrate that interfacial bonding, a new dimension that has yet to be explored, can play an unexpectedly important role in addressing the multifaceted challenge of Si anodes.