Surface-Bound Silicon Nanoparticles with a Planar-Oriented N-Type Polymer for Cycle-Stable Li-Ion Battery Anode.

Silicon is now well-recognized to be a promising alternative anode for advanced lithium-ion batteries because of its highest capacity available today; however, its insufficiently high Coulombic efficiency upon cycling remains a major challenge for practical application. To overcome this challenge, we have developed a facile mechanochemical method to synthesize a core-shell-structured Si/polyphenylene composite (Si/PPP) with a n-type conductive PPP layer tightly bonded in a planar orientation to the surfaces of Si nanocores. Because of its compactness and flexibility, the outer PPP layer can protect the Si core from contacting the electrolyte and maintaining the structural stability of electrode/electrolyte interface during cycles. As a result, the Si/PPP anode demonstrated a high reversible capacity of ∼2387 mAh g-1, a stable cycleability with 88.5% capacity retention over 500 cycles, and, particularly, a high Coulombic efficiency of 99.7% upon extended cycling, offering a new insight for future development of high-capacity and cycle-stable Si anode.