Interface and Morphology Engineered Amorphous Si for Ultrafast Electrochemical Lithium Storage

Abstract Ultrafast high‐capacity lithium‐ion batteries are extremely desirable for portable electronic devices, where Si is the most promising alternative to the conventional graphite anode due to its very high theoretical capacity. However, the low electronic conductivity and poor Li‐diffusivity limit its rate capability. Moreover, high volume expansion/contraction upon Li‐intake/uptake causes severe pulverization of the electrode, leading to drastic capacity fading. Here, interface and morphology‐engineered amorphous Si matrix is being reported utilizing a few‐layer vertical graphene (VG) buffer layer to retain high capacity at both slow and fast (dis)charging rates. The flexible mechanical support of VG due to the van‐der‐Waals interaction between the graphene layers, the weak adhesion between Si and graphene, and the highly porous geometry mitigated stress, while the three‐dimensional mass loading enhanced specific capacity. Additionally, the high electronic conductivity of VG boosted rate‐capability, resulting in a reversible gravimetric capacity of ≈1270 mAh g⁻¹ (areal capacity of ≈37 µAh cm⁻²) even after 100 cycles at an ultrafast cycling rate of 20C, which provides a fascinating way for conductivity and stress management to obtain high‐performance storage devices.