A Highly Reversible Nano‐Si Anode Enabled by Mechanical Confinement in an Electrochemically Activated LixTi₄Ni₄Si₇ Matrix

This paper reports a Si‐Ti‐Ni ternary alloy developed for commercial application as an anode material for lithium ion batteries. Our alloy exhibits a stable capacity above 900 mAh g −1 after 50 cycles and a high coulombic efficiency of up to 99.7% during cycling. To enable a highly reversible nano‐Si anode, melt spinning is employed to embed nano‐Si particles in a Ti 4 Ni 4 Si 7 matrix. The Ti 4 Ni 4 Si 7 matrix fulfills two important purposes. First, it reduces the maximum stress evolved in the nano‐Si particles by applying a compressive stress to mechanically confine Si expansion during lithiation. And second, the Ti 4 Ni 4 Si 7 matrix is a good mixed conductor that isolates nano‐Si from the liquid electrolyte, thus preventing parasitic reactions responsible for the formation of a solid electrolyte interphase. Given that a coulombic efficiency above 99.5% is rarely reported for Si based anode materials, this alloy's performance suggests a promising new approach to engineering Si anode materials.