Si-P-Cu internally bonded anode: An innovative strategy for low-cost and high-performance pseudocapacitive Li-ion storage

Maintaining the structural integrity of silicon and phosphorus anodes during the Li+ insertion and extraction cycles poses a significant challenge. Inspired by the natural process of plant roots anchoring into soil, we present a simple yet effective method for integrating a Sisingle bondP anode into the copper current collector. This approach involves subjecting readily available and cost-effective micrometre-sized silicon particles (50–150 μm) and red phosphorus to mechanochemical treatment. Subsequently, the resulting Si/P composite is coated onto copper foil and subjected to annealing treatment, resulting in the formation of an integrated structure, incorporating Cu3Si, Cu3P, and P-doped Si, firmly established within the copper current collector. The electrode obtained (BM-Si@P/Cu-350), promoted by a crosslinked (polyimide) PI binder, outperforms not only the ball-milled Si and red P but also the same electrode in which the annealing process is absent (BM-Si@P/Cu-100). During the mechanochemical treatment, red P acts as both the doping agent and a lubricant, facilitating the grinding of the Si particles into P-doped Si particles in the range of predominantly 200–300 nm; while during the thermal treatment, Si plays a key role in preventing excessive interaction between the P and the Cu current collector. Instead, a tailored rooting of the active material into the current collector is achieved through the formation of Cu3P and Cu3Si phases, not only increasing the mechanical stability of the electrode to endure volume changes during cycling and limit developing cracks, but also enhancing the electrical conductivity of the system. This article suggests a simple and potentially low-cost strategy for the utilization of highly available micrometre-sized silicon and red-P for Li-ion storage applications.