This study is devoted to a new Si/Sn-Ni/Al/C composite material usable as negative electrode for lithium-ion batteries. The composite microstructure is made from Si nanoparticles embedded in a matrix, consisting of conductive carbon and Ni3.4Sn4 intermetallic compound. The nanostructure and composition of the composite material give excellent properties regarding reversible capacity, electrochemical stability, and reaction kinetics. Mechanical alloying has been chosen as synthesis method. The material structural and chemical properties have been determined by XRD analysis, by electron microscopy TEM and SEM, by EDX and EFTEM analysis and 119Sn Mössbauer spectroscopy. The electrochemical characterization was carried out by galvanostatic cycling and cyclic voltammetry. Lithium reactivity of these materials was studied by in-situ XRD analysis and 119Sn Mössbauer spectroscopy. This manuscript details the structural and electrochemical results obtained from various composite materials based on Ni3.4Sn4 by adding C, Al and Si elements. Reaction mechanisms during mechanical alloying and during electrochemical cycling have been investigated and the role of the different elements has been demonstrated. Finally, a discussion of the microstructure influence on the electrochemical performance of the composite materials is given. The best electrochemical properties are obtained for the composite material with nominal composition Ni0.14Sn0.17Si0.32Al0.04C0.35, which has a reversible capacity of 920 mAh/g with a very good stability of 280 cycles. Excellent kinetics during délithiation are obtained : 90% of capacity can be delivered in less than 5 minutes. However, the irreversible capacity (20 %) remains high and should be improved by stabilizing the solid/electrolyte interface (SEI)
