Liquid Phase Separation and Dual Glassy Structure Formation of Designed Zr-Ce-Co-Cu Alloys

Development of liquid-phase separated bulk metallic glasses is retarded due to difficulties in finding of immiscible systems with high glass-forming ability (GFA) of coexistent liquids. Zr-Ce alloy is a typical liquid immiscible system characterized by a liquid miscibility gap. We added Co and Cu into the Zr-Ce immiscible system and optimized the composition of the designed Zr-Ce-Co-Cu immiscible alloys. The solidification experiments were carried out for the quaternary alloys. The result indicates that the melt separated into ZrCo-rich and CeCu-rich liquids upon cooling through the miscibility gap. By optimizing the relative atomic ratio of Co:Cu, the coexistent ZrCo-rich and CeCu-rich liquids automatically assembled eutectic compositions during the liquid-liquid phase separation (LLPS). Under the condition of fast quenching, the two liquids subsequently undergo liquid-to-glass transition, resulting in the formation of composite structure with two glasses in the samples. We successfully developed phased-separated metallic glasses based on the Zr-Ce-Co-Cu immiscible alloys. This work not only strengthens the understanding in the LLPS but also provides a new strategy on the design of the dual glassy composites.