In this study, high strength CuAg foils with nano-lamellar structures were prepared using a pulse electrodeposition method in an environmental-friendly methanesulfonic acid (MSA)-based solution. In an MSA-based bath, the Ag+ ion acted as the source for solute atoms and as a brightening agent, which allowed the formation of compact and bright CuAg structures in an additive-free bath. The application of pulse plating led to the formation of a nano-lammellar structure, in which Cu-rich and Ag layers were repeatedly stacked. Because of the contribution of the Ag layer, the as-deposited CuAg foil exhibited a high ultimate tensile strength (927 MPa) even at a low Ag content (2.37 wt%). The strength of the CuAg foil was further improved with annealing at 100–250 °C owing to the stabilization of the phase boundary. Despite a high fraction of the phase boundary, the nanostructure was stably maintained even after annealing at 250 °C for 1 h.
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