Aspects described herein generally relate to bimetallic structures, syntheses thereof, and uses thereof. In an embodiment, a process for forming a bimetallic nanoframe is provided. The process includes forming a first bimetallic structure by reacting a first precursor comprising platinum (Pt) and a second precursor comprising a Group 8-11 metal (M2), wherein M2 is free of Pt; reacting a third precursor comprising Pt with the first bimetallic structure to form a second bimetallic structure, the second bimetallic structure having a higher molar ratio of Pt to Group 8-11 metal than the first bimetallic structure; and introducing the second bimetallic structure with an acid to form the bimetallic nanoframe, the bimetallic nanoframe having a higher molar ratio of Pt to Group 8-11 metal than that of the second bimetallic structure, the bimetallic nanoframe having the formula: (Pt)a(M2)b, wherein: a is the amount of Pt; b is the amount of M2.