Atomistic modeling is used to study the role of different alloying additions to metallic U-Zr nuclear fuels in terms of their ability to reduce lanthanide migration to the outer surface of the fuel and thus reduce their interaction with cladding. The Bozzolo-Ferrante-Smith (BFS) method for alloys is used to examine the behavior of each addition, the resulting phase structure, and the evolution of the fuel surface. Different behaviors are observed for each of the additives (In, Tl, Ga, Sb, Pd), all a result of the competition between the formation of bulk precipitates and the tendency of each additive to segregate to the surface. For each case, characteristic temperatures are determined indicating the range of temperatures in which each additive performs a different role. Sb and Pd additives are determined to be the most effective additions, properly balancing their ability to bind lanthanides in the fuel with their own segregating tendencies.