Renewable energy technologies such as fuel cells, batteries, and photoelectrochemical cells are critically dependent on the design of inexpensive, electrochemically stable, and highly active electrocatalysts. However, the most active and stable electrocatalysts rely on the use of precious metals such as Platinum, which limits the commercial viability of these technologies. By coupling quantum chemistry calculations with mechanistic experimental studies, our objective is to reveal new classes of stable and highly active electrocatalysts with reduced precious metal loadings. Our approach will center on obtaining an atomic level understanding of the bond breaking and making events associated with the intrinsic properties of the catalyst. We envision that the body of work resulting for the combined theoretical and experimental studies will provide a robust guide for material selection to replace precious metal nanoparticles.