As the need for clean energy generation and storage grows, the efficiency for low cost hydrogen generation needs to be addressed to further the pragmatic development of this key technology. Given that the efficiency of electrochemical hydrogen generation is limited primarily by the sluggish kinetics of the anodic reaction used, such as the oxygen evolution reaction, extensive efforts have been made to reduce the overpotentials for the anodic reaction in alkaline media with advanced catalysts. The electrooxidation of urea, hydrazine, and other small molecules has attracted considerable attention for the electrochemical generation of hydrogen due to the lower electrochemical potential required to drive these reactions. By tuning the electronic structure of nickel-containing perovskites as well as derivatives of the perovskite structure, higher oxidation states of nickel active sites can be achieved, leading to increased catalytic activities at a fraction of the cost of other nickel-rich materials.