It is well known that rhodium exhibits high catalytic activity towards both reduction and oxidation reactions . Although several Rh-containing materials have been used in electrocatalysis of HER , only a small fraction of these was tested in alkaline media . An example is a Ni 89 Rh 11 alloy which has been experimentally shown to have excellent activity , which can largely be attributed to the bifunctionality of the surface. Furthermore, it was discussed that the Ni/Rh phases play the roles of H-adsorption/desorption sites, while the Ni(OH) 2 and Rh 2 O 3 phases catalyze water dissociation, but no direct pieces of evidence were provided for such claims . Moreover, Ni-Rh catalysts were also used for other catalytic reactions , showing the versatility of this catalytic system. However, the downside of Rh-containing catalysts is the high price of Rh, caused by its scarcity. With this in mind, it is important to optimize the design of novel Rh-containing electrocatalysts, taking advantage of the high catalytic activity of Rh while maintaining its low concentrations. Finally, it is important to note that the application of Ni/Rh electrocatalysts is potentially highly favorable, since not only does Rh enhance the HER performance and the overall water splitting , but, most likely, there is an underlying synergistic effect of Ni and Rh which could go beyond HER catalysis.