“…oxides, hydroxides, sulphides, phosphides, and carbides), nanocarbons, and artificial organometallic molecules, have been proven to be effective for hydrogen production, even with performance surpassing those of noble metals. 9,10,13 Nonetheless, all these findings rely to a great extent on trial-and-error and/or combinatorial approaches, 14,15 with little attention being paid to the investigation of the underlying structure–activity relationships. 16 The real active state of the cocatalyst, the location of the reaction site and its exact structure, as well as the fundamental operating mechanism, thus are all not exactly known, severely impeding the further rational design of efficient hydrogen production cocatalysts.…”