Schematic depiction of the states and charge transfer reactions involved in the proton-coupled electron transfer process of interest, corresponding to the bracketed steps in Fig. 1. The complex shown has methyl substituents on the P and N atoms with all rings in the boat conformation. The ET, PT, and EPT reactions are shown for H2 oxidation, (1a) → (2b), and H2 production, (2b) → (1a).