Falletta, StefanoGono, PatrickGuo, ZhendongKampouri, StavroulaStylianou, Kyriakos C.Pasquarello, Alfredo2020-11-012021-09-232020-11-012020-10-2110.1039/d0ta06028chttps://infoscience.epfl.ch/handle/20.500.14299/172917WOS:000578872600023We investigate the synergy occurring in photocatalytic water splitting between the metal-organic framework MIL-125-NH(2)and two co-catalysts, namely NiO and Ni2P, by calculating their band edge alignment with respect to the redox levels of liquid water. For the NiO/H2O and Ni2P/H2O interfaces, we employ an explicit atomistic description of water and perform molecular dynamics simulations considering both molecular and dissociated water adsorbed at the co-catalyst surface. For the MIL-125-NH2/NiO and MIL-125-NH2/Ni2P interfaces, we rely on the concept of charge neutrality and use a scheme combining the electron affinities and the charge neutrality levels of the interface components. We provide a description of the underlying fundamental processes that is consistent with photoluminescence and intrinsic activity experiments and that supports NiO and Ni2P as suitable co-catalysts for MIL-125-NH(2)as far as the hydrogen evolution reaction is concerned.Chemistry, PhysicalEnergy & FuelsMaterials Science, MultidisciplinaryChemistryEnergy & FuelsMaterials Scienceschottky-barrier heightsband offsetselectronic-propertieshydrogen-productionnickel phosphidesemiconductoralignmentgappotentialsheterojunctionstext::journal::journal article::research article