Published October 14, 2020 | Version v1
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Unraveling the synergy between metal-organic frameworks and co-catalysts in photocatalytic water splitting

  • 1. Chaire de Simulation à l'Echelle Atomique (CSEA), École Polytechnique Fédérale de Lausanne (EPFL), CH-1015 Lausanne, Switzerland
  • 2. Laboratory of Molecular Simulation (LSMO), Institute of Chemical Sciences and Engineering, École Polytechnique Fédérale de Lausanne (EPFL), CH-1951 Sion, Switzerland

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Description

We investigate the synergy occurring in photocatalytic water splitting between the metal-organic framework MIL-125-NH2 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-NH2 as far as the hydrogen evolution reaction is concerned.

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References

Journal reference (Paper in which the method is described)
S. Falletta, P. Gono, Z. Guo, S. Kampouri, K. Stylianou, A. Pasquarello, J. Mater. Chem. A. (2020), doi: 10.1039/D0TA06028C

Journal reference (Paper in which the method is described)
S. Falletta, P. Gono, Z. Guo, S. Kampouri, K. Stylianou, A. Pasquarello, J. Mater. Chem. A. (2020)