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Unraveling the synergy between metal-organic frameworks and co-catalysts in photocatalytic water splitting

Stefano Falletta1*, Patrick Gono1*, Zhendong Guo1*, Stavroula Kampouri2*, Kyriakos C. Stylianou2*, Alfredo Pasquarello1*

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

* Corresponding authors emails: stefano.falletta@epfl.ch, patrick.gono@epfl.ch, zhendongguozju@gmail.com, stavroula.kampouri@epfl.ch, kyriakos.stylianou@oregonstate.edu, alfredo.pasquarello@epfl.ch
DOI10.24435/materialscloud:ge-at [version v1]

Publication date: Oct 14, 2020

How to cite this record

Stefano Falletta, Patrick Gono, Zhendong Guo, Stavroula Kampouri, Kyriakos C. Stylianou, Alfredo Pasquarello, Unraveling the synergy between metal-organic frameworks and co-catalysts in photocatalytic water splitting, Materials Cloud Archive 2020.125 (2020), doi: 10.24435/materialscloud:ge-at.


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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File name Size Description
395.8 MiB Trajectories of the most stable MD at the NiO/H2O and Ni2P/H2O interfaces
25.4 KiB Bulk structures of NiO, Ni2P, and MIL-125-NH2
7.3 KiB Input files for electronic optimization and for the MD simulations
647 Bytes README file containing a description of all files in this record


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External references

Journal reference (Paper in which the method is described)


Density functional calculations Electronic structure of atoms & molecules First-principles calculations Photocatalysis Water splitting Metal-organic frameworks co-catalyst Molecular dynamics Hydrogen evolution MARVEL/DD4

Version history:

2020.125 (version v1) [This version] Oct 14, 2020 DOI10.24435/materialscloud:ge-at