Stefano Falletta^1*, Patrick Gono^1*, Zhendong Guo^1*, Stavroula Kampouri^2*, Kyriakos C. Stylianou^2*, Alfredo Pasquarello^1*

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), https://doi.org/10.24435/materialscloud:ge-at

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.

Materials Cloud sections using this data

Files

File name	Size	Description
trajectories_MD.zip MD5md5:2458ddc0c529d585a610d5cb10566b10	395.8 MiB	Trajectories of the most stable MD at the NiO/H2O and Ni2P/H2O interfaces
atomic_coordinates.zip MD5md5:1134586073197158410a0de0790f61d2	25.4 KiB	Bulk structures of NiO, Ni2P, and MIL-125-NH2
input_files.zip MD5md5:0abe400d452093cd9b8defac0ede60cc	7.3 KiB	Input files for electronic optimization and for the MD simulations
README.txt MD5md5:6da51adb4a8820291d906c61f464071c	647 Bytes	README file containing a description of all files in this record

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External references

Keywords

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