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Structural transformations during dehydroxylation reactions of UiO-66 type metal-organic frameworks

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Fri, 14/11/2014 - 13:45 -- mat

Description 

This project aims at understanding the dehydroxylation behaviour of the Metal-Organic Framework UiO-66 (Zirconium terephthalate), with structural formula Zr6O4(OH)4[terephthalate]6. When placed in vacuum at high temperatures, this material loses its hydroxyl (OH) groups. During this dehydroxylation process water is removed from the framework. It is highly important to investigate dehydroxylation processes, as these lead to more catalytically active UiO-66 type materials.

In this work, climbing image Nudged Elastic Band (cNEB) simulations are needed (1) to unravel reaction pathways of dehydroxylation, (2) to find good initial guesses for transition state structures, and (3) to obtain accurate insight in the active sites after dehydroxylation. To study the dehydroxylation pathways, we will use cNEB simulations making use of the periodic code VASP. Due to the size of the systems and the fact that several images are running in parallel, the amount of calculations that need to be performed goes beyond what can comfortably be done (within a reasonable timeframe) on a TIER2 cluster. The queuing times for such large jobs (16 nodes) can easily go up to one week, and this project requires 59 of this type of calculations.

The obtained insight into the active sites after such a dehydroxylation treatment and their energetic relevance is highly relevant for the Zr-MOF community, and can then be used for further computational studies.

Budget/project

FWO M. Vandichel FWO3E02013004201, FWO MOFs (3G048612) B/12561/*

Period 

Saturday, 15 November, 2014 to Thursday, 30 April, 2015

Node days 

4 720.00 days

Users

M. Vandichel, J. Hajek

Remaining days 

4 720.00 days

TIER1 reference n°

2014-043

Status 

Approved

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