Center for Molecular Modeling - P.G. Yot

Crystals springing into action: metal-organic framework CUK-1 as a pressure-driven molecular spring dagger

louis — Tue, 18 May 2021 12:38:53 +0000

P. Iacomi, J.S. Lee, L. Vanduyfhuys, K. H. Cho, P. Fertey, J. Wieme, D. Granier, G. Maurin, V. Van Speybroeck, J.-S. Chang, P.G. Yot

Chemical Science

12, 5682-5687

2021

Abstract

Mercury porosimetry and in situ high pressure single crystal X-ray diffraction revealed the wine-rack CUK-1 MOF as a unique crystalline material capable of a fully reversible mechanical pressure-triggered structural contraction. The near-absence of hysteresis upon cycling exhibited by this robust MOF, akin to an ideal molecular spring, is associated with a constant work energy storage capacity of 40 J/gr. Molecular simulations were further deployed to uncover the free-energy landscape behind this unprecedented pressure-responsive phenomenon in the area of compliant hybrid porous materials. This discovery is of utmost importance from the perspective of instant energy storage and delivery.

Open Access version available at UGent repository

Green Open Access

DOI

http://dx.doi.org/10.1039/D1SC00205H

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published.pdf

Charting the Metal-Dependent High-Pressure Stability of Bimetallic UiO-66 Materials

sven — Fri, 20 Mar 2020 17:16:34 +0000

S.M.J. Rogge, P.G. Yot, J. Jacobsen, F. Muniz-Miranda, S. Vandenbrande, J. Gosch, V. Ortiz, I. Collings, S. Devautour-Vinot, G. Maurin, N. Stock, V. Van Speybroeck

ACS Materials Letters

2 (4), 438-445

2020

Abstract

In theory, bimetallic UiO-66(Zr:Ce) and UiO-66(Zr:Hf) metal-organic frameworks (MOFs) are extremely versatile and attractive nanoporous materials as they combine the high catalytic activity of UiO-66(Ce) or UiO-66(Hf) with the outstanding stability of UiO-66(Zr). Using in situ high-pressure powder X-ray diffraction, however, we observe that this expected mechanical stability is not achieved when incorporating cerium or hafnium in UiO-66(Zr). This observation is akin to the earlier observed reduced thermal stability of UiO-66(Zr:Ce) compounds. To elucidate the atomic origin of this phenomenon, we chart the loss-of-crystallinity pressures of 22 monometallic and bimetallic UiO-66 materials and systematically isolate their intrinsic mechanical stability from their defect-induced weakening. This complementary experimental/computational approach reveals that the intrinsic mechanical stability of these bimetallic MOFs decreases nonlinearly upon cerium incorporation but remains unaffected by the zirconium:hafnium ratio. Additionally, all experimental samples suffer from defect-induced weakening, a synthesis-controlled effect that is observed to be independent of their intrinsic stability.

Gold Open Access

DOI

http://dx.doi.org/10.1021/acsmaterialslett.0c00042

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acsmaterialslett.0c00042.pdf

Pillared-layered metal-organic frameworks for mechanical energy storage applications

jelle — Thu, 01 Aug 2019 08:13:25 +0000

J. Wieme, S.M.J. Rogge, P.G. Yot, L. Vanduyfhuys, S.-K. Lee, J.-S. Chang, M. Waroquier, G. Maurin, V. Van Speybroeck

Journal of Materials Chemistry A

7 (39), 22663-22674

2019

Abstract

Herein we explore the unique potential of pillared-layered metal–organic frameworks of the DMOF-1 family for mechanical energy storage applications. In this work, we theoretically predict for the guest-free DMOF-1 a new contracted phase by exerting an external mechanical pressure of more than 200 MPa with respect to the stable phase at atmospheric pressure. The breathing transition is accompanied by a very large volume contraction of about 40%. The high transition pressures and associated volume changes make these materials highly promising with an outstanding mechanical energy work. Furthermore, we show that changing the nature of the metal allows to tune the behavior under mechanical pressure. The various phases were revealed by a combination of periodic density-functional theory calculations, force field molecular dynamics simulations and mercury intrusion experiments for DMOF-1(Zn) and DMOF-1(Cu). The combined experimental and theoretical approach allowed to discover the potential of these materials for new technological developments.

Gold Open Access

DOI

http://dx.doi.org/10.1039/C9TA01586H

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c9ta01586h.pdf

Mechanical properties of a gallium fumarate metal-organic framework: a joint experimental-modelling exploration

jelle — Mon, 15 May 2017 07:14:56 +0000

P. Ramaswamy, J. Wieme, E. Alvarez, L. Vanduyfhuys, J.-P. Itié, P. Fabry, V. Van Speybroeck, C. Serre, P.G. Yot, G. Maurin

Journal of Materials Chemistry A

5 (22), 11047-11054

2017

Abstract

A gallium analogue of the commercially available Al-fumarate MOF A520 - recently identified as isotypic to MIL-53(Al)-BDC - has been synthesized and further characterized in its hydrated and dehydrated forms. The structural response under applied mechanical pressure of this MIL-53(Ga)-FA solid was investigated using advanced experimental techniques coupled with computational tools. Hg porosimetry and high-pressure X-Ray Powder Diffraction (XRPD) experiments evidenced that the pristine dehydrated large pore form undergoes an irreversible structure contraction upon an applied pressure of 85 MPa with an associated volume change of ca. 14% which makes this material promising for mechanical energy storage applications, in particular as a shock absorber. The breathing behavior was further rationalized performing a series of periodic Density Functional Theory (DFT) calculations with the construction of an energy profile as a function of volume for both MIL-53(Ga)-FA and its Aluminum analogue. As such we could fully unravel the microscopic origin of the difference in pressure-induced behavior for the aluminum and gallium fumarate based materials.

DOI

http://dx.doi.org/10.1039/C7TA01559C

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Ramaswamy2017.pdf

Mechanical energy storage performance of an aluminum fumarate metal-organic framework

louis — Mon, 14 Sep 2015 07:56:46 +0000

P.G. Yot, L. Vanduyfhuys, E. Alvarez, J. Rodriguez, J.-P. Itié, P. Fabry, N. Guillou, T. Devic, P.L. Llewellyn, V. Van Speybroeck, C. Serre, G. Maurin

Chemical Science

7, 446-450

2016

Abstract

The aluminum fumarate MOF A520 or MIL-53-FA is revealed to be a promising material for mechanical energy-related applications with performances in terms of work and heat energies which surpass those of any porous solids reported so far. Complementary experimental and computational tools are deployed to finely characterize and understand the pressure-induced structural transition at the origin of these unprecedented levels of performance.

Open Access version available at UGent repository

DOI

http://dx.doi.org/10.1039/C5SC02794B

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16-ChemSience-7(2016)446-Yot.pdf

ACL Chem Sci Al-Fum.pdf

Metal-organic frameworks as potential shock absorbers: the case of the highly flexible MIL-53(Al)

michel — Thu, 22 May 2014 12:44:21 +0000

P.G. Yot, Z. Boudene, J. Macia, D. Granier, L. Vanduyfhuys, T. Verstraelen, V. Van Speybroeck, T. Devic, C. Serre, G. Ferey, N. Stock, G. Maurin

Chemical Communications

50, 9462-9464

2014

Abstract

The mechanical energy absorption ability of the highly flexible; MIL-53(Al) MOF material was explored using a combination of; experiments and molecular simulations. A pressure-induced transition; between the large pore and the closed pore forms of this solid; was revealed to be irreversible and associated with a relatively large; energy absorption capacity. Both features make MIL-53(Al) the first; potential MOF candidate for further use as a shock absorber.

Open Access version available at UGent repository

DOI

http://dx.doi.org/10.1039/c4cc03853c

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14_chemcomm_50,9462_Yot.pdf

Impact of the mechanical pressure under various conditions on the flexibility of various metal-organic frameworks

jelle — Mon, 25 Sep 2017 14:08:51 +0000

P.G. Yot, P. Ramaswamy, J. Wieme, L. Vanduyfhuys, C. Serre, V. Van Speybroeck, G. Maurin

ISBN/ISSN:

Talk

Conference / event / venue

EUROMAT 2017

Thessaloniki, Greece

Sunday, 17 September, 2017 to Friday, 22 September, 2017