Center for Molecular Modeling - G. Maurin

High-performance hydrophobic MOFs for selective acetone capture under humid conditions

louis — Tue, 20 Jan 2026 10:05:26 +0000

S. Grigoletto, K. Karami, I. Maye, A. Padunnappattu, S. Ravichandran, M. Wahiduzzaman, L. Vanduyfhuys, V. Van Speybroeck, M. Thommes, J.F.M. Denayer, N. Stock, G. Maurin

Journal of Materials Chemistry A

13, 26401-26412

2025

Abstract

Capturing acetone, a major indoor air pollutant, under humid conditions is a longstanding challenge in materials science. The key obstacle lies in finding porous adsorbents that simultaneously exhibit strong affinity for acetone and intrinsic hydrophobicity, a rare and elusive pairing. Leveraging the structural and chemical versatility of metal-organic frameworks (MOFs), we first explored a diverse set of MOFs using force field Monte Carlo and density-functional theory calculations. This computational strategy identified CAU-11(Al) as a top performer: a hydrophobic, small pore MOF that enables both high acetone affinity and uptake at trace concentrations with excellent selectivity over water. Experimental validation through gas-phase pulse chromatography, adsorption measurements, and breakthrough studies confirmed the outstanding performance of this sorbent under competitive acetone/water conditions. These results position CAU-11(Al) as a promising material for real-world acetone capture in humid indoor environments.

Gold Open Access

DOI

http://dx.doi.org/

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Artificial Intelligence Paradigms for Next-Generation Metal–Organic Framework Research

sven — Tue, 24 Jun 2025 08:59:53 +0000

A. Ozcan, F.-X. Coudert, S.M.J. Rogge, G. Heydenrych, D. Fan, A. P. Sarikas, S. Keskin, G. Maurin, G. E. Froudakis, S. Wuttke, I. Erucar

JACS (Journal of the American Chemical Society)

147, 27, 23367–23380

2025

Abstract

After the development of the famous “Transformer” network architecture and the meteoric rise of artificial intelligence (AI)-powered chatbots, large language models (LLMs) have become an indispensable part of our daily activities. In this rapidly evolving era, “all we need is attention” as Google’s famous transformer paper’s title [Vaswani et al., Adv. Neural Inf. Process. Syst. 2017, 30] implies: We need to focus on and give “attention” to what we have at hand, then consider what we can do further. What can LLMs offer for immediate short-term adaptation? Currently, the most common applications in metal–organic framework (MOF) research include automating literature reviews and data extraction to accelerate the material discovery process. In this perspective, we discuss the latest developments in machine-learning and deep-learning research on MOF materials and reflect on how their utilization has evolved within the LLM domain from this standpoint. We finally explore future benefits to accelerate and automate materials development research.

Open Access version available at UGent repository

Gold Open Access

DOI

http://dx.doi.org/10.1021/jacs.5c08214

Materials for a changing planet

mieke — Wed, 21 Dec 2022 12:57:18 +0000

V. Van Speybroeck, G. Maurin

Nature Materials

Volume: 22, Issue: 1, Pages: 12-13

2023

Abstract

About 700 scientists from 45 countries gathered in Dresden for the first time since the start of the COVID-19 pandemic to share their latest findings on metal-organic frameworks and open frameworks compounds.

DOI

http://dx.doi.org/10.1038/s41563-022-01419-7

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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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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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Frontiers in Modeling Metal–Organic Frameworks

samuel — Wed, 22 Jan 2020 12:38:30 +0000

B. Civalleri, G. Maurin, V. Van Speybroeck

Advanced Theory and Simulations

2, 1900196

2019

Open Access version available at UGent repository

Gold Open Access

DOI

https://doi.org/10.1002/adts.201900196

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Thermodynamic modeling of the selective adsorption of carbon dioxide over methane in the mechanically constrained breathing MIL-53(Cr)

louis — Mon, 26 Aug 2019 16:10:44 +0000

L. Vanduyfhuys, G. Maurin

Advanced Theory and Simulations

1900124

2019

Abstract

The coadsorption of CO2/CH4 in the breathing MIL-53(Cr) under the application of an additional mechanical pressure is investigated through the use of an extended thermodynamic mean-field model. The focus is on the breathing behavior, negative gas adsorption (NGA), and selective adsorption of CO2 as well as to what degree the application of mechanical pressure influences this behavior. To this end, phase diagrams, coadsorption isotherms are constructed and the CO 2 /CH 4 selectivity is computed in terms of the vapor pressure of methane and carbon dioxide as well as the mechanical pressure. As a result, it was found that NGA can be induced by coadsorption of CO2 /CH4 gas mixtures with certain molar compositions. Finally, a specific adsorption/desorption cycle, which includes the application of an additional mechanical pressure, is proposed to allow for an increased CO2/CH4 selectivity as well as for an expected less energy demanding CO2 desorption step.

DOI

http://dx.doi.org/10.1002/adts.201900124

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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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Thermodynamic insight into stimuli-responsive behavior of soft porous crystals

michel — Sat, 11 Nov 2017 15:22:43 +0000

L. Vanduyfhuys, S.M.J. Rogge, J. Wieme, S. Vandenbrande, G. Maurin, M. Waroquier, V. Van Speybroeck

Nature Communications

9, 1, 204

2018

Abstract

Knowledge of the thermodynamic potential in terms of the independent variables allows to characterize the macroscopic state of the system. However, in practice, it is difficult to access this potential experimentally due to irreversible transitions that occur between equilibrium states. A showcase example of sudden transitions between (meta)stable equilibrium states is observed for soft porous crystals possessing a network with long-range structural order, which can transform between various states upon external stimuli such as pressure, temperature and guest adsorption. Such phase transformations are typically characterized by large volume changes and may be followed experimentally by monitoring the volume change in terms of certain external triggers. Herein, we present a generalized thermodynamic approach to construct the underlying Helmholtz free energy as a function of the state variables that governs the observed behaviour based on microscopic simulations. This concept allows a unique identification of the conditions under which a material becomes flexible.

Open Access version available at UGent repository

Gold Open Access

DOI

http://dx.doi.org/10.1038/s41467-017-02666-y

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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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