Center for Molecular Modeling - BOF J.J. Gutierrez-Sevilano BOFPDO2016000101

Modeling Gas Adsorption in Flexible Metal–Organic Frameworks via Hybrid Monte Carlo / Molecular Dynamics Schemes

sven — Fri, 21 Dec 2018 13:00:52 +0000

S.M.J. Rogge, R. Goeminne, R. Demuynck, J.J. Gutiérrez-Sevillano, S. Vandenbrande, L. Vanduyfhuys, M. Waroquier, T. Verstraelen, V. Van Speybroeck

Advanced Theory and Simulations

2 (4), 1800177

2019

Abstract

Herein, a hybrid Monte Carlo (MC)/molecular dynamics (MD) simulation protocol that properly accounts for the extraordinary structural flexibility of metal–organic frameworks (MOFs) is developed and validated. This is vital to accurately predict gas adsorption isotherms and guest‐induced flexibility of these materials. First, the performance of three recent models to predict adsorption isotherms and flexibility in MOFs is critically investigated. While these methods succeed in providing qualitative insight in the gas adsorption process in MOFs, their accuracy remains limited as the intrinsic flexibility of these materials is very hard to account for. To overcome this challenge, a hybrid MC/MD simulation protocol that is specifically designed to handle the flexibility of the adsorbent, including the shape flexibility, is introduced, thereby unifying the strengths of the previous models. It is demonstrated that the application of this new protocol to the adsorption of neon, argon, xenon, methane, and carbon dioxide in MIL‐53(Al), a prototypical flexible MOF, substantially decreases the inaccuracy of the obtained adsorption isotherms and predicted guest‐induced flexibility. As a result, this method is ideally suited to rationalize the adsorption performance of flexible nanoporous materials at the molecular level, paving the way for the conscious design of MOFs as industrial adsorbents.

Gold Open Access

DOI

http://dx.doi.org/10.1002/adts.201800177

Private attachment

main.pdf

Methane Adsorption in Zr-Based MOFs: Comparison and Critical Evaluation of Force Fields

michel — Mon, 11 Sep 2017 13:28:25 +0000

S. Vandenbrande, T. Verstraelen, J. J. Gutierrez-Sevillano, M. Waroquier, V. Van Speybroeck

Journal of Physical Chemistry C

121 (45), 25309-25322

2017

Abstract

The search for nanoporous materials that are highly performing for gas storage and separation is one of the contemporary challenges in material design. The computational tools to aid these experimental efforts are widely available and adsorption isotherms are routinely computed for huge sets of (hypothetical) frameworks. Clearly the computational results depend on the interactions between the adsorbed species and the adsorbent, which are commonly described using force fields. In this paper, an extensive comparison and in-depth investigation of several force fields from literature is reported for the case of methane adsorption in the Zr-based Metal-Organic Frameworks UiO-66, UiO-67, DUT-52, NU-1000 and MOF-808. Significant quantitative differences in the computed uptake are observed when comparing different force fields, but most qualitative features are common which suggests some predictive power of the simulations when it comes to these properties. More insight into to the host-guest interactions is obtained by benchmarking the force fields with an extensive number of ab initio computed single molecule interaction energies. This analysis at the molecular level reveals that especially ab initio derived force fields perform well in reproducing the ab initio interaction energies. Finally, the high sensitivity of uptake predictions on the underlying potential energy surface is explored.

Open Access version available at UGent repository

Gold Open Access

DOI

http://dx.doi.org/10.1021/acs.jpcc.7b08971

Private attachment

acs.jpcc_.7b08971.pdf

J.J. Gutierrez

wim — Wed, 29 Mar 2017 08:06:44 +0000

Project promotor

T. Verstraelen

Financierende instantie

BOF-postdoc

Project data

01/01/2016 to 31/12/2018

Mandaatmaanden

Project titel

BOF15/PDO/075

Personeel

J.J. Gutiérrez-Sevillano

Project ref.

BOF J.J. Gutierrez-Sevilano BOFPDO2016000101

40th Iberian Adsorption Meeting

wim — Tue, 02 Aug 2016 12:02:45 +0000

Évora, Portugal

Monday, 5 September, 2016 to Wednesday, 7 September, 2016

Participant(s)

J.J. Gutiérrez-Sevillano

Project ref.

BOF J.J. Gutierrez-Sevilano BOFPDO2016000101

Conference reference

40th Iberian Adsorption Meeting

Juan José Gutiérrez Sevillano

wim — Mon, 11 Jan 2016 09:30:27 +0000