Center for Molecular Modeling - L. Joos

Cutting the cost of carbon capture: a case for carbon capture and utilization

lennart — Mon, 14 Mar 2016 12:50:51 +0000

L. Joos, J. Huck, V. Van Speybroeck, B. Smit

Faraday Discussions

192, 391-414

2016

Abstract

A significant part of the cost for Carbon Capture and Storage (CCS) is related to the compression of the captured CO2 to its supercritical state, at 150 bar and typically 99% purity. These stringent conditions may however not always be necessary for specific cases of Carbon Capture and Utilization (CCU). In this manuscript, we investigate how much the parasitic energy of an adsorbent-based carbon capture process may be lowered by utilizing CO2 at 1 bar and adapting the final purity requirement for CO2 from 99% to 70% or 50%. We compare different CO2 sources: the flue gases of coal-fired or natural gas-fired power plants and ambient air. We evaluate the carbon capture performance of over 60 nanoporous materials and determine the influence of the initial and final purity on the parasitic energy of the carbon capture process. Moreover, we demonstrate the underlying principles of the parasitic energy minimization in more detail using the commercially available NaX zeolite. Finally, the calculated utilization cost of CO2 is compared with reported prices for CO2 and published costs for CCS.

Open Access version available at UGent repository

DOI

http://dx.doi.org/10.1039/C6FD00031B

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c6fd00031b.pdf

Carbon Capture Turned Upside Down: High-Temperature Adsorption & Low-Temperature Desorption (HALD)

lennart — Sat, 25 Apr 2015 13:25:55 +0000

L. Joos, K. Lejaeghere, J. Huck, V. Van Speybroeck, B. Smit

Energy & Environmental Science

8, 2480-2491

2015

Abstract

Carbon Capture & Sequestration (CCS) could reduce CO2 emissions from large fossil-fuel power plants in the short term, but the high energy penalty of the process hinders its industrial deployment. Moreover, the utility of nanoporous materials, known to be selective for the CO2/N2 separation, is drastically reduced due to the competitive adsorption with H2O. Taking advantage of the power plant's waste heat to perform CCS while at the same time surmounting the negative effect of H2O is therefore an attractive idea. We propose an upside-down approach for CCS in nanoporous materials, High-temperature Adsorption & Low-temperature Desorption (HALD), that exploits the temperature-dependent competitive adsorption of CO2 and H2O. First, we provide a theoretical background for this entropy-driven behavior and demonstrate under what conditions competitive adsorption can be in favor of CO2 at high temperature and in favor of H2O at low temperature. Then, molecular simulations in all-silica MFI provide a proof of concept. The International Zeolite Association database is subsequently screened for potential candidates and finally, the most promising materials are selected using a post-Pareto search algorithm. The proposed post-Pareto approach is able to select the material that shows an optimal combination of multiple criteria, such as CO2/H2O selectivity, CO2/N2 selectivity, CO2 uptake and H2O uptake. As a conclusion, this work provides new perspectives to reduce the energy requirement for CCS and to overcome the competitive adsorption of H2O.

Open Access version available at UGent repository

DOI

http://dx.doi.org/10.1039/C5EE01690H

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C5EE01690H.pdf

Advances in theory and their application within the field of zeolite chemistry

michel — Tue, 13 Jan 2015 10:39:05 +0000

V. Van Speybroeck, K. Hemelsoet, L. Joos, M. Waroquier, R.G. Bell, C.R.A. Catlow

Chemical Society Reviews

Vol. 44 , 7044-7111

2015

Abstract

Zeolites are versatile and fascinating materials which are vital for a wide range of industries, due to their unique structural and chemical properties, which are the basis of applications in gas separation, ion exchange and catalysis. Given their economic impact, there is a powerful incentive for smart design of new materials with enhanced functionalities to obtain the best material for a given application. Over the last decades, theoretical modeling has matured to a level that model guided design has become within reach. Major hurdles have been overcome to reach this point and almost all contemporary methods in computational materials chemistry are actively used in the field of modeling zeolite chemistry and applications. Integration of complementary modeling approaches is necessary to obtain reliable predictions and rationalizations from theory. A close synergy between experimentalists and theoreticians has led to a deep understanding of the complexity of the system at hand, but also allowed the identification of shortcomings in current theoretical approaches. Inspired by the importance of zeolite characterization which can now be performed at the single atom and single molecule level from experiment, computational spectroscopy has grown in importance in the last decade. In this review most of the currently available modeling tools are introduced and illustrated on the most challenging problems in zeolite science. Directions for future model developments will be given.

Open Access version available at UGent repository

DOI

http://dx.doi.org/10.1039/C5CS00029G

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15_ChemSocRev_44-7044_VanSpeybroeck.pdf

Flexibility versus rigidity: what determines the stability of zeolite frameworks? A case study

michel — Tue, 29 Apr 2014 19:07:20 +0000

E. Verheyen, L. Joos, C. Martineau, C.J. Dawson, C. Weidenthaler, W. Schmidt, R. Yuan, E. Breynaerts, V. Van Speybroeck, M. Waroquier, F. Taulelle, M.M.J. Treacy, J.A. Martens, C. Kirschhock

Materials Horizons

Vol. 1 , 582 - 587

2014

Abstract

All silica COK-14/-COK-14 with OKO topology is the first case of a zeolite which reversibly transforms from a systematically interrupted to a fully connected state and back. Analysis of the opening/closing behavior allowed the study of entropy and framework flexibility as determinants for the stability of zeolite topologies, which, until now, has been experimentally inaccessible. Interconversion of the all-silica COK-14 zeolite with fully connected OKO topology and its -COK-14 variant with systematic framework interruption was investigated using high-temperature XRD, thermogravimetric analysis, Si-29 MAS NMR, nitrogen adsorption and a range of modelling techniques. Specific framework bonds in the OKO framework can be reversibly hydrolyzed and condensed. Structural silanols of the parent -COK-14, prepared by degermanation of the IM-12 zeolite, were condensed by heating at 923 K, and hydrolyzed again to the initial state by contacting the zeolite with warm water. Molecular modelling revealed an inversion of the relative stabilities for both variants depending on temperature and hydration. Condensation of the structural silanols in -COK-14 to COK-14 is entropy driven, mainly resulting from the release of water molecules. Framework reopening in the presence of water is spontaneous due to the high rigidity of the fully connected OKO framework. Isomorphous substitution was demonstrated as a viable option for stabilization of the fully connected OKO framework as this renders the closed framework flexible.

DOI

http://dr.doi.org/10.1039/c4mh00127c

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manuscript mat Hor.pdf

Molecular Simulation Study of the Competitive Adsorption of H2O and CO2 in Zeolite 13X

wim — Mon, 13 Jan 2014 07:18:44 +0000

L. Joos, J.A. Swisher, B. Smit, A. Bruder

Langmuir

29 (48), 14743-14747

2013

Abstract

Surfactants exhibit maxima in their critical micelle concentrations upon application of hydrostatic pressure, which is attributable to changes in their volumes of micellization from positive to negative values with increasing pressure. We present a direct molecular simulation analysis of the volumes of micellization of an anionic, cationic, and nonionic surfactant in aqueous solution at pressures up to 2500 bar. Excellent agreement with experiment is observed. A Kirkwood-Buff theory analysis based on proximal solvent distributions permits the breakdown of the volumes of micellization into constituent surfactant headgroup and tailgroup contributions. Although the micellization volume crossover is analogous to the transfer of an alkane from water to its pure liquid, significant differences are observed, including lower compressibilities of micelle volumes compared to that of the alkane liquid, negative partial compressibilites for anionic sulfated surfactant monomers, and large nonionic ethoxy headgroup contributions to the micellization volume.

DOI

http://dx.doi.org/10.1021/la402798f

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13_Langmuir_29(48)14743_Joos.pdf

Reactivity of CO on carbon covered cobalt surfaces in Fischer-Tropsch Synthesis

michel — Tue, 05 Nov 2013 10:56:39 +0000

L. Joos, I. Filot, S. Cottenier, E. Hensen, M. Waroquier, V. Van Speybroeck, R.A. van Santen

Journal of Physical Chemistry C

118 (10), 5317–5327

2014

Abstract

Fischer–Tropsch synthesis is an attractive process to convert alternative carbon sources, such as biomass, natural gas, or coal, to fuels and chemicals. Deactivation of the catalyst is obviously undesirable, and for a commercial plant it is of high importance to keep the catalyst active as long as possible during operating conditions. In this study, the reactivity of CO on carbon-covered cobalt surfaces has been investigated by means of density functional theory (DFT). An attempt is made to provide insight into the role of carbon deposition on the deactivation of two cobalt surfaces: the closed-packed Co(0001) surface and the corrugated Co(112̅1) surface. We also analyzed the adsorption and diffusion of carbon atoms on both surfaces and compared the mobility. Finally, the results for Co(0001) and Co(112̅1) are compared, and the influence of the surface topology is assessed.

DOI

http://dx.doi.org/10.1021/jp4109706

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14_JPhysChemC_118,5317_Joos.pdf

Entropy-Driven Chemisorption of NOx on Phosphotungstic Acid

michel — Fri, 17 Aug 2012 06:49:36 +0000

S. Heylen, L. Joos, V. Van Speybroeck, C. Kirschhock, J.A. Martens

Angewandte Chemie int. Ed.

51 (44), 11010-11013

2012

Abstract

Nitrogen oxides, NOx, are formed in combustion engines. They contribute to acid rain and the formation of ozone and are hazardous for men and environment. In this article, a process was investigated that can 'capture' the NOx from the exhaust gases using heteropoly acids and can later release them for processing. One of the main conclusions is that the mobility of the captured and released molecules is the key to control the reaction. This can now be used to optimize and commercialize the technology.

Stikstofoxiden, aangeduid als NOx, worden gevormd in verbrandingsmotoren. Ze dragen bij tot zure regen, de vorming van ozon en zijn dus schadelijk voor mens en milieu. In dit artikel werd een proces onderzocht dat de NOx kan ‘vangen’ uit de uitlaatgassen aan de hand van heteropolyzuren en later terug kan vrijgeven voor verdere verwerking. Een van de belangrijkste vaststellingen is dat de mobiliteit van de opgeslagen en vrijgegeven moleculen de sleutel is voor het controleren van het proces. De conclusies van het onderzoek kunnen nu verder gebruikt worden voor de optimalisering en commercialisering van het proces.

http://www.ugent.be/nl/actueel/nieuws/persberichten/stikstofoxide-nox-ve...

NOx adsorption on Phosphotungstic acid is entropy-driven due to the watermolecules that are released.

DOI

http://dx.doi.org/10.1002/ange.201205636

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12 angewandte chem 51(44)11010 Heylen.pdf

Effect of carbon fouling of cobalt surfaces on the reactivity of CO in Fischer-Tropsch synthesis

samuel — Thu, 06 Feb 2020 12:44:35 +0000

L. Joos, I. Filot, M. Waroquier, S. Cottenier, V. Van Speybroeck, R.A. van Santen

ISBN/ISSN:

Talk

Conference / event / venue

14th International Conference on Theoretical Aspects of Catalysis (ICTAC-14 - 2012)

Vlissingen, The Netherlands

Tuesday, 26 June, 2012 to Saturday, 30 June, 2012

Modelling - from molecules to megascale: general discussion

wim — Wed, 15 Feb 2017 12:28:15 +0000

B. Smit, P. Styring, W. Grant, G. Rochelle, F. Donat, J. Yao, M. Trusler, C. Adjiman, S. Lyth, J.S.M. Lee, T. Hills, P. Brandl, M. Gazzani, R. Cuellar-Franca, P. Fennell, D. Sutter, M. Bui, C. Scholes, G. Dowson, J. Gibbins, L. Joss, G. Maitland, S. Brandani, P. Garcia-Gutierrez, Y. Zhang, C. Muller, G. Jackson, R. Ocone, L. Joos, R. Bell, R. Graham, A. Barasinski

FARADAY DISCUSSIONS

2016

Modelling – from molecules to mega-scale: general discussion

Research stay @ EPFL

wim — Mon, 18 Jan 2016 09:24:00 +0000

Sion, Switzerland

Monday, 1 February, 2016 to Tuesday, 31 May, 2016

Participant(s)

L. Joos

Project ref.

FWO L. Joos B/12987/01