Center for Molecular Modeling - B. Smit

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

Private attachment

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

Private attachment

C5EE01690H.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

Private attachment

13_Langmuir_29(48)14743_Joos.pdf

On the thermodynamics of framework breathing: A free energy model for gas adsorption in MIL-53

michel — Fri, 09 Nov 2012 10:02:18 +0000

A. Ghysels, L. Vanduyfhuys, M. Vandichel, M. Waroquier, V. Van Speybroeck, B. Smit

Journal of Physical Chemistry C

117, 11540-11554

2013

Abstract

When adsorbing guest molecules, the porous metal-organic framework MIL-53(Cr) may vary its cell parameters drastically while retaining its crystallinity. A first approach to the thermodynamic analysis of this 'framework breathing' consists of comparing the osmotic potential in two distinct shapes only (large-pore and narrow-pore). In this paper, we propose a generic parametrized free energy model including three contributions: host free energy, guest-guest interactions, and host-guest interaction. Free energy landscapes may now be constructed scanning all shapes and any adsorbed amount of guest molecules. This allows to determine which shapes are the most stable states for arbitrary combinations of experimental control parameters, such as the adsorbing gas chemical potential, the external pressure, and the temperature. The new model correctly reproduces the structural transitions along the CO₂ and CH₄ isotherms. Moreover, our model successfully explains the adsorption versus desorption hysteresis as a consequence of the creation, stabilization, destabilization, and disappearance of a second free energy minimum under the assumptions of a first order phase transition and collective behavior. Our general thermodynamic description allows to decouple the gas chemical potential μ and mechanical pressure P as two independent thermodynamic variables and predict the complete (μ,P) phase diagram for CO₂ adsorption in MIL-53(Cr). The free energy model proposed here is an important step towards a general thermodynamics description of flexible metal-organic frameworks.

DOI

http://dx.doi.org/10.1021/jp311601q

Private attachment

Ghysels-JPCC-2013-FreeEnergyModelMIL-53.pdf

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

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

lennart — Mon, 22 Jun 2015 06:19:54 +0000

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

ISBN/ISSN:

Invited talk

Conference / event / venue

Visit group of Prof. Geoffroy Hautier

Louvain-la-Neuve

Tuesday, 23 June, 2015

From Accurate Models to Zero Emissions

lennart — Fri, 12 Jun 2015 08:14:44 +0000

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

ISBN/ISSN:

Poster

Conference / event / venue

15th FEA Research Symposium

Gent, Belgium

Friday, 5 December, 2014

Carbon Capture Turned Upside Down with HALD: High-temperature Adsorption & Low-temperature Desorption

lennart — Fri, 12 Jun 2015 08:11:53 +0000

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

ISBN/ISSN:

Poster

Conference / event / venue

Gordon Research Conference

Easton, MA, USA

Sunday, 31 May, 2015 to Friday, 5 June, 2015

Conference reference

Carbon Capture Utilization & Storage (GRC)

Free energy profile of "breathing" flexible porous frameworks

wim — Mon, 07 May 2012 08:01:37 +0000

A. Ghysels, V. Van Speybroeck, M. Waroquier, B. Smit

P13

Poster

Conference / event / venue

DFTM2012

Ghent University, Het Pand, Ghent, Belgium

Sunday, 1 April, 2012 to Friday, 6 April, 2012

Abstract (private)

DFTM2012_AGhysels.pdf

Conference reference

DFTM2012

Monte carlo simulations to understand "breathing" phenomenon of metal organic Frameworks

wim — Mon, 21 Nov 2011 15:34:50 +0000

A. Ghysels, V. Van Speybroeck, M. Waroquier, B. Smit

Abstract PI 269

Poster

Conference / event / venue

Ninth Triennial Congress of the World Association of Theoretical and Computational Chemists (WATOC)

Santiago de Compostela, Spain

Sunday, 17 July, 2011 to Friday, 22 July, 2011

Abstract

2011 WATOC AG 269.pdf

Conference reference

WATOC 2011