Free energy landscapes for the thermodynamic understanding of adsorption-induced deformations and structural transitions in porous materials
作者： D. Bousquet , F.-X. Coudert , A. Boutin
DOI: 10.1063/1.4738776
关键词: Boltzmann equation 、 Boltzmann constant 、 Chemical physics 、 Porous medium 、 Metastability 、 Volume (thermodynamics) 、 Adsorption 、 Monte Carlo method 、 Thermodynamic equilibrium 、 Materials science
摘要: Soft porous crystals are flexible metal-organic frameworks that respond to physical stimuli such as temperature, pressure, and gas adsorption by large changes in their structure unit cell volume. While they have attracted a lot of interest, molecular simulation methods directly couple structural deformations an efficient manner still lacking. We propose here new Monte Carlo method based on non-Boltzmann sampling (guest loading, volume) space using the Wang–Landau algorithm, show it can be used fully characterize properties material's response at thermodynamic equilibrium. showcase this simple model MIL-53 family breathing materials, demonstrating its potential contrasting with pitfalls direct, Boltzmann simulations. furthermore explanation for hysteretic nature terms free energy barriers between two metastable host phases.
harvard.edu
scitation.org
aip.org
coudert.name 参考文章(35)
Zhenqiang Wang, Seth M. Cohen, Modulating metal-organic frameworks to breathe: a postsynthetic covalent modification approach. Journal of the American Chemical Society. ,vol. 131, pp. 16675- 16677 ,(2009) , 10.1021/JA907742Z
Fabien Cailliez, Mickael Trzpit, Michel Soulard, Isabelle Demachy, Anne Boutin, Joël Patarin, Alain H. Fuchs, Thermodynamics of water intrusion in nanoporous hydrophobic solids Physical Chemistry Chemical Physics. ,vol. 10, pp. 4817- 4826 ,(2008) , 10.1039/B807471B
Chenggang Zhou, R. N. Bhatt, Understanding and improving the Wang-Landau algorithm. Physical Review E. ,vol. 72, pp. 025701- ,(2005) , 10.1103/PHYSREVE.72.025701
C. Serre, S. Bourrelly, A. Vimont, N. A. Ramsahye, G. Maurin, P. L. Llewellyn, M. Daturi, Y. Filinchuk, O. Leynaud, P. Barnes, G. Férey, An Explanation for the Very Large Breathing Effect of a Metal–Organic Framework during CO2 Adsorption Advanced Materials. ,vol. 19, pp. 2246- 2251 ,(2007) , 10.1002/ADMA.200602645
Fugao Wang, D. P. Landau, Efficient, multiple-range random walk algorithm to calculate the density of states. Physical Review Letters. ,vol. 86, pp. 2050- 2053 ,(2001) , 10.1103/PHYSREVLETT.86.2050
Naseem A. Ramsahye, Guillaume Maurin, Sandrine Bourrelly, Philip L. Llewellyn, Thierry Loiseau, Christian Serre, Gérard Férey, On the breathing effect of a metal–organic framework upon CO2 adsorption: Monte Carlo compared to microcalorimetry experiments Chemical Communications. ,vol. 31, pp. 3261- 3263 ,(2007) , 10.1039/B702986A
Marie Jeffroy, François-Xavier Coudert, Anne Boutin, Alain H. Fuchs, Caroline Mellot-Draznieks, Thermodynamics of guest-induced structural transitions in hybrid organic-inorganic frameworks. Journal of the American Chemical Society. ,vol. 130, pp. 14294- 14302 ,(2008) , 10.1021/JA805129C
Manan Chopra, Marcus Müller, Juan José de Pablo, None, Order-parameter-based Monte Carlo simulation of crystallization The Journal of Chemical Physics. ,vol. 124, pp. 134102- 134102 ,(2006) , 10.1063/1.2178324
Marie Jeffroy, Alain H. Fuchs, Anne Boutin, Structural changes in nanoporous solids due to fluid adsorption: thermodynamic analysis and Monte Carlo simulations Chemical Communications. pp. 3275- 3277 ,(2008) , 10.1039/B805117H
A. Ghoufi, G. Maurin, Hybrid Monte Carlo Simulations Combined with a Phase Mixture Model to Predict the Structural Transitions of a Porous Metal−Organic Framework Material upon Adsorption of Guest Molecules Journal of Physical Chemistry C. ,vol. 114, pp. 6496- 6502 ,(2010) , 10.1021/JP911484G