Monte Carlo Potential Energy Sampling for Molecular Entropy in Zeolites
Artikel i vetenskaplig tidskrift, 2018

Zeolites are widely applied as molecular sieves and porous host materials for active sites in heterogeneous catalysis. Adsorption and reaction kinetics depend critically on the molecular entropy in the zeolite. In this work, we introduce a method to calculate the entropy of molecules in zeolites using Monte Carlo integration of the semiclassical partition function. The method is demonstrated for N-2 and CH4 in chabazite and MFI silicalites. We find that the molecular entropy is lowered by a factor between 1/3 and 1/2 with respect to the gas-phase value. The results are corroborated by explicit molecular dynamics simulations revealing the active molecular degrees of freedom. The possibility of accurate entropy estimations opens up for an improved description of catalytic reactions and sorption phenomena in zeolites.


Mikkel Jørgensen

Kompetenscentrum katalys

Chalmers, Fysik, Kemisk fysik

Lin Chen

Chalmers, Fysik, Kemisk fysik

Kompetenscentrum katalys

Henrik Grönbeck

Kompetenscentrum katalys

Chalmers, Fysik, Kemisk fysik

Journal of Physical Chemistry C

1932-7447 (ISSN) 1932-7455 (eISSN)

Vol. 122 35 20351-20357

Länk mellan katalytisk aktivitet och kvantmekaniska beräkningar

Vetenskapsrådet (VR) (2016-05234), 2017-01-01 -- 2020-12-31.


Nanovetenskap och nanoteknik



Fysikalisk kemi

Teoretisk kemi

Den kondenserade materiens fysik


C3SE (Chalmers Centre for Computational Science and Engineering)



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