Enhanced replica exchange reactive Monte Carlo simulations for constructing zeolite frameworks

Cecilia Quijano, Scott M. Auerbach, Peter A. Monson

Research output: Contribution to journalArticle

3 Citations (Scopus)

Abstract

We investigate the ability of a reactive model of silica to build crystalline zeolite frameworks with an enhanced sampling approach based on replica exchange Monte Carlo (REMC) simulations. In our implementation of REMC, the silica hydrolysis/condensation equilibrium constant controlling network formation is chosen as the index parameter characterising each replica. We show that improving the performance of the REMC method by increasing its efficiency in producing zeolite crystals allows zeolites with larger unit cells to be constructed. In particular, we perform an efficiency case study on the sodalite structure, containing 12 tetrahedra per unit cell and then apply the resulting enhancements to construct a significantly larger zeolite. We have improved our simulations in two ways; first, we have analysed the roles of the Monte Carlo parameters on the efficiency of this REMC method. Second, we have implemented an adaptive protocol that resets the values of the hydrolysis/condensation equilibrium constants among the replicas, ‘on the fly’ of each simulation, to optimise replica exchange for the purpose of constructing zeolite crystals. Finally, we show that by applying these enhancements, the REMC method can produce the crystal structure of zeolite AWW, a nanoporous material with 24 tetrahedra per unit cell.

Original languageEnglish (US)
Pages (from-to)453-462
Number of pages10
JournalMolecular Simulation
Volume44
Issue number6
DOIs
StatePublished - Apr 13 2018
Externally publishedYes

Fingerprint

Zeolites
Replica
replicas
Monte Carlo methods
Monte Carlo Simulation
Equilibrium constants
Condensation
Hydrolysis
Silica
Crystals
simulation
Monte Carlo method
Silicon Dioxide
Triangular pyramid
Crystal structure
tetrahedrons
Sampling
Crystalline materials
Unit
hydrolysis

Keywords

  • Replica exchange Monte Carlo
  • Self Assembly
  • Silica Polymerisation
  • Zeolites

ASJC Scopus subject areas

  • Chemistry(all)
  • Information Systems
  • Modeling and Simulation
  • Chemical Engineering(all)
  • Materials Science(all)
  • Condensed Matter Physics

Cite this

Enhanced replica exchange reactive Monte Carlo simulations for constructing zeolite frameworks. / Quijano, Cecilia; Auerbach, Scott M.; Monson, Peter A.

In: Molecular Simulation, Vol. 44, No. 6, 13.04.2018, p. 453-462.

Research output: Contribution to journalArticle

@article{e85226984ae240e2bee991f78a2474e5,
title = "Enhanced replica exchange reactive Monte Carlo simulations for constructing zeolite frameworks",
abstract = "We investigate the ability of a reactive model of silica to build crystalline zeolite frameworks with an enhanced sampling approach based on replica exchange Monte Carlo (REMC) simulations. In our implementation of REMC, the silica hydrolysis/condensation equilibrium constant controlling network formation is chosen as the index parameter characterising each replica. We show that improving the performance of the REMC method by increasing its efficiency in producing zeolite crystals allows zeolites with larger unit cells to be constructed. In particular, we perform an efficiency case study on the sodalite structure, containing 12 tetrahedra per unit cell and then apply the resulting enhancements to construct a significantly larger zeolite. We have improved our simulations in two ways; first, we have analysed the roles of the Monte Carlo parameters on the efficiency of this REMC method. Second, we have implemented an adaptive protocol that resets the values of the hydrolysis/condensation equilibrium constants among the replicas, ‘on the fly’ of each simulation, to optimise replica exchange for the purpose of constructing zeolite crystals. Finally, we show that by applying these enhancements, the REMC method can produce the crystal structure of zeolite AWW, a nanoporous material with 24 tetrahedra per unit cell.",
keywords = "Replica exchange Monte Carlo, Self Assembly, Silica Polymerisation, Zeolites",
author = "Cecilia Quijano and Auerbach, {Scott M.} and Monson, {Peter A.}",
year = "2018",
month = "4",
day = "13",
doi = "10.1080/08927022.2017.1399375",
language = "English (US)",
volume = "44",
pages = "453--462",
journal = "Molecular Simulation",
issn = "0892-7022",
publisher = "Taylor and Francis Ltd.",
number = "6",

}

TY - JOUR

T1 - Enhanced replica exchange reactive Monte Carlo simulations for constructing zeolite frameworks

AU - Quijano, Cecilia

AU - Auerbach, Scott M.

AU - Monson, Peter A.

PY - 2018/4/13

Y1 - 2018/4/13

N2 - We investigate the ability of a reactive model of silica to build crystalline zeolite frameworks with an enhanced sampling approach based on replica exchange Monte Carlo (REMC) simulations. In our implementation of REMC, the silica hydrolysis/condensation equilibrium constant controlling network formation is chosen as the index parameter characterising each replica. We show that improving the performance of the REMC method by increasing its efficiency in producing zeolite crystals allows zeolites with larger unit cells to be constructed. In particular, we perform an efficiency case study on the sodalite structure, containing 12 tetrahedra per unit cell and then apply the resulting enhancements to construct a significantly larger zeolite. We have improved our simulations in two ways; first, we have analysed the roles of the Monte Carlo parameters on the efficiency of this REMC method. Second, we have implemented an adaptive protocol that resets the values of the hydrolysis/condensation equilibrium constants among the replicas, ‘on the fly’ of each simulation, to optimise replica exchange for the purpose of constructing zeolite crystals. Finally, we show that by applying these enhancements, the REMC method can produce the crystal structure of zeolite AWW, a nanoporous material with 24 tetrahedra per unit cell.

AB - We investigate the ability of a reactive model of silica to build crystalline zeolite frameworks with an enhanced sampling approach based on replica exchange Monte Carlo (REMC) simulations. In our implementation of REMC, the silica hydrolysis/condensation equilibrium constant controlling network formation is chosen as the index parameter characterising each replica. We show that improving the performance of the REMC method by increasing its efficiency in producing zeolite crystals allows zeolites with larger unit cells to be constructed. In particular, we perform an efficiency case study on the sodalite structure, containing 12 tetrahedra per unit cell and then apply the resulting enhancements to construct a significantly larger zeolite. We have improved our simulations in two ways; first, we have analysed the roles of the Monte Carlo parameters on the efficiency of this REMC method. Second, we have implemented an adaptive protocol that resets the values of the hydrolysis/condensation equilibrium constants among the replicas, ‘on the fly’ of each simulation, to optimise replica exchange for the purpose of constructing zeolite crystals. Finally, we show that by applying these enhancements, the REMC method can produce the crystal structure of zeolite AWW, a nanoporous material with 24 tetrahedra per unit cell.

KW - Replica exchange Monte Carlo

KW - Self Assembly

KW - Silica Polymerisation

KW - Zeolites

UR - http://www.scopus.com/inward/record.url?scp=85034638409&partnerID=8YFLogxK

UR - http://www.scopus.com/inward/citedby.url?scp=85034638409&partnerID=8YFLogxK

U2 - 10.1080/08927022.2017.1399375

DO - 10.1080/08927022.2017.1399375

M3 - Article

VL - 44

SP - 453

EP - 462

JO - Molecular Simulation

JF - Molecular Simulation

SN - 0892-7022

IS - 6

ER -