ReaxFF reactive molecular dynamics simulation of the hydration of Cu-SSZ-13 zeolite and the formation of Cu dimers

George M. Psofogiannakis, John F. McCleerey, Eugenio Jaramillo, Adri Van Duin

Research output: Contribution to journalArticle

25 Citations (Scopus)

Abstract

A new Cu/Si/Al/O/H reactive ReaxFF force field was developed and used in molecular dynamics simulations of the hydration of Cu-exchanged SSZ-13 catalyst. It was observed that at temperatures close to room temperarture, all Cu cations, including those at the faces of the double 6-member rings (6MRs), become fully hydrated and detach from the framework. The hydrated Cu cations can diffuse through the Cu-SSZ-13 zeolite pore windows. At higher temperatures, the formation of cationic OH-bridged Cu dimers Cu2OH and Cu2(OH)2 within the cages was observed. The simulations show that the temperature at which these species are formed is lower for zeolites that stabilize [CuOH]+ ions, as would be expected for relatively high-Cu- and low-Al-content zeolites. The stable dimers bind preferentially to 8MRs beside the large cages in a configuration that blocks the openings of the pores. The consequences of the present results for selective catalytic reduction and NO oxidation catalysis in Cu-SSZ-13 are discussed.

Original languageEnglish (US)
Pages (from-to)6678-6686
Number of pages9
JournalJournal of Physical Chemistry C
Volume119
Issue number12
DOIs
StatePublished - Mar 26 2015

Fingerprint

Zeolites
zeolites
Hydration
Dimers
hydration
Molecular dynamics
dimers
molecular dynamics
porosity
cations
Cations
Computer simulation
Positive ions
field theory (physics)
catalysis
rooms
Selective catalytic reduction
simulation
catalysts
Temperature

All Science Journal Classification (ASJC) codes

  • Electronic, Optical and Magnetic Materials
  • Energy(all)
  • Physical and Theoretical Chemistry
  • Surfaces, Coatings and Films

Cite this

Psofogiannakis, George M. ; McCleerey, John F. ; Jaramillo, Eugenio ; Van Duin, Adri. / ReaxFF reactive molecular dynamics simulation of the hydration of Cu-SSZ-13 zeolite and the formation of Cu dimers. In: Journal of Physical Chemistry C. 2015 ; Vol. 119, No. 12. pp. 6678-6686.
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ReaxFF reactive molecular dynamics simulation of the hydration of Cu-SSZ-13 zeolite and the formation of Cu dimers. / Psofogiannakis, George M.; McCleerey, John F.; Jaramillo, Eugenio; Van Duin, Adri.

In: Journal of Physical Chemistry C, Vol. 119, No. 12, 26.03.2015, p. 6678-6686.

Research output: Contribution to journalArticle

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AU - Van Duin, Adri

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