Condensation and growth of amorphous aluminosilicate nanoparticles via an aggregation process

Romain Dupuis, Seung Ho Hahn, Adri C.T. van Duin, Roland J.M. Pellenq, Arnaud Poulesquen

Research output: Contribution to journalArticlepeer-review

2 Scopus citations

Abstract

The precipitation of zeolite nanoparticles involves the initial formation of metastable precursors, such as amorphous entities, that crystallize through non-classical pathways. Here, using reactive force field-based simulations, we reveal how aluminosilicate oligomers grow concomitantly to the decondensation of silicate entities during the initial step of the reaction. Aluminate clusters first form in the solution, thus violating the Loewenstein rule in the first instant of the reaction, which is then followed by their connection with silicate oligomers at the terminal silanol groups before reorganization to finally diffuse within the silicate oligomers to form stable amorphous aluminosilicate nanoparticles that do obey the Loewenstein rule. Our results clearly indicate that aluminate does not serve as the nucleation center for the growth of aluminosilicates in a nucleation-like process but rather proceeds via an aggregation process. The coexistence of aluminosilicate oligomers and small silicate entities induces a phase separation that promotes the precipitation of zeolites with aging.

Original languageEnglish (US)
Pages (from-to)9229-9235
Number of pages7
JournalPhysical Chemistry Chemical Physics
Volume24
Issue number16
DOIs
StatePublished - Mar 19 2022

All Science Journal Classification (ASJC) codes

  • General Physics and Astronomy
  • Physical and Theoretical Chemistry

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