abstract
We report a molecular modeling paradigm to describe silica polymerization reactions in aqueous solutions at conditions that are representative of realistic experimental processes like biosilicification or porous silica synthesis - i.e. at close to ambient temperatures and over a wide range of pH. The key point is to describe the Si-O-Si chemical bond formation and breakage processes through a continuous potential with a balance between attractive and repulsive interactions between suitably placed virtual sites and sticky particles. The simplicity of the model, its applicability in standard parallelized molecular dynamics codes, and its compatibility with the widely used MARTINI coarse-grained force-field allows for the study of systems containing millions of atoms over microsecond time scales. The model is calibrated to match experimental results for the temporal evolution of silica polymerization in aqueous solution close to the isoelectric point, and can describe silica polymerization and self-assembly processes during encapsulation of a surfactant micelle.
keywords
SI-O-SI; MONTE-CARLO; MESOPOROUS SILICA; FORCE-FIELD; AB-INITIO; SI-29 NMR; TEMPLATED SYNTHESIS; PART II; ZEOLITE; OLIGOMERIZATION
subject category
Chemistry; Materials Science
authors
Carvalho, AP; Santos, SM; Perez-Sanchez, G; Gouveia, JD; Gomes, JRB; Jorge, M
our authors
Germán Pérez-Sánchez
Junior Researcher
José R. B. Gomes
Principal Researcher
Marcos André Pinto de Carvalho
Research Fellowship
Sérgio Miguel Fernandes dos Santos
Assistant ResearcherProjects
CICECO - Aveiro Institute of Materials (UIDB/50011/2020)
CICECO - Aveiro Institute of Materials (UIDP/50011/2020)
Associated Laboratory CICECO-Aveiro Institute of Materials (LA/P/0006/2020)
Modeling the synthesis of SILica materials VIA multiscale computer simulations (SILVIA)
acknowledgements
This work was developed within the scope of projects CICECO-Aveiro Institute of Materials, refs. UIDB/50011/2020, UIDP/50011/2020 and LA/P/0006/2020, and SILVIA, refs. CENTRO-01-0145-FEDER-31002 and PTDC/QUI-QFI/31002/2017, financed by the Portuguese Fundacao para a Ciencia e a Tecnologia (FCT/MCTES), and co-financed by the European Regional Development Fund (FEDER) under the PT2020 Partnership Agreement, and project ref. QS-2019-2-0034 financed by the Red Espanola de Supercomputacion (RES). G.P-S. acknowledges the national funds (OE), through FCT-Fundacao para a Ciencia e a Tecnologia, I.P., in the scope of the framework contract foreseen in the numbers 4, 5 and 6 of the article 23, of the Decree-Law 57/2016, of August 29, changed by Law 57/2017, of July 19.