Condensation and growth of amorphous aluminosilicate nanoparticles via an aggregation process
文献信息
Romain Dupuis, Seung Ho Hahn, Adri C. T. van Duin, Roland J.-M. Pellenq, Arnaud Poulesquen
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.
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Physical Chemistry Chemical Physics

Physical Chemistry Chemical Physics (PCCP) is an international journal co-owned by 19 physical chemistry and physics societies from around the world. This journal publishes original, cutting-edge research in physical chemistry, chemical physics and biophysical chemistry. To be suitable for publication in PCCP, articles must include significant innovation and/or insight into physical chemistry; this is the most important criterion that reviewers and Editors will judge against when evaluating submissions. The journal has a broad scope and welcomes contributions spanning experiment, theory, computation and data science. Topical coverage includes spectroscopy, dynamics, kinetics, statistical mechanics, thermodynamics, electrochemistry, catalysis, surface science, quantum mechanics, quantum computing and machine learning. Interdisciplinary research areas such as polymers and soft matter, materials, nanoscience, energy, surfaces/interfaces, and biophysical chemistry are welcomed if they demonstrate significant innovation and/or insight into physical chemistry. Joined experimental/theoretical studies are particularly appreciated when complementary and based on up-to-date approaches.




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