Density functional modelling of silicate and aluminosilicate dimerisation solution chemistry.

Area of Science:

• Inorganic chemistry
• Materials science
• Computational chemistry

Background:

• Sol-gel chemistry involves inorganic oxide polymerization and deprotonation, fundamental to zeolite synthesis, aluminosilicate glass formation, and geopolymerization.
• Understanding these reactions, particularly at high pH, is crucial for optimizing material synthesis and predicting material properties.

Purpose of the Study:

• To investigate the fundamental reactions of inorganic oxide polymerization and deprotonation during zeolite synthesis and geopolymerization at high pH.
• To compare density functional theory (DFT) derived energetics with existing literature values and DFT data at near-neutral pH.

Main Methods:

• Utilizing density functional theory (DFT) to model and calculate the energetics of deprotonation and dimerisation reactions.
• Comparing computational results with experimental data and previously published DFT findings for silicate reactions.

Main Results:

• The energetics of deprotonation and dimerisation reactions are highly dependent on the pH of the solution.
• DFT-derived energetics at high pH show good correlation with existing experimental values and trends.
• The study highlights the importance of accurately simulating the solution environment for theoretical chemistry.

Conclusions:

• Accurate simulation of the solution environment, especially pH, is critical for reliable theoretical predictions in non-ideal chemical systems.
• The findings provide valuable insights into the reaction mechanisms underlying zeolite synthesis and geopolymerization.
• This research validates the use of DFT for studying complex inorganic reactions in solution.