Preparation of T8 and double-decker silsesquioxane-based Janus-type molecules: molecular modeling and DFT insights

TL;DR

This paper describes a new method to create Janus-type molecules using silsesquioxanes, combining experiments and computational modeling to understand their structure and aggregation behavior.

Contribution

A novel synthesis method for Janus-type silsesquioxane molecules with high yields and insights into their aggregation behavior via DFT.

Findings

High yields and selectivities were achieved in synthesizing Janus-type silsesquioxane molecules.

Molecular modeling and DFT revealed the propensity for molecular aggregation and the functional groups involved.

The study provides insights for tailoring silsesquioxane properties for applications like nanocomposites and drug delivery.

Abstract

We present a methodology for the synthesis of inorganic-organic Janus-type molecules based on mono-T8 and difunctionalized double-decker silsesquioxanes (DDSQs) via hydrosilylation reactions, achieving exceptionally high yields and selectivities. The synthesized compounds were extensively characterized using various spectroscopic techniques, and their sizes and spatial arrangements were predicted through molecular modelling and density functional theory (DFT) calculations. Quantum chemical calculations were employed to examine the interactions among four molecules of the synthesized compounds. These computational results allowed us to determine the propensity for molecular aggregation, identify the functional groups involved in these interactions, and understand the changes in interatomic distances during aggregation. Understanding the aggregation behaviour of silsesquioxane molecules is crucial for tailoring their properties for specific applications, such as nanocomposites, surface coatings, drug delivery systems, and catalysts. Through a combination of experimental and computational approaches, this study provides valuable insights into the design and optimization of silsesquioxane-based Janus-type molecules for enhanced performance across various fields.

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