Validation of the CoGEF Method as a Predictive Tool for Polymer Mechanochemistry

• DOI: 10.1021/jacs.0c06868
• Publication Date: 2020-09-09T16:19:18Z
• Authors: Isabel M. Klein; Corey C. Husic; Dávid P. Kovács; Nicolas J. Choquette; Maxwell J. Robb
• Keywords: Mechanochemistry

The development of force-responsive molecules called mechanophores is a central component the field polymer mechanochemistry. Mechanophores enable design and fabrication polymers for variety applications ranging from sensing to molecular release self-healing materials. Nevertheless, an insufficient understanding structure-activity relationships limits experimental development, thus computation necessary guide structural mechanophores. constrained geometries simulate external force (CoGEF) method highly accessible straightforward computational technique that simulates effect mechanical on molecule enables prediction mechanochemical reactivity. Here, we use CoGEF systematically evaluate every covalent mechanophore reported date compare predicted reactivity results. Molecules are mechanochemically inactive also studied as negative controls. In general, reactions with at common B3LYP/6-31G* level density functional theory in excellent agreement determined experimentally. Moreover, bond rupture forces obtained calculations compared experimentally measured demonstrated be reliable indicators activity. This investigation validates powerful tool predicting reactivity, enabling its widespread adoption support developing Secondarily, this study provides contemporary catalog over 100 developed date.