Revealing Dinitrogen Activation via Mesoionic Carbenes: A Computational Design with Frustrated Lewis Pairs

Abstract Activating dinitrogen under metal‐free conditions remains a significant challenge in chemistry. In this study, we computationally designed a frustrated Lewis pair (FLP) system incorporating a bis(trimethylsilyl)boryl substituent on a mesoionic carbene (MIC) framework. Our models show both kinetic and thermodynamic favorability for dinitrogen activation. Aromaticity enhancement along the potential energy surface (PES) plays a critical role in driving the reaction. This work provides insights into utilizing main‐group elements for dinitrogen activation and offers potential applications in inert molecule activation and optical materials.