Mechanistic Insights Into CO 2 Activation via Phosphorus–Boron Frustrated Lewis Pairs: A Density Functional Theory Study

This study investigates the reactivity of a novel intermolecular phosphine/borane (P/B) frustrated Lewis pair in the activation of CO 2 via a push‐pull mechanism. Detailed computational analyses, particularly intrinsic reaction coordinate calculations, reveal a single‐step and concerted mechanism for CO 2 activation. The reaction is characterized as exergonic, with notable efficiency in bromobenzene solvent. Furthermore, natural bond orbital analysis provides critical insights into the electron transfer processes, elucidating the roles of key donor–acceptor interactions in facilitating the reaction. These findings enhance the understanding of frustrated Lewis pair‐mediated CO 2 activation and highlight the potential of this system for catalytic applications.