Dinitrogen Activation within Frustrated Lewis Pairs Is Promoted by Adding External Electric Fields

• Published in: The journal of physical chemistry. A, Molecules, spectroscopy, kinetics, environment, & general theory Molecules, spectroscopy, kinetics, environment, & general theory, 2024-05, Vol.128 (23), p.4595-4604
• Main Authors: Jain, Shailja, Danovich, David, Shaik, Sason
• Format: Article
• Language: English
• Subjects: A: Structure, Spectroscopy, and Reactivity of Molecules and Clusters
• ISSN: 1089-5639; 1520-5215; 1520-5215
• DOI: 10.1021/acs.jpca.4c00437

This study uses computational means to explore the feasibility of N2 cleavage by frustrated Lewis pair (FLPs) species. The employed FLP systems are phosphane/borane (1) and carbene/borane (2). Previous studies show that 1 and 2 react with H2 and CO2 but do not activate N2. The present study demonstrates that N2 is indeed inert, and its activation requires augmentation of the FLPs by an external tool. As we demonstrate here, FLP-mediated N2 activation can be achieved by an external electric field oriented along the reaction axis of the FLP. Additionally, the study demonstrates that FLP –N2 activation generates useful nitrogen compound, e.g., hydrazine (H2N–NH2). In summary, we conclude that FLP effectively activates N2 in tandem with oriented external electric fields (OEEFs), which play a crucial role. This FLP/OEEF combination may serve as a general activator of inert molecules.