We will focus on the applications of computational chemistry to further optimize exploring the chemical space of Frustrated Lewis Pairs in methane activation, which has not been experimentally reported. DFT calculations are utilized to elucidate the reaction mechanism of methane activation by triel trihalide and pnictogen pentahalide-ammonia Lewis pairs. Two reaction mechanisms were modelled for methane activation: proton abstraction and hydride abstraction. In all cases, deprotonation was thermodynamically and kinetically favored versus hydride abstraction. The use of heavier pnictogens and bigger triels were calculated to be more favorable for methane activation. To discern factors affecting the activation energies, different descriptors were correlated – ground state thermodynamics, orbital energies, transition state strain energies, <i>etc</i>. - but no consistent patterns were identified. Thus, machine learning methods were used to correlate ground state parameters to barrier heights(R<sup>2</sup> = 0.90). Using computational programs, a molecule builder was designed to model thousands of reactions, paired with machine learning algorithms, it has permitted broad exploration of chemical space. Close to 7,000 molecules have been calculated thus far, with hundreds of potential candidates for methane activation.

Automated exploration of frustrated lewis pair chemical space for methane activation.

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ACS Fall 2022

The official archive and repository for all ACS Meetings & Expositions abstracts and select posters or presentations.