Because of the steric hindrance[1], the Lewis acid/Lewis base may have no route to the classically quenched adduct and at the same time they often mimic the reaction properties of metal-containing complexes. [2],[3] In many cases, the non-covalent interactions play an essential role in how a possible acid/base encounter complexes could be formed. The mechanistic importance of the inherent structural flexibility of the binuclear Lewis acid/Lewis base systems motivated us to launch a systematic investigation of their inherent dynamics and the dynamics-driven pathways of H2 cleavage. Here we present recent results regarding the bond-activation and catalysis based on the ab initio molecular dynamics (AIMD) study of the pair of B(F5C6)3 and P(tBu)3. With a large volume of AIMD data as a support, we propose a model of the reaction-competent a collisional encounter complex in which Lewis acid and Lewis base are reminiscent of coupled parametric oscillators which evolve on the so-called funneled potential energy surface[4] - our recent AIMD calculations and the implications to the reactions of the bi-molecular acid/base systems with small molecules, i.e. H2,will be presented.[1]. Brown, H. C. J. Chem. Soc. 1956 , 1248.[2]. (a) Welch, G. C.; Juan, R. R. S.; Masuda, J. D.; Stephan, D. W. Science 2006 , 314, 1124; (b) Stephan D. W., Erker G.,Angew. Chem. Int. Ed., 2010 , 49, 46; (c)  Stephan, D. W., Org. Biomol. Chem. 2008 , 6, 1535; (d) Stephan D. W. Chem. Commun.,2010 , 8526; (e) Stephan D. W., Dalton Trans., 2009 , 3129.[3] Power P. P., Nature, 2010 , 463, 171.[4]. Pu, M.; Privalov, T. to be submitted.

Ab initio molecular dynamics of the catalytically-competent frustrated Lewis pair of B(F5C6)3 and P(tBu)3

245th National Meeting (2013)

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