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On the Variability of Ligand pKa during Homogeneously Catalyzed Aqueous Methanol Dehydrogenation

submitted on 01.09.2020, 09:24 and posted on 01.09.2020, 13:13 by Nitish Govindarajan, Hugo Beks, E.J. Meijer

Using DFT based molecular dynamics simulations

incorporating explicit water solvent, we elucidate the varying behaviour of the ligand pKa of a molecular catalyst for methanol dehydrogenation, using the Ru(PNP) catalytic system

as a case study. The pKa of the amido ligand moiety in this catalytic system is highly sensitive to the species adsorbed on the metal

center, resulting in a substantial variation of the ligand pKa along the catalytic cycle. Since the ligand pKa is an important characteristic that determines the exact role of the ligand during aqueous methanol dehydrogenation, this characteristic has important implications on metal ligand cooperative pathways.


Computational Sciences for Energy Research (Project 14CSER044) which is financially supported by the Netherlands Organization for Scientific Research (NWO)


Email Address of Submitting Author


Technical University of Denmark



ORCID For Submitting Author


Declaration of Conflict of Interest

No conflict of interest to declare