Invited Talk 21st International Conference on Biological Inorganic Chemistry 2025

Thermodynamic principles for regulating of H-atom transfer reactivity and selectivity (121966)

Martin Srnec 1 , Jan Kovář 1 , Zuzanna Wojdyla 1 , Jishnu Gopinath 1 , Radek Fučík 2 , Jakub Klinkovský 2
  1. J. Heyrovsky Institute of Physical Chemistry, Czech Academy of Sciences, Prague 8, CZECH REPUBLIC, Czech Republic
  2. Czech Technical University, Prague, Czech Republic

Recently, we have formulated a concept going beyond the traditional relationship between thermodynamics and kinetics, which includes the effect of off-diagonal thermodynamics on reactivity. Here, I will present the latest advances in the concept. Among others, this will cover the discussion of the difference between H-atom transfer and proton-coupled electron transfer in terms of the relationship between thermodynamics and reactivity, and in relation to the predictability of reaction selectivity from thermodynamics. Also, I will show how the off-diagonal thermodynamics controls the shift from proton-coupled to hydride-coupled electron transfer. If time allows, I will also touch on some additional aspects of the concept, such as the connection of the off-diagonal thermodynamics with some electronic-structure descriptors.