The reorganization energy is one of the three parameters necessary for calculation of electron transfer rate constants. Here we report the use of Marcus-Gerischer theory to experimentally determine the reorganization energy for interfacial electron transfer reactions occurring form transparent conductive oxides (TCOs) to molecular acceptors that were initiated with light. A significant advantage of TCOs is that their metallic character allows potentiostatic control of the Fermi level (EF) and thus the driving force for electron transfer, −ΔG° = nF(E°′ − EF). Experimentally determined kinetic rate constants measured as a function of −ΔG° have provided the reorganization energy for proton-coupled electron transfer to a water oxidation catalyst and for acceptors positioned at specific locations within the electric double layer. The impact of these results on photocatalysis will be discussed.

Reorganization energies for electron and proton-coupled electron transfer reactions at conductive interfaces

ACS Spring Meeting 2021

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