The design of electrocatalysts for the evolution of H2, the reduction of O2, N2, and CO2, as well as the splitting of water into protons, electrons, and O2 is essential for the development of the alternative energy sources. Typically, the catalytic cycle for the electrocatalysts is controlled by key proton-coupled electron transfer (PCET) processes including sequential or concerted electron transfer (ET) and proton transfer (PT) steps. Studying the thermodynamics and kinetics of PCET processes can give insights into which pathway is dominant, sequential (ET-PT/PT-ET) or concerted (EPT), in order to design more effective electrocatalysts. Herein, the focus is on complexes with the scorpionate ligand hydrotris(1,2,4-triazole-1-yl)borate (Ttz), [M(Ttz)(CO)3], which have been less studied as electrocatalysts. To the best of our knowledge, a systematic study of PCET reactions for mid – late 3d, 4d–transition metals complexes of Ttz has not been reported. Preliminary results indicate in the sequential process the preferred mechanism is ET-PT over PT-ET for most of the studied 3d and 4d metals.

Computational analysis of proton-coupled electron transfer in molecular electrocatalysts containing tris(triazolyl)borate ligand

2019 Spring National Meeting

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