Linear Scaling Relationships to Predict pK_a's and Reduction Potentials for Bioinspired Hydrogenase Catalysis.

ABSTRACT: Biomimetic catalysts inspired by the active site of the [FeFe] hydrogenase enzyme can convert protons into molecular hydrogen. Minimizing the overpotential of the electrocatalytic process remains a major challenge for practical application of the catalyst. The catalytic cycle of the hydrogen production follows an ECEC mechanism (E represents an electron transfer step, and C refers to a chemical step), in which the electron and proton transfer steps can be either sequential or coupled (PCET). In this study, we have calculated the pK_a's and the reduction potentials for a series of commonly used ligands (80 different complexes) using density functional theory. We establish that the required acid strength for protonation at the Fe-Fe site correlates with the standard reductio

SUBMITTER: Puthenkalathil RC 

PROVIDER: S-EPMC8753599 | biostudies-literature | 2022 Jan

REPOSITORIES: biostudies-literature