Switchable molecular electrocatalysis.

ABSTRACT: We demonstrate a switchable electrocatalysis mechanism modulated by hydrogen bonding interactions in ligand geometries. By manipulating these geometries, specific electrochemical processes at a single catalytic site can be selectively and precisely activated or deactivated. The α geometry enhances dioxygen electroreduction (ORR) while inhibiting protium redox processes, with the opposite effect seen in the β geometry. Intramolecular hydrogen bonding in the α geometry boosts electron density at the catalytic center, facilitating a shift of ORR to a 4-electron pathway. Conversely, the β geometry promotes a 2-electron ORR and facilitates electrocatalytic hydrogen evolution through an extensive proton charge assembly; offering a paradigm shift to conventional electrocatalytic principles. The e

SUBMITTER: Dutt S 

PROVIDER: S-EPMC11339944 | biostudies-literature | 2024 Aug

REPOSITORIES: biostudies-literature