Proton-coupled electron transfer (PCET) reactions are central to many catalytic processes. Here, we describe our efforts in developing a nanoscale electrochemical platform to modulate the proton and electron transfer rates independently for oxygen reduction reaction (ORR). ORR is the chemical reaction that critically limits the performance of fuel cells and related energy conversion technologies. Our versatile electrode features a hybrid bilayer membrane comprising of a self-assembled monolayer (SAM), an ORR electrocatalyst, a phospholipid layer, and a proton transfer agent [1]. Each of these four controls one aspect of ORR, and together they determine the overall catalytic performance. Utilizing this hybrid bilayer membrane (HBM) system, the proton transfer rate can be tuned by the proton transfer agent in the lipid layer. Typically, proton carriers are turned on to deliver transmembrane proton delivery upon acidification. Here, we demonstrate the development of a unique nitrile-based proton transfer agent with its proton delivery ability enhanced under alkaline conditions. Taking advantage of this newly enabled base-triggered proton delivery system, we achieve higher ORR activity in base without covalent modification of the ligand framework. These modular HBM will offer new opportunities to enhance the performance of catalysts involved in other renewnable energy schemes.
[1] Zeng, T.; Gautam, R.; Barile, C. J.; Li, Y.; Tse, E. C. M. “Nitrile-Facilitated Proton Transfer for Enhanced Oxygen Reduction by Hybrid Electrocatalysts” ACS Catal. 2020, 10, 13149-13155.

Facilitating PCET Kinetics in Alkaline Using Lipid-Modified Electrodes

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