Synergy between Heterobimetallic Active Sites in Hybrid Bilayer Membranes Enhances the Electrocatalytic Activity and Product Selectivity of O2 Reduction

29 May 2023, Version 1
This content is a preprint and has not undergone peer review at the time of posting.

Abstract

The development of proton exchange membrane fuel cells is hindered by the sluggish O2 reduction reaction (ORR) kinetics. At present, precious metal catalysts are unable to enhance the ORR kinetics efficiently. To address this challenge, hybrid bilayer membranes (HBMs) with non-precious catalytic sites have been developed to independently control proton and electron transfer kinetics in ORR. Inspired by the structural properties of oxidases, a biomimetic CuFe active center was examined as an ORR electrocatalyst. This bimetallic HBM displayed an ORR activity that is 1.4 times higher than the monometallic systems and the highest Faradaic efficiency for H2O (~94%) among Cu-, Fe-, Ni-, and Co-based HBMs. Further investigation into H2O2 reduction revealed a parallel 2e–+2e– mechanism, highlighting the synergistic effect of the CuFe site in catalyzing ORR. These findings are envisioned to spark future rational design and optimization of catalysts for more efficient electrochemical processes.

Keywords

Oxygen Reduction Reaction
Hybrid Bilayer Membrane
Heterobimetallic Active Site
Interfacial Electrocatalysis
Self-assembled Monolayer
Proton-coupled Electron Transfer
Mechanistic Control
Parallel Redox Pathways
Biomimetic Platform

Supplementary materials

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Supplementary Materials for "Synergy between Heterobimetallic Active Sites in Hybrid Bilayer Membranes Enhances the Electrocatalytic Activity and Product Selectivity of O2 Reduction"
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