Synergistic Spin-Mediated Catalysis for the Oxygen Evolution Reaction

Aravind Vadakkayil,F. Fahim,Wiley A. Dunlap-Shohl,Michael Vullo,B. Bloom,D. Waldeck

Published 2025 in Journal of the American Chemical Society

ABSTRACT

The oxygen evolution reaction (OER), the anodic half-reaction in water electrolysis, remains a critical bottleneck to the widespread adoption of a hydrogen-based economy. While spin polarization of reaction intermediates has been shown to enhance the performance of the OER, existing studies often overlook the distinctions between different ways of spin-polarizing intermediates and their correlation with catalytic efficiency. In this study, we conduct a comprehensive analysis of spin-mediated catalysis, revealing that the efficiency of the OER is highly sensitive to the nature and magnitude of the spin polarization applied. More significantly, we explore the interplay among different methods for generating spin polarization at catalysts and demonstrate how their combination can have a constructive or destructive impact on catalytic performance. To provide deeper insight into the mechanisms driving spin-controlled catalysis, we interpreted these findings using a statistical model.

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