Spin Polarization in Chiral Nanostructured Pd Films for Enhanced Oxygen Evolution Performance

Abstract

The slow kinetics and high overpotentials of the oxygen evolution reaction (OER) remains a major challenge for electrocatalytic energy conversion. Spin manipulation has emerged as a promising strategy for enhancing OER performance by modulating the adsorption of intermediates, thereby reducing the reaction energy barrier and accelerating OER kinetics. Herein, we demonstrate that chiral nanostructured Pd films (CNPFs) can enhance OER performance. CNPFs were electrodeposited on a nickel foam substrate using methionine as a symmetry-breaking agent. The optimal CNPFs catalyst achieves a current density of 50 mA∙cm⁻² at 1.57 V versus RHE, representing a 180 mV reduction in overpotential compared to achiral Pd films. By varying the electrodeposition time, a series of CNPFs with tunable spin polarization were synthesized. The enhanced OER performance in CNPFs exhibits a positive correlation with spin polarization, primarily due to the spin-polarized electron transfer promoting the formation of triplet oxygen. This work elucidates the fundamental relationship between spin polarization and OER performance, highlighting the critical role of chiral structure in the design of efficient spin-polarized electrocatalysts.

Keywords

chiral nanostructured Pd films / chirality-induced spin selectivity / oxygen evolution reaction / spin polarization / triplet oxygen

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