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Competing Magnetic Anisotropy and Domain-Wall Density for Optimizing Magnetization-Induced Water-Oxidation Enhancement

Anke Yu1,*, Durgesh Kumar2,*, Zizhao Gong3, Leonhard Tannesia1,4, Hasibur Rahaman2, Pengfei Song1, Tianze Wu1, Ramu Maddu2, Pinkesh Kumar Mishra2 et al.

Xiao Renshaw Wang2,5, S. N. Piramanayagam2,†, and Zhichuan J. Xu1,6,‡

  • *These authors contributed equally to this work.
  • †Contact author: prem@ntu.edu.sg
  • ‡Contact author: xuzc@ntu.edu.sg

Phys. Rev. Lett. 136, 108001 – Published 11 March, 2026

DOI: https://doi.org/10.1103/bdr5-bg1j

Abstract

The application of a magnetic field has emerged as an effective method for studying the spin-related effects in the oxygen evolution reaction (OER). However, the presence of spin-unrelated effects under a magnetic field also contributes to the observed OER increment, complicating the identification of spin-related enhancement. This is primarily associated with the intrinsic limitation of the conventional magnetic catalysts that require the continuous application of an external magnetic field to maintain the magnetization. Here, we have developed magnetron-sputtered Co/PtCo multilayer catalysts with perpendicular magnetic anisotropy, enabling a stable magnetization state without continuous magnetic fields. The magnetic anisotropy of the multilayers is controlled through the number of repetitions of Co/PtCo bilayers. As the bilayer number increases from 2 to 25, the domain size at the demagnetized state gradually reduces to the nanometer scale due to the enhanced magnetostatic energy. Upon premagnetization with out-of-plane magnetic fields, the pure spin-enhanced OER is numerically correlated to the change in domain wall ratios, where the global non-spin-related enhancement is effectively excluded. Such spin-enhanced OER is found to be favored by magnetic anisotropy due to the higher magnetic stability to maintain the magnetization state. This Letter provides a new strategy for achieving stable spin-related OER enhancement by magnetic anisotropy, advancing magnetic-field-free spin electrocatalysts to optimize OER performance.

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