Relaxation engineering modulates oxygen evolution reaction activity in metallic glass catalysts

doi:10.1016/j.jmst.2025.11.050

Abstract

Abstract: Metallic glasses (MGs), with their isotropic disordered structure, broad composition tunability, and excellent electrocatalytic stability, have emerged as promising candidates for developing high-performance oxygen evolution reaction (OER) catalysts. However, the relationship between electrocatalytic performance and the inherent non-equilibrium and non-ergodic properties of MGs remains elusive. In this study, dynamic stress relaxation is employed to strategically modulate the OER activity of MGs without altering their composition, establishing the underlying linkages between catalytic performance and the energy/kinetic state of the amorphous system. The composition with a glass-glass transition (Pd₃₅Ni₄₀Cu₅P₂₀) shows decreased activity after relaxation, whereas the composition without such a transition (Pd₃₅Ni₃₀Cu₁₅P₂₀) exhibits increased activity, demonstrating that the relaxation engineering is influenced by the intrinsic structure of MGs. High-energy diffraction analysis further elucidates that these distinct relaxation-performance evolution pathways can be attributed to a unified structural picture: the reduced coordination number of short-range order (SRO) clusters combined with modified inter-cluster packing connectivity collectively increases electronic density and optimizes surface reconstruction, thereby boosting OER catalytic performance. This work establishes a quantitative correlation between the structural state of MGs and their OER catalytic performance, providing a universal structural design principle for developing high-performance and high-stability amorphous OER electrocatalysts via relaxation engineering.

Key words: Metallic glass, Relaxation, Amorphous catalysts, Electronic and atomic structure, Oxygen evolution reaction

Yiqing Wang, Xuan Ge, Saichao Cao, Yurong Gao, Huanyi Zhou, XinXin Xiao, Xiujun Han, Fan Yang, Jianguo Li, Qiaodan Hu. Relaxation engineering modulates oxygen evolution reaction activity in metallic glass catalysts[J]. J. Mater. Sci. Technol., 2026, 265: 23-31.

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