Self-reconstructing amorphous high-entropy oxides for CO2-free methanol electroreforming and hydrogen generation

X Liu and XT Zhao and ZW Lu and K Chen and JY Gao and HB Wang and JX Chen and ZH Wen, APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY, 379, 125721 (2025).

DOI: 10.1016/j.apcatb.2025.125721

Amorphous electrocatalysts, unconstrained by crystalline order, offer a versatile landscape of active sites that promote enhanced reactivity and structural adaptability. When fused with the compositional complexity of highentropy materials, this disordered architecture yields enhanced electronic interactions and catalytic adaptability. In this work, we design a self-supporting amorphous high-entropy oxide (a-HEO) electrode by in-situ growth of FeCoNiMnMo-based nanosheets on nickel foam (a-FeCoNiMnMoO/NF). Electrochemical activation triggers a self- reconstruction process, yielding oxyhydroxide species embedded with oxygen vacancies that collectively enhance electron conductivity and catalytic performance for the alkaline methanol oxidation reaction (MOR). Machine learning potential-based simulations demonstrate that the amorphous oxyhydroxide layer offers a diverse array of catalytic sites, fine-tunes the electronic structure, and optimizes intermediates adsorption, thus enhancing the reaction dynamics of methanol oxidation. When employed in a hybrid acid/alkali flow electrolyzer, the system operates at just 0.54 V to reach 10 mA cm-2, enabling over 300 h of continuous, CO2-free production of hydrogen and formate, demonstrating a durable and energy-saving strategy for sustainable fuel and chemical generation. This study highlights the compelling synergy between structural disorder and elemental complexity, charting a promising course toward low-energy, carbon-neutral methanol reforming and sustainable hydrogen production.

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