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Anchoring Cuδ+ at oxygen-vacancy-rich Y-Ov-Cr interfaces: A self-activated catalyst for ultra-stable and highly selective methanol reforming

Shufan Yu,Zhao Sun,Zhiqiang Sun

Methanol steam reforming is a promising approach for real-time hydrogen production, while its practical application is hindered by catalyst deactivation and undesired CO byproduct formation. In this study, we propose a self-activation approach to anchoring a series of x CuO/YCrO 4 catalysts by employing methanol and steam as reductants. The self-activated 0.8CuO/YCrO 4 catalyst achieves a high hydrogen production rate of 22.3 μmol H 2 ·g −1 cat ·s −1 and demonstrates exceptional stability over 3000 min at 220°C. TEM-EDS, XPS, EPR, and XAS collectively reveal the promotion of generating Cu δ + /Y-O v -Cr interfacial sites and oxygen vacancies via self-activation, and in situ Raman spectroscopy confirms the structural stability of the Y-O v -Cr framework. In situ DRIFTS analysis further confirms that Cu δ + /Y-O v -Cr interfacial sites effectively anchor and promote the hydrogenation of bidentate formate intermediates, mitigating active site blockage by byproduct species and enhancing catalytic efficiency. This work provides new insights into the self-activation mechanism of Cu-based catalysts and offers a promising strategy for developing highly active and durable catalysts.