Abstract

Methanol steam reforming faces a significant challenge due to CO formation, which can lead to poisoning of fuel cell electrodes. This study introduces a series of Pd/ZnO catalysts prepared by ethylene glycol reduction, exhibiting remarkable selectivity in methanol steam reforming (MSR). The majority of palladium species exist in the form of PdZn alloy, attributed to the dual reduction process. This process, along with the generation of zinc vacancies and oxygen vacancies, enhances the interaction between the metal-carrier, promoting the formation of PdZn alloy, significantly improving CO2 selectivity and catalytic activity. Even at a high temperature of 400 °C, the active phase remains stable. After 5 hours of MSR, the 3% Pd/ZnO-300 H2 catalyst achieves a hydrogen production rate of 1628.0 mmol·gcat−1·h−1, with methanol conversion stabilized at 94%, CO2 selectivity reaching 97.7%, and CO content as low as 0.5%. These results outperform recent studies on hydrogen production. Furthermore, DFT calculations elucidate the complete reaction pathway (111) on PdZn. This study provides initial insights into the influence of metal-carrier interaction on the formation of PdZn alloy, suggesting a new direction for palladium-based catalysts in methanol steam reforming.

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