Abstract
Cu-based catalysts with excellent activity at low temperatures are widely used for methanol steam reforming (MSR) but suffer from deactivation problems. The present work aims to elucidate the deactivation and regeneration mechanisms of the commercial Cu/ZnO/Al2O3 catalyst in low temperature MSR. By employing a series of (quasi) in situ characterization methods, it is found that the deactivation of the catalyst at a high weight hourly space velocity (WHSV) and a low reaction temperature is mainly due to the poisoning of Cu species associated with surface-oxygenated species with less Cu sintering, rather than carbon deposition, and strong metal-support interaction (SMSI). An in situ regeneration method was developed for the deactivated commercial Cu/ZnO/Al2O3 catalyst via the simultaneous supply of O2. It is shown that the addition of O2 (≥1 vol%) can reverse the deactivation caused by surface-oxygenated poisoning due to the weak interaction between formed surface copper oxide and surface-oxygenated species, facilitating their desorption, but not deactivation caused by sintering, thereby partially restoring the catalytic activity.
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Acknowledgements
This work was sponsored by the National Natural Science Foundation of China (22078089), the Program for Professor of Special Appointment (Eastern Scholar) at Shanghai Institutions of Higher Learning and Shanghai Sailing Program (19YF1410600).
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Supporting information The supporting information is available online at chem.scichina.com and link.springer.com/journal/11426. The supporting materials are published as submitted, without typesetting or editing. The responsibility for scientific accuracy and content remains entirely with the authors.
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Li, D., Wang, Z., Jin, S. et al. Deactivation and regeneration of the commercial Cu/ZnO/Al2O3 catalyst in low-temperature methanol steam reforming. Sci. China Chem. 66, 3645–3652 (2023). https://doi.org/10.1007/s11426-023-1789-3
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DOI: https://doi.org/10.1007/s11426-023-1789-3