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Steam-induced dimeric CoOx sites with strong Lewis acid–base pairs for boosting propane dehydrogenation
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DOI：10.1002/aic.70517.png)
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Abstract
En 中文
Propane dehydrogenation (PDH) is an on-purpose route for propylene production. High-temperature steam is inherent in catalyst regeneration via coke combustion, making it essential to elucidate the steam-induced active site evolution and its effect on PDH performance. Herein, combined spectroscopic characterizations and metadynamics simulations reveal that controlled steam pre-treatment transforms isolated framework Co2+ sites into dimeric CoOx sites, yielding a propylene formation rate about 8 times that of the untreated catalyst. The superior performance of dimeric CoOx sites is attributed to the enhanced Lewis acidity at the Co2+ centers and increased basicity at nearby oxygen atoms, facilitating propane C–H bond cleavage via a σ-bond metathesis mechanism. The efficient PDH performance of the dimeric CoOx structure was conceptually validated through an ion-exchange procedure from the cobaltosilicate zeolite. This work offers a new strategy for constructing highly active dimeric CoOx sites for PDH and provides mechanistic insights into the co-catalyzed PDH reaction.
Keywords:
C–H activation
dimeric sites
dynamic transformation
propane dehydrogenation
zeolite catalysts
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