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>Lewis acid-base modulation for efficient CO2 oxidative propane dehydrogenation: A case study of a La-modified binuclear Fe_(oxo) site
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Lewis acid-base modulation for efficient CO2 oxidative propane dehydrogenation: A case study of a La-modified binuclear Fe_(oxo) site
CO2 oxidative propane dehydrogenation to propylene (CO2-ODH) is promising for propylene production and CO2 utilization. Developing an efficient bifunctional CO2-ODH site capable of activating C-H and C=O bonds with inhibited C-C scission capacity remains a challenge. This work describes a La-modified binuclear Fe_(oxo) (La-Fe_(oxo)) site stabilized on a silicalite-1 support; it achieves 32.7 propane conversion (1.72 times higher than the direct propane dehy-drogenation PDH counterpart) with 83.2 propylene selectivity. The promising CO2-ODH performance, attributed to the appropriate FeOx dispersion and La modification, balances the acid-base property, which helps stabilize key HCOO* intermediates toward enhanced CO2-assisted H removal efficiency. The inferior CO2-ODH performance of isolated Fe_(iso) and clustered Fe4O6 was rationalized by insufficient CO2 activation and huge dry reforming contribution, respectively. We propose H2 dissociative binding energy and O* binding energy as descriptors for the acid-base strength and catalytic CO2 dissociation capacity in that they predict the CO2-ODH and extent of propane dry reforming.
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