Synergistic sites over the ZnxZrO catalyst for targeted cleavage of the C–H bonds of ethane in tandem with CO2 activation
ethylene, as one of the most important light olefins, serves as a fundamental feedstock for producing various high-value-added chemical products. Industrial ethylene production primarily relies on steam cracking of ethane and naphtha feedstock, which suffers from several drawbacks including excessive energy consumption, significant carbon emissions, and severe coke deposition.
The tandem reaction achieved by the synergistic effect of Zn-O-Zr sites and oxygen vacancies, the ethane C–H bond was selectively clipped over the Zn-O-Zr sites and the CO2 C=O bonds was activated over the oxygen vacancies.
Chinese Journal of Catalysis
The CO₂-assisted oxidative dehydrogenation of ethane (CO₂-ODHE) represents an eco-friendly process that enables resource utilization of ethane with the greenhouse gas CO₂. This technology demonstrates significant potential for advancing carbon neutrality initiatives and establishing sustainable chemical production systems. The current catalyst systems exhibit inherent limitations originating from the activity-selectivity trade-off and insufficient stability. The design of catalysts capable of simultaneously achieving selective C–H bond scission of ethane and efficient CO₂ activation represents a key challenge in CO₂-ODHE.
The ZnxZrO bifunctional catalyst developed in this study exhibits synergistic effects in the simultaneous activation of C–H and C=O bonds. Comprehensive characterization techniques were employed to probe the surface chemical states of ZnxZrO catalysts during CO₂-ODHE, identifying distinct functions of active sites. The Zn-O-Zr sites selectively cleave C–H bonds of ethane, while oxygen vacancies effectively activate CO₂ C=O bonds, enabling synergistic conversion of ethane and CO₂. In situ FTIR further elucidated the tandem reaction mechanism involving ethane dehydrogenation and reverse water-gas shift (RWGS).
This study provides fundamental insights into developing cost-effective, highly active, and stable catalysts for CO₂-ODHE, while establishing a novel catalyst design strategy for targeting alkane C–H bond scission in olefin production and CO₂ utilization.
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