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Switching from Reforming to Selective Dehydrogenation for Ethane-CO2 Coconversion on CeO2-Based Catalysts via
Feigang Zhao1, Tiantian Xiao1,2, Yong Wang1
1Key Laboratory for Green Chemical Technology of Ministry of Education, Collaborative Innovation Center of Chemical Science and Engineering, School of Chemical Engineering and Technology, Tianjin University, Tianjin300072, P. R. China.
Journal of the American Chemical Society
|June 25, 2026
Summary
Engineered nanoporous ceria (np-CeO2) with high-index facets enhances ethane-CO2 coconversion selectivity to ethylene. This crystal facet engineering approach offers a novel strategy for efficient greenhouse gas valorization.
Area of Science:
- Materials Science
- Catalysis
- Chemical Engineering
Background:
- Cerium dioxide (CeO2)-supported metal catalysts are crucial for ethane-CO2 coconversion, primarily yielding syngas via dry reforming of ethane (DRE).
- Achieving selective dehydrogenation to ethylene, a valuable olefin, remains a significant challenge in this process.
Purpose of the Study:
- To develop a catalyst strategy for selective ethane dehydrogenation to ethylene using ethane-CO2 coconversion.
- To investigate the role of catalyst crystal facets in controlling reaction pathways and product selectivity.
Main Methods:
- Fabrication of nanoporous CeO2 (np-CeO2) with exposed high-index facets (HIFs) via crystal-facet engineering.
- Utilized in situ characterizations and theoretical calculations to analyze catalyst structure-activity relationships.
- Tested catalyst performance in ethane-CO2 coconversion, comparing HIFs with low-index facets (LIFs).
Main Results:
- The np-CeO2 with HIFs, featuring electron-deficient Co species (Coδ+), achieved 88% ethylene selectivity in ethane-CO2 coconversion.
- In contrast, Co on CeO2 with LIFs predominantly favored DRE, yielding only 2% ethylene.
- Electron-deficient Coδ+ species were found to moderate C-H bond activation, suppress DRE intermediates, and weaken ethylene π-orbital hybridization.
Conclusions:
- Exposing high-index facets on CeO2 is an effective strategy for designing catalysts with high ethylene selectivity in ethane-CO2 coconversion.
- The electron-deficient nature of metal species at the metal-CeO2 interface plays a critical role in promoting olefin selectivity.
- This research provides valuable insights for developing catalysts for selective alkane functionalization and CO2 utilization.
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