Journal of Energy Chemistry ›› 2023, Vol. 80 ›› Issue (5): 614-624.DOI: 10.1016/j.jechem.2023.02.007

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Boosting CO2 hydrogenation to high-value olefins with highly stable performance over Ba and Na co-modified Fe catalyst

Joshua Iseoluwa Oregea,b, Na Liua,b, Cederick Cyril Amooa,b, Jian Weia,*, Qingjie Gea,*, Jian Suna   

  1. aDalian National Laboratory for Clean Energy, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, China;
    bUniversity of Chinese Academy of Sciences, Beijing 100049, China
  • Received:2022-12-06 Revised:2023-01-19 Accepted:2023-02-03 Online:2023-05-15 Published:2023-05-29
  • Contact: * E-mail addresses: weijian@dicp.ac.cn (J. Wei), geqj@dicp.ac.cn (Q. Ge).

Abstract: CO2 hydrogenation has been considered to be a highly promising route for the production of high-value olefins (HVOs) while also mitigating CO2 emissions. However, it is challenging to achieve high selectivity and maintain stable performance for HVOs (ethylene, propylene, and linear a-olefins) over a prolonged reaction time due to the difficulty in precise control of carbon coupling and rapid catalyst deactivation. Herein, we present a selective Ba and Na co-modified Fe catalyst enriched with Fe5C2 and Fe3C active sites that can boost HVO synthesis with up to 66.1% selectivity at an average CO2 conversion of 38% for over 500 h. Compared to traditional NaFe catalyst, the combined effect of Ba and Na additives in the NaBaFe-0.5 catalyst suppressed excess oxidation of FeCx sites by H2O. The absence of Fe3O4 phase in the spent NaBaFe-0.5 catalyst reflects the stabilization effect of the co-modifiers on the FeCx sites. This study pro-vides a strategy to design Fe-based catalysts that can be scaled up for the stable synthesis of HVOs from CO2 hydrogenation.

Key words: CO2 hydrogenation, High-value olefins, Barium additive, Iron carbide, Catalytic stability