Abstract
Direct catalytic hydrogenation of CO2 is a highly promising route for olefin synthesis. However, achieving high olefin selectivity is predicated on the development of a selective catalyst with acceptable yield and stability. Herein, we report a Sr and Na co-decorated Fe catalyst that showed stable performance in the synthesis of high-valued olefins (ethene, propene and linear α-olefins) with space-time yield up to 290 mg gcat−1 h−1 without significant deactivation for over 500 h on-stream. The excellent catalytic performance is attributed to the cooperative effect of Sr and Na on the distinct sites (Fe5C2, Fe3C, Fe3O4) in catalyst. In particular, SrCO3 promoted the dispersion of binding Fe sites that facilitated the formation and stabilization of FeCx phase. Simultaneously, Sr contributed to the electron interaction between Na and Fe species. The dual effect of Sr as both structural and electronic promoters coordinatively improved C–O dissociative adsorption and subsequent C–C coupling, thus facilitated CO2 hydrogenation.
| Original language | English |
|---|---|
| Article number | 121640 |
| Journal | Applied Catalysis B: Environmental |
| Volume | 316 |
| DOIs | |
| State | Published - Nov 5 2022 |
Funding
This work was supported by the National Natural Science Foundation of China (21802138, 21773234 and 22078315), the “Transformational Technologies for Clean Energy and Demonstration”, Strategic Priority Research Program of the Chinese Academy of Sciences (XDA 21090203), the Youth Innovation Promotion Association of Chinese Academy of Sciences (2020189 and 2018214), the Youth Science and Technology Star Project Support Program of Dalian City (2021RQ123), and Dalian Institute of Chemical Physics (DICP I202138 and I202012). We also thank the assistance of Center for Advanced Mössbauer Spectroscopy, DICP, CAS. Joshua Iseoluwa Orege would like to express his gratitude to the University of Chinese Academy of Sciences (UCAS) for the UCAS Scholarship for International Students, as well as Engineer Shoufu Hou and other members of the Small Carbon Molecules and Hydrogen Utilization Group, DICP, CAS.. This work was supported by the National Natural Science Foundation of China ( 21802138 , 21773234 and 22078315 ), the “Transformational Technologies for Clean Energy and Demonstration”, Strategic Priority Research Program of the Chinese Academy of Sciences (XDA 21090203 ), the Youth Innovation Promotion Association of Chinese Academy of Sciences (2020189 and 2018214), the Youth Science and Technology Star Project Support Program of Dalian City ( 2021RQ123 ), and Dalian Institute of Chemical Physics (DICP I202138 and I202012 ). We also thank the assistance of Center for Advanced Mössbauer Spectroscopy, DICP, CAS. Joshua Iseoluwa Orege would like to express his gratitude to the University of Chinese Academy of Sciences (UCAS) for the UCAS Scholarship for International Students, as well as Engineer Shoufu Hou and other members of the Small Carbon Molecules and Hydrogen Utilization Group, DICP, CAS..
Keywords
- CO hydrogenation
- Catalytic stability
- Fe-based catalyst
- High-valued olefins
- Strontium promoter