4.8 Article

Uncovering the electronic effects of zinc on the structure of Fe5C2-ZnO catalysts for CO2 hydrogenation to linear α-olefins

期刊

APPLIED CATALYSIS B-ENVIRONMENTAL
卷 295, 期 -, 页码 -

出版社

ELSEVIER
DOI: 10.1016/j.apcatb.2021.120287

关键词

CO2 hydrogenation; Linear alpha-olefins; Fe5C2-ZnO catalyst; Chemical state; Electronic effect

资金

  1. National Natural Science Foundation of China [21878080, 21808058, 21576084]
  2. Shanghai Sailing Program [18YF1406100]
  3. Fundamental Research Funds for the Central Universities [222201718002, 222201814006]
  4. InnovationScientists and Technicians Troop Construction Projects of Henan Province

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The addition of ZnO significantly improved the performance of Fe-based catalysts in the reaction of CO2 hydrogenation to linear α-olefins (LAOs), leading to enhanced selectivity and improved activity. In situ X-ray photon spectroscopy (XPS) revealed the chemical state of Zn and its electronic effects, shedding light on the structure evolution during the induction period of the reaction.
The performance of Fe-based catalysts has found to be remarkably improved by the addition of ZnO in the reaction of CO2 hydrogenation to linear a-olefins (LAO). The space time yield (STY) of C4-20 alpha-olefins for bimetallic Fe2Zn1 is 2.4 times of the Fe alone; while a C4-20 olefins selectivity of 60.7 % with an 89.3 % LAOs/olefins ratio in C4-20 alkenes at a CO2 conversion of 43.5 % was achieved as well. Using in situ X-ray photon spectroscopy (XPS), we have proved that the chemical state of Zn varied between 0 and +2 (Zn delta+), accompanying by electronic donating from ZnOx to Fe. Focusing on electronic effects, we revealed the structure evolution during the induction period. The introduction of ZnO changed the ratios of FeCx/FeOx during the reaction. This study uncovered the chemical valence of Zn for CO2 to LAOs and its effects on the structure of active sites and the performance of Fe5C2-ZnO catalysts.

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