Journal
ACS CATALYSIS
Volume 10, Issue 20, Pages 12098-12108Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.0c03215
Keywords
CO2 hydrogenation; high-valued olefins; carbonaceous K-promoters; Fe5C2-K2CO3 interface; proximity
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Funding
- National Natural Science Foundation of China [91745107, 21773234]
- Liaoning Revitalization Talents Program [XLYC1907066]
- Dalian Outstanding Young Scientific and Technological Talents Program [2018RJ06]
- Transformational Technologies for Clean Energy and Demonstration, Strategic Priority Research Program of the Chinese Academy of Sciences [XDA 21090203]
- DICP [DICP I202012]
- Youth Innovation Promotion Association of Chinese Academy of Sciences [2018214]
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Directly converting carbon dioxide into high-valued olefins (ethylene, propylene, and linear alpha-olefins) with regenerative hydrogen could be a way of reducing CO2 emissions and replacing fossil fuels. However, precise control of C-O activation and subsequent C-C coupling toward those olefins remain a challenge, due to the unclear catalytic mechanism on active sites and surrounding promoters. Herein, we demonstrate that the carbonaceous series K-promoters from K2CO3, CH3COOK, KHCO3, and KOH can induce Fe/C catalysts to form a more active and distinct Fe5C2-K2CO3 interface in nanoscale via CO2 hydrogenation, which boosts the production of high-valued olefins by facilitating electron transfer from potassium to iron species. A high olefin selectivity of near 75% in hydrocarbons is realized at a conversion of more than 32%. The maximum yield of high-valued olefins reaches up to 20.1%, which is the record-breaking highest value among all Fe based CO2 hydrogenation in the literature. More interestingly, the appropriate proximity between carbonaceous K-promoters and Fe/C catalyst endow the catalytic system with an outstanding high-valued olefin yield and high catalytic stability. These findings enrich the chemistry of CO2 conversion and provide a strategy to design highly selective catalysts for high-valued chemicals.
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