Journal
CHEMICAL SCIENCE
Volume 10, Issue 24, Pages 6083-6090Publisher
ROYAL SOC CHEMISTRY
DOI: 10.1039/c9sc01210a
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Funding
- National Key Research and Development Program of China [2017YFA0206500, 2018YFA0209103]
- National Natural Science Foundation of China [21832003, 21773111, 51571110, 21573107]
- Fundamental Research Funds for the Central Universities [020514380126]
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Fischer-Tropsch synthesis of lower olefins (FTO) is a classical yet modern topic of great significance in which the supported Fe-based nanoparticles are the most promising catalysts. The performance deterioration of catalysts is a big challenge due to the instability of the nanosized active phase of iron carbides. Herein, by in situ mass spectrometry, theoretical analysis, and atmospheric-and high-pressure experimental examinations, we revealed the Ostwald-ripening-like growth mechanism of the active phase of iron carbides in FTO, which involves the cyclic formation-decomposition of iron carbonyl intermediates to transport iron species from small particles to large ones. Accordingly, by suppressing the formation of iron carbonyl species with a high-N-content carbon support, the size and structure of the active phase were regulated and stabilized, and durable iron-based catalysts were conveniently obtained with the highest selectivity for lower olefins up to 54.1%. This study provides a practical strategy for exploring advanced FTO catalysts.
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