Journal
APPLIED CATALYSIS B-ENVIRONMENTAL
Volume 298, Issue -, Pages -Publisher
ELSEVIER
DOI: 10.1016/j.apcatb.2021.120556
Keywords
CO2 hydrogenation; Higher alcohols; Iron catalysts; Na-S synergy
Funding
- Transformational Technologies for Clean Energy and Demonstration, Strategic Priority Research Program of the Chinese Academy of Sciences [XDA 21090203]
- National Natural Science Foundation of China [22078315, 91745107, 21773234, 21802138]
- Youth Innovation Promotion Association of Chinese Academy of Sciences [2018214, 2020189]
- Liaoning Revitalization Talents Program [XLYC1907066]
- DICP [DICP I202012]
- Foundation of State Key Laboratory of High-efficiency Coal Utilization and Green Chemical Engineering [2019-KF-11]
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In this study, an iron catalyst co-modified with sodium and sulfur was proposed for direct hydrogenation of CO2 to higher alcohols, achieving high space-time yield with over 98% of C2+ alcohols. The synergistic effects of sodium and sulfur played a key role in providing matched molecularly adsorbed CO and alkyl species on the monometallic iron catalyst. Density functional theory modeling also supported the facile formation of alcohols on the Na and S co-modified iron catalyst.
Direct hydrogenation of CO2 to higher alcohols is highly attractive and challenging. Iron catalysts are generally not regarded as ideal candidates, owing to its poor ability for non-dissociative CO activation, and needs to combine with other metals (such as Rh, Pd, Cu) for above process. Herein, we proposed an iron catalyst comodified with Na and S (FeNaS-0.6), achieving a space-time yield of 80.5 mg g(cat)(-1) h(-1) for alcohols, more than 98 % of which corresponds to C2+ alcohols. The synergistic effects of Na and S enable the monometallic iron catalyst to provide matched molecularly adsorbed CO and alkyl species simultaneously required for higher alcohols synthesis. Sulfur existed in the form of sulfate, and its electron-withdrawing effects could transfrom the surrounding Fe sites for CO dissociation to those for non-dissociative CO adsorption. The DFT modeling also confirmed more facile formation of alcohols on the Na and S co-modified iron catalyst.
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