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High-yield production of aromatics over CuFeO2/hierarchical HZSM-5 via CO2 Fischer–Tropsch synthesis.
- Source :
- Green Chemistry; 5/7/2023, Vol. 25 Issue 9, p3570-3584, 15p
- Publication Year :
- 2023
-
Abstract
- The direct conversion of CO<subscript>2</subscript> to aromatics with the aid of renewable hydrogen sources is a promising way to mitigate the CO<subscript>2</subscript> emissions and simultaneously replace the dwindling fossil resources for the production of valuable chemicals. Even though some excellent results have been obtained for the direct conversion of CO<subscript>2</subscript> to aromatics via the methanol-mediated or modified Fischer–Tropsch synthesis (FTS) pathway, the low space–time yield (STY) of aromatics and the high selectivity of C<subscript>1</subscript> by-products (CO and CH<subscript>4</subscript>) are the main bottlenecks. Herein, we demonstrate that the bifunctional catalyst (CuFeO<subscript>2</subscript>/hierarchical HZSM-5) composed of defafossite-CuFeO<subscript>2</subscript> exhibits outstanding catalytic performance for producing olefins from CO<subscript>2</subscript> hydrogenation, and hierarchical HZSM-5 can catalyze the direct CO<subscript>2</subscript> conversion to aromatics with a high efficiency by single pass. Under the optimized reaction conditions, the CuFeO<subscript>2</subscript>/hierarchical HZSM-5 bifunctional catalyst can suppress the total selectivity of CO and CH<subscript>4</subscript> to less than 12% with a high aromatics STY of 431.8 mgCH<subscript>2</subscript> gcat<superscript>−1</superscript> h<superscript>−1</superscript> at a CO<subscript>2</subscript> conversion of 52.8% and outperforms previously reported catalysts. In addition, upon the selective elimination of external surface acidity via epitaxial growth of a Silicalite-1 shell on the hierarchical HZSM-5 surface, the fraction of p-xylene in xylenes is improved from 27.8% to 66.9%. Furthermore, H recycling is realized via the intimate synergy between CuFeO<subscript>2</subscript> and hierarchical HZSM-5 and demonstrated to be significantly vital for improving the aromatics formation. The CO<subscript>2</subscript> adsorbed on CuFeO<subscript>2</subscript> also acts as an acceptor for H species produced from the olefin dehydrogenative aromatization in hierarchical HZSM-5, which in turn increases the aromatics STY by shifting the chemical thermodynamic equilibrium. [ABSTRACT FROM AUTHOR]
- Subjects :
- CHEMICAL equilibrium
EPITAXY
THERMODYNAMIC equilibrium
STYE
ALKENES
Subjects
Details
- Language :
- English
- ISSN :
- 14639262
- Volume :
- 25
- Issue :
- 9
- Database :
- Complementary Index
- Journal :
- Green Chemistry
- Publication Type :
- Academic Journal
- Accession number :
- 163579725
- Full Text :
- https://doi.org/10.1039/d2gc04896e