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Selective production of bio-based para-xylene over an FeOx-modified Pd/Al2O3 catalyst.
- Source :
- Green Chemistry; 7/7/2020, Vol. 22 Issue 13, p4341-4349, 9p
- Publication Year :
- 2020
-
Abstract
- para-Xylene (PX) is a basic building block of polyethylene terephthalate, which is currently produced from petroleum resources. Developing a renewable route to PX is highly desirable to address both economic and environmental concerns. Several attempts used noble metal catalysts, e.g. Pd/Al<subscript>2</subscript>O<subscript>3</subscript>, to synthesize PX from biomass-derived 4-methyl-3-cyclohexene-1-carboxaldehyde (4-MCHCA), but suffered from a severe decarbonylation reaction, resulting in toluene as the main product. In this paper, we report an FeO<subscript>x</subscript> modification strategy to suppress the decarbonylation reaction on a Pd/Al<subscript>2</subscript>O<subscript>3</subscript> catalyst, leading to a drastic shift in selectivity towards PX with a yield up to 81% via a cascade dehydroaromatization–hydrodeoxygenation (DHA–HDO) pathway. Characterization and control experiments revealed that the electron density of Pd sites decreased in an FeO<subscript>x</subscript>-modified Pd/Al<subscript>2</subscript>O<subscript>3</subscript> catalyst compared to Pd/Al<subscript>2</subscript>O<subscript>3</subscript>, thus tuning the preferential adsorption mode of the substrate from η<superscript>2</superscript>-(C,O), the key transition state of the decarbonylation reaction, to the η<superscript>1</superscript>-(O) mode that favors the hydrodeoxygenation process. Notably, this designed catalyst is highly stable and is readily applicable in the selective synthesis of a broad range of desired aromatic chemicals via the same DHA–HDO pathway from cyclohex-3-enecarbaldehyde derivatives. Overall, this work develops a controllable catalyst modification strategy that tailors an efficient catalyst for petroleum-independent bio-PX synthesis. [ABSTRACT FROM AUTHOR]
Details
- Language :
- English
- ISSN :
- 14639262
- Volume :
- 22
- Issue :
- 13
- Database :
- Complementary Index
- Journal :
- Green Chemistry
- Publication Type :
- Academic Journal
- Accession number :
- 144410711
- Full Text :
- https://doi.org/10.1039/d0gc00944j