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Selective Upcycling of Polyethylene Terephthalate towards High‐valued Oxygenated Chemical Methyl p‐Methyl Benzoate using a Cu/ZrO2 Catalyst.
- Source :
-
Angewandte Chemie International Edition . 3/11/2024, Vol. 63 Issue 11, p1-8. 8p. - Publication Year :
- 2024
-
Abstract
- Upgrading of polyethylene terephthalate (PET) waste into valuable oxygenated molecules is a fascinating process, yet it remains challenging. Herein, we developed a two‐step strategy involving methanolysis of PET to dimethyl terephthalate (DMT), followed by hydrogenation of DMT to produce the high‐valued chemical methyl p‐methyl benzoate (MMB) using a fixed‐bed reactor and a Cu/ZrO2 catalyst. Interestingly, we discovered the phase structure of ZrO2 significantly regulates the selectivity of products. Cu supported on monoclinic ZrO2 (5 %Cu/m‐ZrO2) exhibits an exceptional selectivity of 86 % for conversion of DMT to MMB, while Cu supported on tetragonal ZrO2 (5 %Cu/t‐ZrO2) predominantly produces p‐xylene (PX) with selectivity of 75 %. The superior selectivity of MMB over Cu/m‐ZrO2 can be attributed to the weaker acid sites present on m‐ZrO2 compared to t‐ZrO2. This weak acidity of m‐ZrO2 leads to a moderate adsorption capability of MMB, and facilitating its desorption. Furthermore, DFT calculations reveal Cu/m‐ZrO2 catalyst shows a higher effective energy barrier for cleavage of second C−O bond compared to Cu/t‐ZrO2 catalyst; this distinction ensures the high selectivity of MMB. This catalyst not only presents an approach for upgrading of PET waste into fine chemicals but also offers a strategy for controlling the primary product in a multistep hydrogenation reaction. [ABSTRACT FROM AUTHOR]
Details
- Language :
- English
- ISSN :
- 14337851
- Volume :
- 63
- Issue :
- 11
- Database :
- Academic Search Index
- Journal :
- Angewandte Chemie International Edition
- Publication Type :
- Academic Journal
- Accession number :
- 175826557
- Full Text :
- https://doi.org/10.1002/anie.202319896