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1.
Angew Chem Int Ed Engl ; : e202408561, 2024 Jun 25.
Artículo en Inglés | MEDLINE | ID: mdl-38923654

RESUMEN

We present an innovative process for directly transforming poly(ethylene terephthalate) (PET), a polymer extensively used in food and beverage packaging, into trans-isomer-enriched 1,4-cyclo- hexanedimethanol (CHDM), a key ingredient in advanced specialty polymers. Our approach leverages a dual-catalyst system featuring palladium on reduced graphene oxide (Pd/r-GO) and oxalate-gel-derived copper-zinc oxide (og-CuZn), utilizing hydrogenation/hydrog- enolysis relay catalysis. This method efficiently transforms PET into polyethylene-1,4-cyclohexanedicarboxylate (PECHD), which is then converted into CHDM with an impressive overall yield of 95% in a two-stage process. Our process effectively handles various post-consumer PET plastics, converting them into CHDM with yields between 78% and 89% across different substrates. Additionally, we demonstrate the applicability and scalability of this approach through a temperature-programmed three-stage relay process on a 10-gram scale, which results in purified CHDM with an isolated yield of 87% and a notably higher trans/cis ratio of up to 4.09/1, far exceeding that of commercially available CHDM. This research not only provides a viable route for repurposing PET waste but also enhances the control of selectivity patterns in multistage relay catalysis.

2.
Chem Commun (Camb) ; 60(58): 7483-7486, 2024 Jul 16.
Artículo en Inglés | MEDLINE | ID: mdl-38939946

RESUMEN

Here we present a hybrid catalytic pathway for efficient synthesis of 5-aminomethyl-2-furancarboxylic acid (AMFC), a bio-based nylon-6 analogue monomer, from 5-hydroxymethylfurfural (HMF). This method combines homogeneous-catalyzed selective oxidation of HMF to 5-formyl-2-furancarboxylic acid (FFCA) with heterogeneous-catalyzed reductive amination using ammonia as the nitrogen source. Through this relay strategy, we achieve significant enhancements in overall efficiency, resulting in isolation yields of up to 92% for highly selective and scalable AMFC production from HMF.

3.
ChemSusChem ; 16(24): e202301128, 2023 Dec 19.
Artículo en Inglés | MEDLINE | ID: mdl-37793185

RESUMEN

As plastic waste pollution continues to pose significant challenges to our environment, it is crucial to develop eco-friendly processes that can transform plastic waste into valuable chemical products in line with the principles of green chemistry. One major challenge is breaking down plastic waste into economically valuable carbon resources. This however presents an opportunity for sustainable circular economies. In this regard, a flexible approach is presented that involves the use of supported-metal catalysts to selectively degrade polylactide waste using molecular oxygen. This protocol has several advantages, including its operation under organic solvent-free and mild conditions, simplicity of implementation, and high atom efficiency, resulting in minimal waste. This approach enables the chemical upcycling of polylactide waste into valuable chemicals such as pyruvic acid, acetic acid, or a mixture containing equimolar amounts of acetic acid and formaldehyde, providing a viable alternative for accessing key value-added feedstocks from waste and spent plastics.

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