Layered Double Hydroxide Derivatives for Polyolefin Upcycling

Journal of the American Chemical Society, Journal Year: 2024, Volume and Issue: 146(15), P. 10655 - 10665

Published: April 2, 2024

While Ru-catalyzed hydrogenolysis holds significant promise in converting waste polyolefins into value-added alkane fuels, a major constraint is the high cost of noble metal catalysts. In this work, we propose, for first time, that Co-based catalysts derived from CoAl-layered double hydroxide (LDH) are alternatives efficient polyolefin hydrogenolysis. Leveraging chemical flexibility LDH platform, reveal metallic Co species serve as highly active sites Furthermore, introduced Ni framework to tackle issue restricted hydrogenation ability associated with contiguous Co–Co sites. In-situ analysis indicates integration induces electron transfer and facilitates hydrogen spillover. This dual effect synergistically enhances hydrogenation/desorption olefin intermediates, resulting reduction yield low-value CH4 27.1 12.6%. Through leveraging unique properties LDH, have developed cost-effective sustainable recycling valorization materials.

Language: Английский

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Selective Upcycling of Polyethylene Terephthalate towards High‐valued Oxygenated Chemical Methyl p‐Methyl Benzoate using a Cu/ZrO₂ Catalyst

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(11)

Published: Jan. 10, 2024

Abstract Upgrading of polyethylene terephthalate (PET) waste into valuable oxygenated molecules is a fascinating process, yet it remains challenging. Herein, we developed two‐step strategy involving methanolysis PET to dimethyl (DMT), followed by hydrogenation DMT produce the high‐valued chemical methyl p‐methyl benzoate (MMB) using fixed‐bed reactor and Cu/ZrO 2 catalyst. Interestingly, discovered phase structure ZrO significantly regulates selectivity products. Cu supported on monoclinic (5 %Cu/m‐ZrO ) exhibits an exceptional 86 % for conversion MMB, while tetragonal %Cu/t‐ZrO predominantly produces p‐xylene (PX) with 75 %. The superior MMB over Cu/m‐ZrO can be attributed weaker acid sites present m‐ZrO compared t‐ZrO . This weak acidity leads moderate adsorption capability facilitating its desorption. Furthermore, DFT calculations reveal catalyst shows higher effective energy barrier cleavage second C−O bond Cu/t‐ZrO catalyst; this distinction ensures high MMB. not only presents approach upgrading fine chemicals but also offers controlling primary product in multistep reaction.

Language: Английский

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Photo- and electrochemical processes to convert plastic waste into fuels and high-value chemicals

Chemical Engineering Journal, Journal Year: 2024, Volume and Issue: 482, P. 148827 - 148827

Published: Jan. 18, 2024

Language: Английский

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Full valorisation of waste PET into dimethyl terephthalate and cyclic arylboronic esters

Applied Catalysis B Environment and Energy, Journal Year: 2024, Volume and Issue: 352, P. 124055 - 124055

Published: April 21, 2024

Language: Английский

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Depolymerization mechanisms and closed-loop assessment in polyester waste recycling

Nature Communications, Journal Year: 2024, Volume and Issue: 15(1)

Published: July 25, 2024

Alcoholysis of poly(ethylene terephthalate) (PET) waste to produce monomers, including methanolysis yield dimethyl terephthalate (DMT) and glycolysis generate bis-2-hydroxyethyl (BHET), is a promising strategy in PET management. Here, we introduce an efficient PET-alcoholysis approach utilizing oxygen-vacancy (V

Language: Английский

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