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DOE OSTI · 3218395

Catalytic Autoxidation for Depolymerization of Multilayer Plastic Films

Lahive, Ciaran W. [National Laboratory of the Rockies (NLR), Golden, CO (United States). Renewable Resources and Enabling Sciences Center; BOTTLE Consortium, Golden, CO (United States)]·Cuthbertson, Amy A. [National Laboratory of the Rockies (NLR), Golden, CO (United States). Renewable Resources and Enabling Sciences Center; BOTTLE Consortium, Golden, CO (United States)]·Walsh, Anna N. [National Laboratory of the Rockies (NLR), Golden, CO (United States). Renewable Resources and Enabling Sciences Center]·Reiber, Sydney E. [National Laboratory of the Rockies (NLR), Golden, CO (United States). Renewable Resources and Enabling Sciences Center; BOTTLE Consortium, Golden, CO (United States)]·Alt, Hannah M. [National Laboratory of the Rockies (NLR), Golden, CO (United States). Renewable Resources and Enabling Sciences Center; BOTTLE Consortium, Golden, CO (United States)] (ORCID:0000000265597800)·Black, Brenna A. [National Laboratory of the Rockies (NLR), Golden, CO (United States). Renewable Resources and Enabling Sciences Center; BOTTLE Consortium, Golden, CO (United States)] (ORCID:0000000300357942)·Botello, Christopher [National Laboratory of the Rockies (NLR), Golden, CO (United States). Renewable Resources and Enabling Sciences Center; Rice Univ., Houston, TX (United States)]·DesVeaux, Jason S. [National Laboratory of the Rockies (NLR), Golden, CO (United States). Renewable Resources and Enabling Sciences Center; BOTTLE Consortium, Golden, CO (United States)] (ORCID:0000000179266327)·Lask, Spencer [National Laboratory of the Rockies (NLR), Golden, CO (United States). Renewable Resources and Enabling Sciences Center; BOTTLE Consortium, Golden, CO (United States)]·Lincoln, Clarissa [National Laboratory of the Rockies (NLR), Golden, CO (United States). Renewable Resources and Enabling Sciences Center; BOTTLE Consortium, Golden, CO (United States)]·Michener, William E. [National Laboratory of the Rockies (NLR), Golden, CO (United States). Renewable Resources and Enabling Sciences Center; BOTTLE Consortium, Golden, CO (United States)] (ORCID:0000000160237286)·Miscall, Joel [National Laboratory of the Rockies (NLR), Golden, CO (United States). Renewable Resources and Enabling Sciences Center; BOTTLE Consortium, Golden, CO (United States)]·Ramirez, Kelsey J. [National Laboratory of the Rockies (NLR), Golden, CO (United States). Renewable Resources and Enabling Sciences Center; BOTTLE Consortium, Golden, CO (United States)]·Stanley, Lisa M. [National Laboratory of the Rockies (NLR), Golden, CO (United States). Renewable Resources and Enabling Sciences Center; BOTTLE Consortium, Golden, CO (United States)]·Woodworth, Sean P. [National Laboratory of the Rockies (NLR), Golden, CO (United States). Renewable Resources and Enabling Sciences Center; BOTTLE Consortium, Golden, CO (United States)] (ORCID:0000000337929553)·Stahl, Shannon S. [BOTTLE Consortium, Golden, CO (United States); Univ. of Wisconsin, Madison, WI (United States)] (ORCID:0000000290007665)·Beckham, Gregg T. [National Laboratory of the Rockies (NLR), Golden, CO (United States). Renewable Resources and Enabling Sciences Center; BOTTLE Consortium, Golden, CO (United States)] (ORCID:000000023480212X)

Abstract

Recycling multilayer plastic films is challenged by a diversity of polymers, prompting development of new recycling methods. For the depolymerization of mixed polymers like those in multilayer films, metal-catalyzed autoxidation offers a versatile chemical recycling method to deconstruct multiple polymers to useful oxygenates. Here, we demonstrate that catalytic autoxidation is effective for depolymerizing multilayer films across diverse chemistries. We investigated conditions for a model polyethylene substrate using a Co, Mn, and Br cocatalyst system, achieving full carbon closure with oxygenated small molecules contributing up to 48 mol% carbon. Subsequently, we characterized product distributions for several common polymers used in multilayer films using high-resolution mass spectrometry (HRMS) and developed analytical methods to quantify the resulting complex product streams. Optimized conditions for polyethylene were applied to 11 multilayer plastic films containing 10 different polymers, including films with nonpolymeric potential disrupters like aluminum foil and titanium dioxide, showing that catalytic autoxidation is effective across a broad range of polymer types and is resistant to disrupters and additives. The generation of CO 2 in these reactions overall suggests that both reaction engineering and modifications to the reaction conditions will be required to achieve higher yields of soluble oxygenated products.

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BibTeXRIS

Lahive, Ciaran W. [National Laboratory of the Rockies (NLR), Golden, CO (United States). Renewable Resources and Enabling Sciences Center; BOTTLE Consortium, Golden, CO (United States)], Cuthbertson, Amy A. [National Laboratory of the Rockies (NLR), Golden, CO (United States). Renewable Resources and Enabling Sciences Center; BOTTLE Consortium, Golden, CO (United States)], Walsh, Anna N. [National Laboratory of the Rockies (NLR), Golden, CO (United States). Renewable Resources and Enabling Sciences Center], Reiber, Sydney E. [National Laboratory of the Rockies (NLR), Golden, CO (United States). Renewable Resources and Enabling Sciences Center; BOTTLE Consortium, Golden, CO (United States)], Alt, Hannah M. [National Laboratory of the Rockies (NLR), Golden, CO (United States). Renewable Resources and Enabling Sciences Center; BOTTLE Consortium, Golden, CO (United States)] (ORCID:0000000265597800), Black, Brenna A. [National Laboratory of the Rockies (NLR), Golden, CO (United States). Renewable Resources and Enabling Sciences Center; BOTTLE Consortium, Golden, CO (United States)] (ORCID:0000000300357942), Botello, Christopher [National Laboratory of the Rockies (NLR), Golden, CO (United States). Renewable Resources and Enabling Sciences Center; Rice Univ., Houston, TX (United States)], DesVeaux, Jason S. [National Laboratory of the Rockies (NLR), Golden, CO (United States). Renewable Resources and Enabling Sciences Center; BOTTLE Consortium, Golden, CO (United States)] (ORCID:0000000179266327), Lask, Spencer [National Laboratory of the Rockies (NLR), Golden, CO (United States). Renewable Resources and Enabling Sciences Center; BOTTLE Consortium, Golden, CO (United States)], Lincoln, Clarissa [National Laboratory of the Rockies (NLR), Golden, CO (United States). Renewable Resources and Enabling Sciences Center; BOTTLE Consortium, Golden, CO (United States)], Michener, William E. [National Laboratory of the Rockies (NLR), Golden, CO (United States). Renewable Resources and Enabling Sciences Center; BOTTLE Consortium, Golden, CO (United States)] (ORCID:0000000160237286), Miscall, Joel [National Laboratory of the Rockies (NLR), Golden, CO (United States). Renewable Resources and Enabling Sciences Center; BOTTLE Consortium, Golden, CO (United States)], Ramirez, Kelsey J. [National Laboratory of the Rockies (NLR), Golden, CO (United States). Renewable Resources and Enabling Sciences Center; BOTTLE Consortium, Golden, CO (United States)], Stanley, Lisa M. [National Laboratory of the Rockies (NLR), Golden, CO (United States). Renewable Resources and Enabling Sciences Center; BOTTLE Consortium, Golden, CO (United States)], Woodworth, Sean P. [National Laboratory of the Rockies (NLR), Golden, CO (United States). Renewable Resources and Enabling Sciences Center; BOTTLE Consortium, Golden, CO (United States)] (ORCID:0000000337929553), Stahl, Shannon S. [BOTTLE Consortium, Golden, CO (United States); Univ. of Wisconsin, Madison, WI (United States)] (ORCID:0000000290007665), Beckham, Gregg T. [National Laboratory of the Rockies (NLR), Golden, CO (United States). Renewable Resources and Enabling Sciences Center; BOTTLE Consortium, Golden, CO (United States)] (ORCID:000000023480212X). 2026-04-13. Catalytic Autoxidation for Depolymerization of Multilayer Plastic Films. https://doi.org/10.1002/cssc.70564

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