Catalytic Deconstruction of Ethylene Vinyl Acetate Copolymer and Polyethylene Mixtures via Hydroconversion: Challenges and Solutions

Pedro Moura; Pavel A. Kots; Brandon C. Vance; Zoé O.G. Schyns; Sean Najmi; Zachary R. Hinton; Caitlin M. Quinn; Thomas H. Epps; La Shanda T.J. Korley; Dionisios G. Vlachos

doi:10.1021/acssuschemeng.4c01220

Catalytic Deconstruction of Ethylene Vinyl Acetate Copolymer and Polyethylene Mixtures via Hydroconversion: Challenges and Solutions

Pedro Moura, Pavel A. Kots, Brandon C. Vance, Zoé O.G. Schyns, Sean Najmi, Zachary R. Hinton, Caitlin M. Quinn, Thomas H. Epps, La Shanda T.J. Korley, Dionisios G. Vlachos

Chemical and Biomolecular Engineering

Research output: Contribution to journal › Article › peer-review

Abstract

We explore hydrogenolysis over ruthenium supported on zirconia (Ru/ZrO₂) and hydrocracking over platinum (Pt) supported on zeolites as an effective end-of-life strategy for ethylene vinyl acetate (EVA)─a widely used performance heat sealant in hard-to-recycle multilayer packaging. For Ru/ZrO₂ hydrogenolysis, EVA reacts slower than low-density polyethylene (LDPE) and the catalyst deactivates due to carbonaceous deposits originating from polyenes generated in situ during EVA thermal degradation. High H₂ pressures and temperatures can overcome catalyst deactivation; however, CH₄ yields are excessive due to cascade hydrogenolysis stemming from strong C═C/metal interactions. Polyene hydrogenation allows chains anchored by C═C to desorb from Ru, shifting product selectivity from CH₄ to higher-value liquids. Hydrogenolysis of mixed EVA and linear low-density polyethylene (LLDPE), mirroring typical frozen food packaging formulations, results in comparable catalyst activity and CH₄ yield as the pure EVA resin. For Pt/zeolite hydrocracking, pure EVA and EVA:LLDPE mixtures are deconstructed to propane or light naphtha with minimal CH₄ production. Among catalysts tested, Pt/HY gives the highest liquid productivity (g_C5+products/g_cat·h). These findings showcase the recalcitrant nature of EVA and its associated mixtures for Ru/ZrO₂ hydrogenolysis, highlighting that hydrocracking catalysts may be superior for complex packaging waste.

Original language	English (US)
Pages (from-to)	8717-8728
Number of pages	12
Journal	ACS Sustainable Chemistry and Engineering
Volume	12
Issue number	23
DOIs	https://doi.org/10.1021/acssuschemeng.4c01220
State	Published - Jun 10 2024

Keywords

hydrocracking
hydrogenolysis
plastics waste
platinum
ruthenium
valorization

ASJC Scopus subject areas

General Chemistry
Environmental Chemistry
General Chemical Engineering
Renewable Energy, Sustainability and the Environment

Access to Document

10.1021/acssuschemeng.4c01220

Cite this

Moura, P., Kots, P. A., Vance, B. C., Schyns, Z. O. G., Najmi, S., Hinton, Z. R., Quinn, C. M., Epps, T. H., Korley, L. S. T. J., & Vlachos, D. G. (2024). Catalytic Deconstruction of Ethylene Vinyl Acetate Copolymer and Polyethylene Mixtures via Hydroconversion: Challenges and Solutions. ACS Sustainable Chemistry and Engineering, 12(23), 8717-8728. https://doi.org/10.1021/acssuschemeng.4c01220

Moura, P, Kots, PA, Vance, BC, Schyns, ZOG, Najmi, S, Hinton, ZR, Quinn, CM, Epps, TH, Korley, LSTJ & Vlachos, DG 2024, 'Catalytic Deconstruction of Ethylene Vinyl Acetate Copolymer and Polyethylene Mixtures via Hydroconversion: Challenges and Solutions', ACS Sustainable Chemistry and Engineering, vol. 12, no. 23, pp. 8717-8728. https://doi.org/10.1021/acssuschemeng.4c01220

@article{c5cc0dc8313e405ca20febf5ab11d7e1,

title = "Catalytic Deconstruction of Ethylene Vinyl Acetate Copolymer and Polyethylene Mixtures via Hydroconversion: Challenges and Solutions",

abstract = "We explore hydrogenolysis over ruthenium supported on zirconia (Ru/ZrO2) and hydrocracking over platinum (Pt) supported on zeolites as an effective end-of-life strategy for ethylene vinyl acetate (EVA)─a widely used performance heat sealant in hard-to-recycle multilayer packaging. For Ru/ZrO2 hydrogenolysis, EVA reacts slower than low-density polyethylene (LDPE) and the catalyst deactivates due to carbonaceous deposits originating from polyenes generated in situ during EVA thermal degradation. High H2 pressures and temperatures can overcome catalyst deactivation; however, CH4 yields are excessive due to cascade hydrogenolysis stemming from strong C═C/metal interactions. Polyene hydrogenation allows chains anchored by C═C to desorb from Ru, shifting product selectivity from CH4 to higher-value liquids. Hydrogenolysis of mixed EVA and linear low-density polyethylene (LLDPE), mirroring typical frozen food packaging formulations, results in comparable catalyst activity and CH4 yield as the pure EVA resin. For Pt/zeolite hydrocracking, pure EVA and EVA:LLDPE mixtures are deconstructed to propane or light naphtha with minimal CH4 production. Among catalysts tested, Pt/HY gives the highest liquid productivity (gC5+products/gcat·h). These findings showcase the recalcitrant nature of EVA and its associated mixtures for Ru/ZrO2 hydrogenolysis, highlighting that hydrocracking catalysts may be superior for complex packaging waste.",

keywords = "hydrocracking, hydrogenolysis, plastics waste, platinum, ruthenium, valorization",

author = "Pedro Moura and Kots, {Pavel A.} and Vance, {Brandon C.} and Schyns, {Zo{\'e} O.G.} and Sean Najmi and Hinton, {Zachary R.} and Quinn, {Caitlin M.} and Epps, {Thomas H.} and Korley, {La Shanda T.J.} and Vlachos, {Dionisios G.}",

note = "Publisher Copyright: {\textcopyright} 2024 American Chemical Society.",

year = "2024",

month = jun,

day = "10",

doi = "10.1021/acssuschemeng.4c01220",

language = "English (US)",

volume = "12",

pages = "8717--8728",

journal = "ACS Sustainable Chemistry and Engineering",

issn = "2168-0485",

publisher = "American Chemical Society",

number = "23",

}

TY - JOUR

T1 - Catalytic Deconstruction of Ethylene Vinyl Acetate Copolymer and Polyethylene Mixtures via Hydroconversion

T2 - Challenges and Solutions

AU - Moura, Pedro

AU - Kots, Pavel A.

AU - Vance, Brandon C.

AU - Schyns, Zoé O.G.

AU - Najmi, Sean

AU - Hinton, Zachary R.

AU - Quinn, Caitlin M.

AU - Epps, Thomas H.

AU - Korley, La Shanda T.J.

AU - Vlachos, Dionisios G.

PY - 2024/6/10

Y1 - 2024/6/10

N2 - We explore hydrogenolysis over ruthenium supported on zirconia (Ru/ZrO2) and hydrocracking over platinum (Pt) supported on zeolites as an effective end-of-life strategy for ethylene vinyl acetate (EVA)─a widely used performance heat sealant in hard-to-recycle multilayer packaging. For Ru/ZrO2 hydrogenolysis, EVA reacts slower than low-density polyethylene (LDPE) and the catalyst deactivates due to carbonaceous deposits originating from polyenes generated in situ during EVA thermal degradation. High H2 pressures and temperatures can overcome catalyst deactivation; however, CH4 yields are excessive due to cascade hydrogenolysis stemming from strong C═C/metal interactions. Polyene hydrogenation allows chains anchored by C═C to desorb from Ru, shifting product selectivity from CH4 to higher-value liquids. Hydrogenolysis of mixed EVA and linear low-density polyethylene (LLDPE), mirroring typical frozen food packaging formulations, results in comparable catalyst activity and CH4 yield as the pure EVA resin. For Pt/zeolite hydrocracking, pure EVA and EVA:LLDPE mixtures are deconstructed to propane or light naphtha with minimal CH4 production. Among catalysts tested, Pt/HY gives the highest liquid productivity (gC5+products/gcat·h). These findings showcase the recalcitrant nature of EVA and its associated mixtures for Ru/ZrO2 hydrogenolysis, highlighting that hydrocracking catalysts may be superior for complex packaging waste.

AB - We explore hydrogenolysis over ruthenium supported on zirconia (Ru/ZrO2) and hydrocracking over platinum (Pt) supported on zeolites as an effective end-of-life strategy for ethylene vinyl acetate (EVA)─a widely used performance heat sealant in hard-to-recycle multilayer packaging. For Ru/ZrO2 hydrogenolysis, EVA reacts slower than low-density polyethylene (LDPE) and the catalyst deactivates due to carbonaceous deposits originating from polyenes generated in situ during EVA thermal degradation. High H2 pressures and temperatures can overcome catalyst deactivation; however, CH4 yields are excessive due to cascade hydrogenolysis stemming from strong C═C/metal interactions. Polyene hydrogenation allows chains anchored by C═C to desorb from Ru, shifting product selectivity from CH4 to higher-value liquids. Hydrogenolysis of mixed EVA and linear low-density polyethylene (LLDPE), mirroring typical frozen food packaging formulations, results in comparable catalyst activity and CH4 yield as the pure EVA resin. For Pt/zeolite hydrocracking, pure EVA and EVA:LLDPE mixtures are deconstructed to propane or light naphtha with minimal CH4 production. Among catalysts tested, Pt/HY gives the highest liquid productivity (gC5+products/gcat·h). These findings showcase the recalcitrant nature of EVA and its associated mixtures for Ru/ZrO2 hydrogenolysis, highlighting that hydrocracking catalysts may be superior for complex packaging waste.

KW - hydrocracking

KW - hydrogenolysis

KW - plastics waste

KW - platinum

KW - ruthenium

KW - valorization

UR - http://www.scopus.com/inward/record.url?scp=85195050781&partnerID=8YFLogxK

UR - http://www.scopus.com/inward/citedby.url?scp=85195050781&partnerID=8YFLogxK

U2 - 10.1021/acssuschemeng.4c01220

DO - 10.1021/acssuschemeng.4c01220

M3 - Article

AN - SCOPUS:85195050781

SN - 2168-0485

VL - 12

SP - 8717

EP - 8728

JO - ACS Sustainable Chemistry and Engineering

JF - ACS Sustainable Chemistry and Engineering

IS - 23

ER -

Catalytic Deconstruction of Ethylene Vinyl Acetate Copolymer and Polyethylene Mixtures via Hydroconversion: Challenges and Solutions

Abstract

Keywords

ASJC Scopus subject areas

Access to Document

Other files and links

Fingerprint

Cite this