Catalytic Consequences of Hierarchical Pore Architectures within MFI and FAU Zeolites for Polyethylene Conversion

Tan, Jun Zhi; Ortega, Maaso; Miller, Sophia A.; Hullfish, Cole W.; Kim, Hojoon; Kim, Sungmin; Hu, Wenda; Hu, Jian Zhi; Lercher, Johannes A.; Koel, Bruce E.; Sarazen, Michele L.

doi:10.1021/acscatal.4c01213

Title: Catalytic Consequences of Hierarchical Pore Architectures within MFI and FAU Zeolites for Polyethylene Conversion

Journal Article · 29 April 2024 · ACS Catalysis

DOI: https://doi.org/10.1021/acscatal.4c01213 · OSTI ID:2446686

^[1]; Ortega, Maaso ^[1]; Miller, Sophia A. ^[1];

^[1]; Kim, Hojoon ^[1];

^[2]; Hu, Wenda ^[3];

^[4];

^[5];

^[1];

^[1]

Princeton Univ., NJ (United States)
Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)
Washington State Univ., Pullman, WA (United States)
Pacific Northwest National Laboratory (PNNL), Richland, WA (United States); Washington State Univ., Pullman, WA (United States)
Pacific Northwest National Laboratory (PNNL), Richland, WA (United States); Technische Univ. München, Garching (Germany)

The benefits of hierarchical zeolites for the conversion of bulky molecules like polymeric waste have been reported in the literature; however, the impact of mesopore sizes and connectivities on rates, product selectivities, and catalyst deactivation in the context of plastic upcycling has not been systematically probed. Here, in this study, we synthesized a suite of hierarchical MFI and FAU zeolites via desilication under varying conditions for metal-free polyethylene conversion reactions under batch and flow conditions (473–523 K). Polyethylene (solid) conversion rates (normalized by Bro̷nsted acid site density) were higher on hierarchical than parent microporous MFI regardless of mesopore connectivities, i.e., open or constricted, suggesting that the incorporation of mesopores facilitates diffusion of intermediate products to access medium-pore protons for successive scission events. Furthermore, higher branched:linear gaseous product ratios were produced on hierarchical than parent MFI, since mesopores allow for egress of bulkier molecules without undergoing further secondary events, e.g., isomerization back to linear alkanes/alkenes or beta scission. Solid conversion rates on hierarchical FAU synthesized via desilication with cetyltrimethylammonium bromide (CTABr), however, were not higher than parent FAU, likely because the presence of CTABr facilitates recrystallization of leached species to form composites (hierarchical FAU and ordered mesoporous materials) with more isolated mesopores. The stagnation in rates, despite increased mesopore volumes (>0.22 cm³ g^–1), highlights the importance of confinement effects provided by micropores for cleaving C–C bonds at modest reaction conditions. In situ ¹H MAS NMR performed on polyethylene with MFI zeolite show that PE isomerizes (and potentially deconstructs) at temperatures near 450 K, highlighting the role of Bro̷nsted acid sites in activating C–C bonds under mild reaction conditions. Catalyst recyclability studies showed that all catalysts undergo deactivation during plastic upcycling reactions, but to varying extents. Overall, hierarchical materials have better catalyst stability than parent materials, although the differences in stability between hierarchical and parent FAU are smaller than those for MFI. Taken together, these findings demonstrate how rates, selectivities, and catalyst deactivation from plastic upcycling reactions can be controlled via fine-tuning the identity and connectivity of mesopores.

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Research Organization:: Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

Sponsoring Organization:: National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division (CSGB)

Grant/Contract Number:: AC05-76RL01830

OSTI ID:: 2446686

Report Number(s):: PNNL-SA--197621

Journal Information:: ACS Catalysis, Journal Name: ACS Catalysis Journal Issue: 10 Vol. 14; ISSN 2155-5435

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
catalyst deactivation
hierarchical zeolites
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postsynthetic modification
solid acid catalysis

Title: Catalytic Consequences of Hierarchical Pore Architectures within MFI and FAU Zeolites for Polyethylene Conversion

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References (85)

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