Supported Platinum Nanoparticles Catalyzed Carbon–Carbon Bond Cleavage of Polyolefins: Role of the Oxide Support Acidity

Lamb, Jessica V.; Lee, Yu-Hsuan; Sun, Jiakai; Byron, Carly; Uppuluri, Ritesh; Kennedy, Robert M.; Meng, Chao; Behera, Ranjan K.; Wang, Yi-Yu; Qi, Long; Sadow, Aaron D.; Huang, Wenyu; Ferrandon, Magali S.; Scott, Susannah L.; Poeppelmeier, Kenneth R.; Abu-Omar, Mahdi M.; Delferro, Massimiliano

doi:10.1021/acsami.3c15350

Title: Supported Platinum Nanoparticles Catalyzed Carbon–Carbon Bond Cleavage of Polyolefins: Role of the Oxide Support Acidity

Journal Article · 23 February 2024 · ACS Applied Materials and Interfaces

DOI: https://doi.org/10.1021/acsami.3c15350 · OSTI ID:2481424

^[1]; Lee, Yu-Hsuan ^[2]; Sun, Jiakai ^[2]; Byron, Carly ^[1]; Uppuluri, Ritesh ^[3];

^[4]; Meng, Chao ^[5]; Behera, Ranjan K. ^[5]; Wang, Yi-Yu ^[5];

^[6];

^[7];

^[7]; Ferrandon, Magali S. ^[1];

^[2];

^[8]; Abu-Omar, Mahdi M. ^[2];

^[1]

Argonne National Laboratory (ANL), Argonne, IL (United States)
Univ. of California, Santa Barbara, CA (United States)
Northwestern Univ., Evanston, IL (United States)
Aeternal Upcycling, Inc., Chicago, IL (United States)
Iowa State Univ., Ames, IA (United States)
Ames Laboratory (AMES), Ames, IA (United States)
Iowa State Univ., Ames, IA (United States); Ames Laboratory (AMES), Ames, IA (United States)
Argonne National Laboratory (ANL), Argonne, IL (United States); Northwestern Univ., Evanston, IL (United States)

Supported platinum nanoparticle catalysts are known to convert polyolefins to high-quality liquid hydrocarbons using hydrogen under relatively mild conditions. To date, few studies using platinum grafted onto various metal oxide (M_xO_y) supports have been undertaken to understand the role of the acidity of the oxide support in the carbon-carbon bond cleavage of polyethylene under consistent catalytic conditions. Specifically, two Pt/M_xO_y catalysts (M_xO_y = SrTiO₃ and SiO₂-Al₂O₃; Al = 3.0 wt %, target Pt loading 2 wt % Pt similar to 1.5 nm), under identical catalytic polyethylene hydrogenolysis conditions (T = 300 degree celsius, P(H₂) = 170 psi, t = 24 h; M_w = similar to 3,800 g/mol, M_n = similar to 1,100 g/mol, D = 3.45, N_branch/100C = 1.0), yielded a narrow distribution of hydrocarbons with molecular weights in the range of lubricants (M_w = < 600 g/mol; M_n < 400 g/mol; D = 1.5). While Pt/SrTiO₃ formed saturated hydrocarbons with negligible branching, Pt/SiO₂-Al₂O₃ formed partially unsaturated hydrocarbons (<1 mol % alkenes and similar to 4 mol % alkyl aromatics) with increased branch density (N_branch/100C = 5.5). Further investigations suggest evidence for a competitive hydrocracking mechanism occurring alongside hydrogenolysis, stemming from the increased acidity of Pt/SiO₂-Al₂O₃ compared to Pt/SrTiO₃. Additionally, the products of these polymer deconstruction reactions were found to be independent of the polyethylene feedstock, allowing the potential to upcycle polyethylenes with various properties into a value-added product.

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Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE), Energy Efficiency Office. Advanced Materials & Manufacturing Technologies Office (AMMTO); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)

Grant/Contract Number:: AC02-06CH11357; AC02-07CH11358

OSTI ID:: 2481424

Report Number(s):: CRADA A22111; 186840

Journal Information:: ACS Applied Materials and Interfaces, Journal Name: ACS Applied Materials and Interfaces Journal Issue: 9 Vol. 16; ISSN 1944-8244

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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