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Role of Bifunctional Ru/Acid Catalysts in the Selective Hydrocracking of Polyethylene and Polypropylene Waste to Liquid Hydrocarbons

  • Julie E. Rorrer
    Julie E. Rorrer
    Department of Chemical Engineering, Massachusetts Institute of Technology, 77 Massachusetts Avenue, Cambridge, Massachusetts02139, United States
  • Amani M. Ebrahim
    Amani M. Ebrahim
    SLAC National Accelerator Laboratory, Menlo Park, California94025, United States
    BOTTLE Consortium, Golden, Colorado80401, United States
  • Ydna Questell-Santiago
    Ydna Questell-Santiago
    Department of Chemical Engineering, Massachusetts Institute of Technology, 77 Massachusetts Avenue, Cambridge, Massachusetts02139, United States
  • Jie Zhu
    Jie Zhu
    Department of Chemical Engineering, Massachusetts Institute of Technology, 77 Massachusetts Avenue, Cambridge, Massachusetts02139, United States
    More by Jie Zhu
  • Clara Troyano-Valls
    Clara Troyano-Valls
    Department of Chemical Engineering, Massachusetts Institute of Technology, 77 Massachusetts Avenue, Cambridge, Massachusetts02139, United States
  • Arun S. Asundi
    Arun S. Asundi
    SLAC National Accelerator Laboratory, Menlo Park, California94025, United States
    BOTTLE Consortium, Golden, Colorado80401, United States
  • Anna E. Brenner
    Anna E. Brenner
    Department of Chemical Engineering, Massachusetts Institute of Technology, 77 Massachusetts Avenue, Cambridge, Massachusetts02139, United States
  • Simon R. Bare
    Simon R. Bare
    SLAC National Accelerator Laboratory, Menlo Park, California94025, United States
    BOTTLE Consortium, Golden, Colorado80401, United States
  • Christopher J. Tassone
    Christopher J. Tassone
    SLAC National Accelerator Laboratory, Menlo Park, California94025, United States
    BOTTLE Consortium, Golden, Colorado80401, United States
  • Gregg T. Beckham
    Gregg T. Beckham
    Renewable Resources and Enabling Sciences Center, National Renewable Energy Laboratory, Golden, Colorado80401, United States
    BOTTLE Consortium, Golden, Colorado80401, United States
  • , and 
  • Yuriy Román-Leshkov*
    Yuriy Román-Leshkov
    Department of Chemical Engineering, Massachusetts Institute of Technology, 77 Massachusetts Avenue, Cambridge, Massachusetts02139, United States
    *Email: [email protected]
Cite this: ACS Catal. 2022, 12, 22, 13969–13979
Publication Date (Web):October 31, 2022
https://doi.org/10.1021/acscatal.2c03596
Copyright © 2022 American Chemical Society

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    Abstract

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    Hydrogenolysis of C–C bonds over Ru-based catalysts has emerged as a deconstruction strategy to convert single-use polyolefin waste to liquid alkanes at relatively mild conditions, but this approach exhibits limitations, including methane formation resulting from terminal C–C bond scission. In this study, a variety of catalysts were investigated for the reductive deconstruction of polyethylene (PE) and polypropylene (PP) to identify supports that promote nonterminal C–C bond scission. We found that Ru nanoparticles supported on Brønsted-acidic zeolites with the faujasite (FAU) and Beta (BEA) topologies were highly active for the cleavage of C–C bonds in PE and PP, exhibiting improved liquid yields and suppressed methane formation. For the deconstruction of PE, supporting ruthenium nanoparticles (5 wt %) on FAU increased the yields of liquid alkanes to 67% compared to 33% over an inert silica support (5 wt % Ru/SiO2) at 200 °C, 16 h, under 30 bar of H2. A dramatic selectivity enhancement toward liquid hydrocarbons was also observed for PP over Ru/FAU and Ru/BEA compared to Ru/SiO2. To understand the origin of this selectivity improvement, a combination of ex situ and operando characterization techniques were used to reveal that both catalyst structure and acidity play key roles in PE and PP conversion. Operando X-ray absorption spectroscopy studies with model polyolefins over Ru-supported catalysts with varying acidity levels revealed that the local chemical environment of Ru[0] during the reaction is consistent across multiple acidic supports, although the onset of reduction during synthesis of the nanoparticles varies across different supports. These results, combined with reactivity data, demonstrate the importance of the acid-noble metal cooperativity in promoting selective C–C bond scission toward liquid alkanes that shifts the mechanism from hydrogenolysis to ideal hydrocracking.

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    Cited By

    This article is cited by 9 publications.

    1. Jun Zhi Tan, Maaso Ortega, Sophia A. Miller, Cole W. Hullfish, Hojoon Kim, Sungmin Kim, Wenda Hu, Jian Zhi Hu, Johannes A. Lercher, Bruce E. Koel, Michele L. Sarazen. Catalytic Consequences of Hierarchical Pore Architectures within MFI and FAU Zeolites for Polyethylene Conversion. ACS Catalysis 2024, 14 (10) , 7536-7552. https://doi.org/10.1021/acscatal.4c01213
    2. Xinru Zhou, Xinlei Han, Zhengyan Qu, Jiuxuan Zhang, Feng Zeng, Zhenchen Tang, Rizhi Chen. Hierarchical FAU Zeolites Boosting the Hydrocracking of Polyolefin Waste into Liquid Fuels. ACS Sustainable Chemistry & Engineering 2024, 12 (15) , 6013-6022. https://doi.org/10.1021/acssuschemeng.4c01097
    3. Shaodan Xu, Junhong Tang, Li Fu. Catalytic Strategies for the Upcycling of Polyolefin Plastic Waste. Langmuir 2024, 40 (8) , 3984-4000. https://doi.org/10.1021/acs.langmuir.3c03195
    4. Wilson C. Edenfield, Alexander H. Mason, Qingheng Lai, Amol Agarwal, Takeshi Kobayashi, Yosi Kratish, Tobin J. Marks. Rapid Polyolefin Plastic Hydrogenolysis Mediated by Single-Site Heterogeneous Electrophilic/Cationic Organo-group IV Catalysts. ACS Catalysis 2024, 14 (1) , 554-565. https://doi.org/10.1021/acscatal.3c05161
    5. Fabio Colasuonno, Martina Lessio. Thermodynamic and Kinetic Insights into Hydrogen Adsorption and Dissociation on the Ru (0001) Surface under STM and Catalytic Conditions. The Journal of Physical Chemistry C 2023, 127 (49) , 23645-23653. https://doi.org/10.1021/acs.jpcc.3c05348
    6. Cole W. Hullfish, Jun Zhi Tan, Hayat I. Adawi, Michele L. Sarazen. Toward Intrinsic Catalytic Rates and Selectivities of Zeolites in the Presence of Limiting Diffusion and Deactivation. ACS Catalysis 2023, 13 (19) , 13140-13150. https://doi.org/10.1021/acscatal.3c03559
    7. Bernard Whajah, Joseph N. Heil, Cameron L. Roman, James A. Dorman, Kerry M. Dooley. Zeolite Supported Pt for Depolymerization of Polyethylene by Induction Heating. Industrial & Engineering Chemistry Research 2023, 62 (22) , 8635-8643. https://doi.org/10.1021/acs.iecr.2c04568
    8. Junde Wei, Jieyi Liu, Weihao Zeng, Zichen Dong, Jingkuo Song, Sibao Liu, Guozhu Liu. Catalytic hydroconversion processes for upcycling plastic waste to fuels and chemicals. Catalysis Science & Technology 2023, 13 (5) , 1258-1280. https://doi.org/10.1039/D2CY01886A
    9. Shenglu Lu, Yaxuan Jing, Shengchao Jia, Mohsen Shakouri, Yongfeng Hu, Xiaohui Liu, Yong Guo, Yanqin Wang. Enhanced Production of Liquid Alkanes from Waste Polyethylene via the Electronic Effect‐Favored C secondary −C secondary Bond Cleavage. ChemCatChem 2023, 15 (3) https://doi.org/10.1002/cctc.202201375

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