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Electronic modulation of metal-support interactions improves polypropylene hydrogenolysis over ruthenium catalysts

Author

Listed:
  • Pavel A. Kots

    (University of Delaware)

  • Tianjun Xie

    (University of Delaware)

  • Brandon C. Vance

    (University of Delaware
    University of Delaware)

  • Caitlin M. Quinn

    (University of Delaware)

  • Matheus Dorneles Mello

    (Brookhaven National Laboratory)

  • J. Anibal Boscoboinik

    (Brookhaven National Laboratory)

  • Cong Wang

    (University of Delaware)

  • Pawan Kumar

    (University of Pennsylvania)

  • Eric A. Stach

    (University of Pennsylvania)

  • Nebojsa S. Marinkovic

    (Columbia University)

  • Lu Ma

    (Brookhaven National Laboratory)

  • Steven N. Ehrlich

    (Brookhaven National Laboratory)

  • Dionisios G. Vlachos

    (University of Delaware
    University of Delaware)

Abstract

Ruthenium (Ru) is the one of the most promising catalysts for polyolefin hydrogenolysis. Its performance varies widely with the support, but the reasons remain unknown. Here, we introduce a simple synthetic strategy (using ammonia as a modulator) to tune metal-support interactions and apply it to Ru deposited on titania (TiO2). We demonstrate that combining deuterium nuclear magnetic resonance spectroscopy with temperature variation and density functional theory can reveal the complex nature, binding strength, and H amount. H2 activation occurs heterolytically, leading to a hydride on Ru, an H+ on the nearest oxygen, and a partially positively charged Ru. This leads to partial reduction of TiO2 and high coverages of H for spillover, showcasing a threefold increase in hydrogenolysis rates. This result points to the key role of the surface hydrogen coverage in improving hydrogenolysis catalyst performance.

Suggested Citation

  • Pavel A. Kots & Tianjun Xie & Brandon C. Vance & Caitlin M. Quinn & Matheus Dorneles Mello & J. Anibal Boscoboinik & Cong Wang & Pawan Kumar & Eric A. Stach & Nebojsa S. Marinkovic & Lu Ma & Steven N., 2022. "Electronic modulation of metal-support interactions improves polypropylene hydrogenolysis over ruthenium catalysts," Nature Communications, Nature, vol. 13(1), pages 1-11, December.
    • Handle: RePEc:nat:natcom:v:13:y:2022:i:1:d:10.1038_s41467-022-32934-5
    DOI: 10.1038/s41467-022-32934-5
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    References listed on IDEAS

    as
    1. Jiajia Zheng & Sangwon Suh, 2019. "Strategies to reduce the global carbon footprint of plastics," Nature Climate Change, Nature, vol. 9(5), pages 374-378, May.
    2. Jun Zhou & Zhe Gao & Guolei Xiang & Tianyu Zhai & Zikai Liu & Weixin Zhao & Xin Liang & Leyu Wang, 2022. "Interfacial compatibility critically controls Ru/TiO2 metal-support interaction modes in CO2 hydrogenation," Nature Communications, Nature, vol. 13(1), pages 1-10, December.
    3. Yaru Zhang & Xiaoli Yang & Xiaofeng Yang & Hongmin Duan & Haifeng Qi & Yang Su & Binglian Liang & Huabing Tao & Bin Liu & De Chen & Xiong Su & Yanqiang Huang & Tao Zhang, 2020. "Tuning reactivity of Fischer–Tropsch synthesis by regulating TiOx overlayer over Ru/TiO2 nanocatalysts," Nature Communications, Nature, vol. 11(1), pages 1-8, December.
    4. Jiajia Zheng & Sangwon Suh, 2019. "Publisher Correction: Strategies to reduce the global carbon footprint of plastics," Nature Climate Change, Nature, vol. 9(7), pages 567-567, July.
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    Cited by:

    1. Pavel A. Kots & Brandon C. Vance & Caitlin M. Quinn & Cong Wang & Dionisios G. Vlachos, 2023. "A two-stage strategy for upcycling chlorine-contaminated plastic waste," Nature Sustainability, Nature, vol. 6(10), pages 1258-1267, October.

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