IDEAS home Printed from https://ideas.repec.org/a/nat/natcom/v15y2024i1d10.1038_s41467-024-50083-9.html
   My bibliography  Save this article

Unveiling the mechanism of triphos-Ru catalysed C–O bond disconnections in polymers

Author

Listed:
  • Alexander Ahrens

    (Aarhus University)

  • Gabriel Martins Ferreira Batista

    (Aarhus University)

  • Hans Christian D. Hammershøj

    (Aarhus University)

  • Emil Vincent Schwibinger

    (Aarhus University)

  • Ainara Nova

    (University of Oslo)

  • Troels Skrydstrup

    (Aarhus University)

Abstract

Ruthenium complexes with facially coordinating tripodal phosphine ligands are privileged catalysts for a broad range of (de-)hydrogenation-based transformations. Among these, C–O bond hydrogenolysis holds potential for the depolymerisation of both the biopolymer lignin and epoxy resins applied in wind turbine blades, aircrafts and more. However, this methodology is poorly understood in mechanistic terms. Here, we present a detailed investigation on the triphos-Ru catalysed C–O bond scission on a molecular level. A combination of experimental, spectroscopical and theoretical studies elucidates the reactivity of the ruthenium trimethylenemethane precatalyst, revealing the key roles of ruthenium phenolates in both catalyst activation as well as the catalytic cycle itself. Furthermore, a Ru(0)/Ru(II) oxidative addition into the C–O bond is disclosed, with a triphos-Ru(0) dihydrogen complex as entry point. With the molecular nature of the operating triphos-Ru species and the thermodynamics and kinetics of the catalysis unravelled, improvements of established methods as well as design of related transformations may become possible.

Suggested Citation

  • Alexander Ahrens & Gabriel Martins Ferreira Batista & Hans Christian D. Hammershøj & Emil Vincent Schwibinger & Ainara Nova & Troels Skrydstrup, 2024. "Unveiling the mechanism of triphos-Ru catalysed C–O bond disconnections in polymers," Nature Communications, Nature, vol. 15(1), pages 1-10, December.
    • Handle: RePEc:nat:natcom:v:15:y:2024:i:1:d:10.1038_s41467-024-50083-9
    DOI: 10.1038/s41467-024-50083-9
    as

    Download full text from publisher

    File URL: https://www.nature.com/articles/s41467-024-50083-9
    File Function: Abstract
    Download Restriction: no
    File URL: https://libkey.io/10.1038/s41467-024-50083-9?utm_source=ideas
    LibKey link: if access is restricted and if your library uses this service, LibKey will redirect you to where you can use your library subscription to access this item
    ---><---

    References listed on IDEAS

    as
    1. Marvin Bachmann & Christian Zibunas & Jan Hartmann & Victor Tulus & Sangwon Suh & Gonzalo Guillén-Gosálbez & André Bardow, 2023. "Towards circular plastics within planetary boundaries," Nature Sustainability, Nature, vol. 6(5), pages 599-610, May.
    Full references (including those not matched with items on IDEAS)

    Most related items

    These are the items that most often cite the same works as this one and are cited by the same works as this one.
    1. Kai Li & Hauke Ward & Hai Xiang Lin & Arnold Tukker, 2024. "Economic viability requires higher recycling rates for imported plastic waste than expected," Nature Communications, Nature, vol. 15(1), pages 1-9, December.
    2. Meng Jiang & Yuheng Cao & Changgong Liu & Dingjiang Chen & Wenji Zhou & Qian Wen & Hejiang Yu & Jian Jiang & Yucheng Ren & Shanying Hu & Edgar Hertwich & Bing Zhu, 2024. "Tracing fossil-based plastics, chemicals and fertilizers production in China," Nature Communications, Nature, vol. 15(1), pages 1-12, December.
    3. Guilherme Pessoa Nogueira & Gabriel Palma Petrielli & Mateus Ferreira Chagas & Isabelle Lobo de Mesquita Sampaio & Liliana Zanelli de Oliveira Martins & Tassia Lopes Junqueira & Edvaldo Rodrigo Morais, 2024. "Sustainability synergies and trade-offs considering circularity and land availability for bioplastics production in Brazil," Nature Communications, Nature, vol. 15(1), pages 1-13, December.
    4. Lorenz P. Manker & Maxime A. Hedou & Clement Broggi & Marie J. Jones & Kristoffer Kortsen & Kalaiyarasi Puvanenthiran & Yildiz Kupper & Holger Frauenrath & François Marechal & Veronique Michaud & Roge, 2024. "Performance polyamides built on a sustainable carbohydrate core," Nature Sustainability, Nature, vol. 7(5), pages 640-651, May.

    More about this item

    Statistics

    Access and download statistics

    Corrections

    All material on this site has been provided by the respective publishers and authors. You can help correct errors and omissions. When requesting a correction, please mention this item's handle: RePEc:nat:natcom:v:15:y:2024:i:1:d:10.1038_s41467-024-50083-9. See general information about how to correct material in RePEc.

    If you have authored this item and are not yet registered with RePEc, we encourage you to do it here. This allows to link your profile to this item. It also allows you to accept potential citations to this item that we are uncertain about.

    If CitEc recognized a bibliographic reference but did not link an item in RePEc to it, you can help with this form .

    If you know of missing items citing this one, you can help us creating those links by adding the relevant references in the same way as above, for each refering item. If you are a registered author of this item, you may also want to check the "citations" tab in your RePEc Author Service profile, as there may be some citations waiting for confirmation.

    For technical questions regarding this item, or to correct its authors, title, abstract, bibliographic or download information, contact: Sonal Shukla or Springer Nature Abstracting and Indexing (email available below). General contact details of provider: http://www.nature.com .

    Please note that corrections may take a couple of weeks to filter through the various RePEc services.

    IDEAS is a RePEc service. RePEc uses bibliographic data supplied by the respective publishers.