Synthesis of Platinum Nanoparticles on Strontium Titanate Nanocuboids via Surface Organometallic Grafting for the Catalytic Hydrogenolysis of Plastic Waste

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2022-12-12
Authors
McCullough, Katherine E.
Peczak, Ian L.
Kennedy, Robert
Wang, Yi-Yu
Lin, James
Wu, Xun
Paterson, Alexander L.
Perras, Frédéric
Hall, Jacklyn
Kropf, A. Jeremy
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Royal Society of Chemistry
Abstract
Single-use plastics are inexpensive, durable, light, and chemically resistant compounds. Such properties, while desirable for many applications, make them difficult to process after use and have contributed to a global plastic pollution problem. Tackling this problem will require establishing a circular economy based on catalytic technologies that can chemically convert (i.e. upcycle) waste plastics into value-added products. Although many promising technologies exist, there is an urgent need to scale them up and remove obstacles to their commercialization if they are to move the needle on plastics pollution. To that effect, this work details a scalable synthesis for Pt/STO made by surface organometallic chemistry (SOMC) techniques using either trimethyl(methylcyclopentadienyl)platinum(IV) (Cp*PtMe3) or Pt(II)acetylacetonate (Pt(acac)2). The STO support was calcined (550 oC), treated with ozone (200 oC), and finally steamed (200 oC) to afford a clean STO surface populated with only hydroxyl groups. Pt precursors were dissolved in toluene and deposited onto STO. Pt(acac)2 was found to produce higher Pt loading on the STO surface than CP*PtMe3 and was chosen for further optimization. After reduction at 300 oC, the STO support was decorated with 1.3 – 1.5 nm Pt nanoparticles. The size and loading of these nanoparticles were varied by employing a multi-cycle deposition and oxidation and/or reduction process similar to atomic layer deposition techniques. These Pt/STO catalysts hydrogenolyzed isotactic polypropylene into liquid products (> 95% yield) with average molecular weights of 200 – 300 Da (~25 carbon atoms) and narrow size distributions at 300 oC and 180 psi H2. Negligible differences in product Mn and polydispersity were observed even when the Pt/STO catalyst was reused for up to 5 consecutive runs. The results demonstrate that Pt/STO hydrogenolysis catalysts could be promising, industrially viable solutions for waste plastic upcycling.
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This is a manuscript of an article published as McCullough, Katherine, Ian L. Peczak, Robert Maxwell Kennedy, Yi-Yu Wang, Frédéric A. Perras, Jacklyn Hall, A. Jeremy Kropf et al. "Synthesis of Platinum Nanoparticles on Strontium Titanate Nanocuboids via Surface Organometallic Grafting for the Catalytic Hydrogenolysis of Plastic Waste." Journal of Materials Chemistry A (2022). DOI: 10.1039/D2TA08133D. Copyright 2022 The Royal Society of Chemistry. Posted with permission.
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