Ultrasmall amorphous zirconia nanoparticles catalyse polyolefin hydrogenolysis

Shaojiang Chen, Akalanka Tennakoon, Kyung Eun You, Alexander L. Paterson, Ryan Yappert, Selim Alayoglu, Lingzhe Fang, Xun Wu, Tommy Yunpu Zhao, Michelle P. Lapak, Mukunth Saravanan, Ryan A. Hackler, Yi Yu Wang, Long Qi, Massimiliano Delferro, Tao Li, Byeongdu Lee, Baron Peters, Kenneth R. Poeppelmeier, Salai C. AmmalClifford R. Bowers, Frédéric A. Perras, Andreas Heyden, Aaron D. Sadow, Wenyu Huang

Research output: Contribution to journalArticlepeer-review


Carbon–carbon bond cleavage reactions, adapted to deconstruct aliphatic hydrocarbon polymers and recover the intrinsic energy and carbon value in plastic waste, have typically been catalysed by metal nanoparticles or air-sensitive organometallics. Metal oxides that serve as supports for these catalysts are typically considered to be inert. Here we show that Earth-abundant, non-reducible zirconia catalyses the hydrogenolysis of polyolefins with activity rivalling that of precious metal nanoparticles. To harness this unusual reactivity, our catalytic architecture localizes ultrasmall amorphous zirconia nanoparticles between two fused platelets of mesoporous silica. Macromolecules translocate from bulk through radial mesopores to the highly active zirconia particles, where the chains undergo selective hydrogenolytic cleavage into a narrow, C18-centred distribution. Calculations indicated that C–H bond heterolysis across a Zr–O bond of a Zr(O)2 adatom model for unsaturated surface sites gives a zirconium hydrocarbyl, which cleaves a C–C bond via β-alkyl elimination. [Figure not available: see fulltext.].

Original languageEnglish (US)
Pages (from-to)161-173
Number of pages13
JournalNature Catalysis
Issue number2
StatePublished - Feb 2023

ASJC Scopus subject areas

  • Catalysis
  • Bioengineering
  • Biochemistry
  • Process Chemistry and Technology


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