Ultrasmall amorphous zirconia nanoparticles catalyse polyolefin hydrogenolysis

61Citations
Citations of this article
86Readers
Mendeley users who have this article in their library.

This article is free to access.

Abstract

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.].

Cite

CITATION STYLE

APA

Chen, S., Tennakoon, A., You, K. E., Paterson, A. L., Yappert, R., Alayoglu, S., … Huang, W. (2023). Ultrasmall amorphous zirconia nanoparticles catalyse polyolefin hydrogenolysis. Nature Catalysis, 6(2), 161–173. https://doi.org/10.1038/s41929-023-00910-x

Register to see more suggestions

Mendeley helps you to discover research relevant for your work.

Already have an account?

Save time finding and organizing research with Mendeley

Sign up for free