Solid-State Chemical Recycling of Polycarbonates to Epoxides and Carbon Dioxide Using a Heterodinuclear Mg(II)Co(II) Catalyst: Journal of the American Chemical Society

Thomas M. McGuire; Arron C. Deacy; Antoine Buchard; Charlotte K. Williams

doi:10.1021/jacs.2c06937

Solid-State Chemical Recycling of Polycarbonates to Epoxides and Carbon Dioxide Using a Heterodinuclear Mg(II)Co(II) Catalyst: Journal of the American Chemical Society

Thomas M. McGuire, Arron C. Deacy, Antoine Buchard, Charlotte K. Williams

Chemistry

Research output: Contribution to journal › Article › peer-review

Abstract

Polymer chemical recycling to monomers (CRM) could help improve polymer sustainability, but its implementation requires much better understanding of depolymerization catalysis, ensuring high rates and selectivity. Here, a heterodinuclear [Mg(II)Co(II)] catalyst is applied for CRM of aliphatic polycarbonates, including poly(cyclohexene carbonate) (PCHC), to epoxides and carbon dioxide using solid-state conditions, in contrast with many other CRM strategies that rely on high dilution. The depolymerizations are performed in the solid state giving very high activity and selectivity (PCHC, TOF = 25700 h–1, CHO selectivity >99 %, 0.02 mol %, 140 °C). Reactions may also be performed in air without impacting on the rate or selectivity of epoxide formation. The depolymerization can be performed on a 2 g scale to isolate the epoxides in up to 95 % yield with >99 % selectivity. In addition, the catalyst can be re-used four times without compromising its productivity or selectivity.

Original language	English
Pages (from-to)	18444–18449
Journal	Journal of the American Chemical Society
Volume	144
Issue number	40
DOIs	https://doi.org/10.1021/jacs.2c06937
Publication status	Published - 12 Oct 2022

Bibliographical note

The EPSRC ((EP/S018603/1, EP/R027129/1, EP/V003321/1), Oxford Martin School (Future of Plastics), The Royal Society (UF/160021, Fellowship to A.B.), and the UK Catalysis Hub (EP/R027129/1) are acknowledged for research funding. We thank the Material and Chemical Characterization Facility (MC2) at the University of Bath for assistance with TGA-MS experiments.

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10.1021/jacs.2c06937Licence: CC BY

Cite this

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title = "Solid-State Chemical Recycling of Polycarbonates to Epoxides and Carbon Dioxide Using a Heterodinuclear Mg(II)Co(II) Catalyst: Journal of the American Chemical Society",

abstract = "Polymer chemical recycling to monomers (CRM) could help improve polymer sustainability, but its implementation requires much better understanding of depolymerization catalysis, ensuring high rates and selectivity. Here, a heterodinuclear [Mg(II)Co(II)] catalyst is applied for CRM of aliphatic polycarbonates, including poly(cyclohexene carbonate) (PCHC), to epoxides and carbon dioxide using solid-state conditions, in contrast with many other CRM strategies that rely on high dilution. The depolymerizations are performed in the solid state giving very high activity and selectivity (PCHC, TOF = 25700 h–1, CHO selectivity >99 %, 0.02 mol %, 140 °C). Reactions may also be performed in air without impacting on the rate or selectivity of epoxide formation. The depolymerization can be performed on a 2 g scale to isolate the epoxides in up to 95 % yield with >99 % selectivity. In addition, the catalyst can be re-used four times without compromising its productivity or selectivity.",

author = "McGuire, {Thomas M.} and Deacy, {Arron C.} and Antoine Buchard and Williams, {Charlotte K.}",

note = "The EPSRC ((EP/S018603/1, EP/R027129/1, EP/V003321/1), Oxford Martin School (Future of Plastics), The Royal Society (UF/160021, Fellowship to A.B.), and the UK Catalysis Hub (EP/R027129/1) are acknowledged for research funding. We thank the Material and Chemical Characterization Facility (MC2) at the University of Bath for assistance with TGA-MS experiments.",

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Solid-State Chemical Recycling of Polycarbonates to Epoxides and Carbon Dioxide Using a Heterodinuclear Mg(II)Co(II) Catalyst: Journal of the American Chemical Society. / McGuire, Thomas M.; Deacy, Arron C.; Buchard, Antoine et al.
In: Journal of the American Chemical Society, Vol. 144, No. 40, 12.10.2022, p. 18444–18449.

Research output: Contribution to journal › Article › peer-review

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