Polyethylene Terephthalate Deconstruction Catalyzed by a Carbon-Supported Single-Site Molybdenum-Dioxo Complex

Yosi Kratish, Jiaqi Li, Shanfu Liu, Yanshan Gao*, Tobin J. Marks*

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

153 Scopus citations

Abstract

Polyethylene terephthalate (PET) is selectively depolymerized by a carbon-supported single-site molybdenum-dioxo catalyst to terephthalic acid (PTA) and ethylene. The solventless reactions are most efficient under 1 atmosphere of H2. The catalyst exhibits high stability and can be recycled multiple times without loss of activity. Waste beverage bottle PET or a PET + polypropylene (PP) mixture (simulating the bottle + cap) proceeds at 260 °C with complete PET deconstruction and quantitative PTA isolation. Mechanistic studies with a model diester, 1,2-ethanediol dibenzoate, suggest the reaction proceeds by initial retro-hydroalkoxylation/β-C−O scission and subsequent hydrogenolysis of the vinyl benzoate intermediate.

Original languageEnglish (US)
Pages (from-to)19857-19861
Number of pages5
JournalAngewandte Chemie - International Edition
Volume59
Issue number45
DOIs
StatePublished - Nov 2 2020

Funding

Financial support from the Office of Basic Energy Sciences, Department of Energy (DE-FG02-03ER15457) to the Institute for Catalysis in Energy Processes (ICEP) at Northwestern University (Y.K., J.L.) is gratefully acknowledged. Purchase of the NMR instrumentation at IMSERC was supported by NSF (CHE-1048773). We thank Katia Kratish for expert graphics design. Financial support from the Office of Basic Energy Sciences, Department of Energy (DE‐FG02‐03ER15457) to the Institute for Catalysis in Energy Processes (ICEP) at Northwestern University (Y.K., J.L.) is gratefully acknowledged. Purchase of the NMR instrumentation at IMSERC was supported by NSF (CHE‐1048773). We thank Katia Kratish for expert graphics design.

Keywords

  • heterogenous catalysis
  • hydrogenolysis
  • molybdenum
  • polymers
  • reaction mechanisms

ASJC Scopus subject areas

  • Catalysis
  • General Chemistry

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