DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Catalytic Degradation of Polyethylene Terephthalate Using a Phase-Transitional Zirconium-Based Metal–Organic Framework

Journal Article · · Angewandte Chemie (International Edition)
 [1];  [2];  [2];  [2];  [2];  [2];  [2];  [2];  [3];  [2]; ORCiD logo [2]
  1. South China University of Technology (SCUT), Guangzhou (China); Northwestern University, Evanston, IL (United States)
  2. Northwestern University, Evanston, IL (United States)
  3. South China University of Technology (SCUT), Guangzhou (China)

Abstract Polyethylene terephthalate (PET) is utilized as one of the most popular consumer plastics worldwide, but difficulties associated with recycling PET have generated a severe environmental crisis with most PET ending its lifecycle in landfills. We report that zirconium‐based metal–organic framework (Zr‐MOF) UiO‐66 deconstructs waste PET into the building blocks terephthalic acid (TA) and mono‐methyl terephthalate (MMT) within 24 hours at 260 °C (total yield of 98 % under 1 atm H 2 and 81 % under 1 atm Ar). Extensive structural characterization studies reveal that during the degradation process, UiO‐66 undergoes an intriguing transformation into MIL‐140A, which is another Zr‐MOF that shows good catalytic activity toward PET degradation under similar reaction conditions. These results illustrate the diversity of applications for Zr‐MOFs and establish MOFs as a new class of polymer degradation catalysts with the potential to address long‐standing challenges associated with plastic waste.

Research Organization:
Northwestern Univ., Evanston, IL (United States); Univ. of Minnesota, Minneapolis, MN (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF); Ryan Fellowship; Northwestern University International Institute for Nanotechnology; Oversea Study Program of Guangzhou Elite Project; USDOE
Grant/Contract Number:
SC0001329; SC0012702; DMR-1720139; JY201901; ECCS-2025633; DE-SC0001329
OSTI ID:
1976279
Alternate ID(s):
OSTI ID: 1864087
Journal Information:
Angewandte Chemie (International Edition), Vol. 61, Issue 24; ISSN 1433-7851
Publisher:
WileyCopyright Statement
Country of Publication:
United States
Language:
English

References (59)

Production, use, and fate of all plastics ever made journal July 2017
Improving MOF stability: approaches and applications journal January 2019
Thermal stability and flame-retardancy mechanism of poly(ethylene terephthalate)/boehmite nanocomposites journal July 2010
A Low‐Temperature Approach for the Phase‐Pure Synthesis of MIL‐140 Structured Metal–Organic Frameworks journal September 2019
Zr 6 O 8 Node-Catalyzed Butene Hydrogenation and Isomerization in the Metal–Organic Framework NU-1000 journal December 2020
Thermal degradation kinetics and decomposition mechanism of polyesters based on 2,5-furandicarboxylic acid and low molecular weight aliphatic diols journal March 2015
A Series of Isoreticular, Highly Stable, Porous Zirconium Oxide Based Metal-Organic Frameworks journal August 2012
Benign by Design: Green and Scalable Synthesis of Zirconium UiO-Metal–Organic Frameworks by Water-Assisted Mechanochemistry journal October 2018
p K a -Directed Incorporation of Phosphonates into MOF-808 via Ligand Exchange: Stability and Adsorption Properties for Uranium journal August 2019
Enzymatic depolymerization of highly crystalline polyethylene terephthalate enabled in moist-solid reaction mixtures journal July 2021
A review on thermal decomposition and combustion of thermoplastic polyesters journal December 2004
Identification of the strong Brønsted acid site in a metal–organic framework solid acid catalyst journal November 2018
Exchange reactions in metal-organic frameworks: New advances journal October 2020
Thermal degradation of poly(ethylene terephthalate) at the processing temperature journal January 2004
Balancing volumetric and gravimetric uptake in highly porous materials for clean energy journal April 2020
Engineering zirconium-based UiO-66 for effective chemical conversion of d -xylose to lactic acid in aqueous condition journal January 2020
Metal–Organic Frameworks (MOFs) journal January 2014
Low-energy catalytic methanolysis of poly(ethyleneterephthalate) journal January 2021
Metal-Organic Frameworks as Platforms for Catalytic Applications journal November 2017
Introduction to Metal–Organic Frameworks journal September 2011
Pyrolysis of poly(ethylene terephthalate) in a fluidised bed plant journal December 2004
An engineered PET depolymerase to break down and recycle plastic bottles journal April 2020
Biodegradation of PET: Current Status and Application Aspects journal April 2019
Chemical recycling of waste plastics for new materials production journal June 2017
A Series of Isoreticular, Highly Stable, Porous Zirconium Oxide Based Metal-Organic Frameworks journal August 2012
Molecular catalyst systems as key enablers for tailored polyesters and polycarbonate recycling concepts journal August 2018
Enzyme discovery and engineering for sustainable plastic recycling journal January 2022
Variations in capping the Zr6O4(OH)4 cluster core: X-ray structure analyses of [Zr6(OH)4O4(OOC–CHCH2)10]2(μ-OOC–CHCH2)4 and Zr6(OH)4O4(OOCR)12(PrOH) (R=Ph, CMe=CH2) journal January 1999
A bacterium that degrades and assimilates poly(ethylene terephthalate) journal March 2016
Nature of active sites on UiO-66 and beneficial influence of water in the catalysis of Fischer esterification journal August 2017
Catalysis by Metal Organic Frameworks: Perspective and Suggestions for Future Research journal January 2019
Primary thermal degradation mechanisms of PET and PBT journal January 1993
Brønsted Acidity in Metal–Organic Frameworks journal June 2015
Chemolytic depolymerisation of PET: a review journal January 2021
Zirconium-Based Metal–Organic Frameworks for the Catalytic Hydrolysis of Organophosphorus Nerve Agents journal January 2020
Cobalt–molybdenum synergistic catalysis for the hydrogenolysis of terephthalate-based polyesters journal January 2021
Zr-based metal–organic frameworks: design, synthesis, structure, and applications journal January 2016
Instantaneous hydrolysis of PET bottles: an efficient pathway for the chemical recycling of condensation polymers journal January 2021
Highly efficient catalytic transfer hydrogenation of biomass-derived furfural to furfuryl alcohol using UiO-66 without metal catalysts journal July 2020
Selective Chemical Upcycling of Mixed Plastics Guided by a Thermally Stable Organocatalyst journal February 2021
Py-GC/MS analyses of poly(ethylene terephthalate) film without and with the presence of tetramethylammonium acetate reagent. Comparative study journal February 2018
Advances and approaches for chemical recycling of plastic waste journal April 2020
Die nächste Generation des Recyclings – neues Leben für Kunststoffmüll journal June 2020
Upcycling and catalytic degradation of plastic wastes journal August 2021
Chemical, thermal and mechanical stabilities of metal–organic frameworks journal February 2016
Polyethylene Terephthalate Deconstruction Catalyzed by a Carbon‐Supported Single‐Site Molybdenum‐Dioxo Complex journal September 2020
Decomposition of the PET Film by MHETase Using Exo-PETase Function journal February 2020
Insights into the Structure and Dynamics of Metal–Organic Frameworks via Transmission Electron Microscopy journal September 2020
A New Zirconium Inorganic Building Brick Forming Metal Organic Frameworks with Exceptional Stability
  • Cavka, Jasmina Hafizovic; Jakobsen, Søren; Olsbye, Unni
  • Journal of the American Chemical Society, Vol. 130, Issue 42, p. 13850-13851 https://doi.org/10.1021/ja8057953
journal October 2008
Role of Modulators in Controlling the Colloidal Stability and Polydispersity of the UiO-66 Metal–Organic Framework journal April 2017
One-Pot Chemo-bioprocess of PET Depolymerization and Recycling Enabled by a Biocompatible Catalyst, Betaine journal March 2021
Chemical and biological catalysis for plastics recycling and upcycling journal July 2021
Selective Chemical Upcycling of Mixed Plastics Guided by a Thermally Stable Organocatalyst journal February 2021
Beyond Mechanical Recycling: Giving New Life to Plastic Waste journal June 2020
The Chemistry and Applications of Metal-Organic Frameworks journal August 2013
Controlled hydrogenative depolymerization of polyesters and polycarbonates catalyzed by ruthenium(ii) PNN pincer complexes journal January 2014
Possibilities and limitations of biotechnological plastic degradation and recycling journal October 2020
Rational Protein Engineering of Thermo-Stable PETase from Ideonella sakaiensis for Highly Efficient PET Degradation journal March 2019
Polyethylene Terephthalate Deconstruction Catalyzed by a Carbon‐Supported Single‐Site Molybdenum‐Dioxo Complex journal September 2020

Figures / Tables (8)