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 H2 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.
Original language | English (US) |
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Article number | e202117528 |
Journal | Angewandte Chemie - International Edition |
Volume | 61 |
Issue number | 24 |
DOIs | |
State | Published - Jun 13 2022 |
Funding
O.K.F. acknowledges support from the Inorganometallic Catalyst Design Center, an EFRC funded by the DOE, Office of Basic Energy Sciences (DE‐SC0012702). O.K.F. and N.C.G. gratefully acknowledge support from National Science Foundation's MRSEC program (grant number NSF DMR‐1720139). X.G. is supported by the Ryan Fellowship and the Northwestern University International Institute for Nanotechnology. K.O.K. gratefully acknowledges support from the IIN Postdoctoral Fellowship and the Northwestern University International Institute for Nanotechnology. Y.W. gratefully acknowledges support from the Oversea Study Program of Guangzhou Elite Project during her visit to Northwestern University (JY201901). This work made use of the IMSERC facility at Northwestern University, which has received support from the Soft and Hybrid Nanotechnology Experimental (SHyNE) Resource (NSF ECCS‐2025633), and Northwestern University. This work made use of the EPIC facility of Northwestern University's NUANCE Center, which has received support from the Soft and Hybrid Nanotechnology Experimental (SHyNE) Resource (NSF ECCS‐2025633), the International Institute for Nanotechnology (IIN) and the Northwestern's MRSEC program (NSF DMR‐1720139). The REACT Core facility acknowledges funding from the U.S. Department of Energy, Catalysis Science program (DE‐SC0001329). The authors thank Dr. Timur Islamoglu and Dr. Massimiliano Delferro for helpful discussions.
Keywords
- Metal–Organic Frameworks
- PET Degradation
- Phase Transitions
- Plastic Recycling
ASJC Scopus subject areas
- Catalysis
- General Chemistry