Wu Yufang, Wang Xingjie, Kirlikovali Kent O, Gong Xinyi, Atilgan Ahmet, Ma Kaikai, Schweitzer Neil M, Gianneschi Nathan C, Li Zhong, Zhang Xuan, Farha Omar K
School of Chemistry and Chemical Engineering, South China University of Technology, Guangzhou, Guangdong, 510640, P. R. China.
Department of Chemistry and International Institute for Nanotechnology, Northwestern University, 2145 Sheridan Road, Evanston, IL 60208, USA.
Angew Chem Int Ed Engl. 2022 Jun 13;61(24):e202117528. doi: 10.1002/anie.202117528. Epub 2022 Apr 20.
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 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.
聚对苯二甲酸乙二酯（PET）是全球最常用的消费塑料之一，但PET回收利用存在的困难引发了严重的环境危机，大部分PET最终在垃圾填埋场结束其生命周期。我们报道，锆基金属有机框架（Zr-MOF）UiO-66在260°C下24小时内可将废弃PET分解为对苯二甲酸（TA）和单甲基对苯二甲酸酯（MMT）（在1个大气压氢气下总产率为98%，在1个大气压氩气下为81%）。广泛的结构表征研究表明，在降解过程中，UiO-66会发生有趣的转变，生成MIL-140A，MIL-140A是另一种Zr-MOF，在类似反应条件下对PET降解表现出良好的催化活性。这些结果说明了Zr-MOFs应用的多样性，并确立了金属有机框架作为一类新型聚合物降解催化剂的地位，有望解决与塑料垃圾相关的长期挑战。
