Polyethylene terephthalate (PET) is the most widespread synthetic polyester, having been utilized in textile fibers and packaging materials for beverages and food, contributing considerably to the global solid waste stream and environmental plastic pollution. While enzymatic PET recycling and upcycling have recently emerged as viable disposal methods for a circular plastic economy, only a handful of benchmark enzymes have been thoroughly described and subjected to protein engineering for improved properties over the last 16 years. By analyzing the specific material properties of PET and the reaction mechanisms in the context of interfacial biocatalysis, this Perspective identifies several limitations in current enzymatic PET degradation approaches. Unbalanced enzyme-substrate interactions, limited thermostability, and low catalytic efficiency at elevated reaction temperatures, and inhibition caused by oligomeric degradation intermediates still hamper industrial applications that require high catalytic efficiency. To overcome these limitations, successful protein engineering studies using innovative experimental and computational approaches have been published extensively in recent years in this thriving research field and are summarized and discussed in detail here. The acquired knowledge and experience will be applied in the near future to address plastic waste contributed by other mass-produced polymer types (e.g., polyamides and polyurethanes) that should also be properly disposed by biotechnological approaches.

Institute of Biochemistry Department of Biotechnology and Enzyme Catalysis University of Greifswald Felix Hausdorff Str 4 D 17487 Greifswald Germany

International Clinical Research Center St Anne's University Hospital and Faculty of Medicine Masaryk University 656 91 Brno Czech Republic

Loschmidt Laboratories Department of Experimental Biology and RECETOX Faculty of Science Masaryk University 625 00 Brno Czech Republic

Macromolecular Crystallography Helmholtz Zentrum Berlin für Materialien und Energie Albert Einstein Straße 15 D 12489 Berlin Germany

Tianjin Institute of Industrial Biotechnology Chinese Academy of Sciences 32 West 7th Avenue Tianjin Airport Economic Area Tianjin 300308 China

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Structural Insights into (Tere)phthalate-Ester Hydrolysis by a Carboxylesterase and Its Role in Promoting PET Depolymerization

Multiple Substrate Binding Mode-Guided Engineering of a Thermophilic PET Hydrolase