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At least 19 records
All sourcesNASA NTRSDOE OSTI
DOE OSTI2025

Recent advances in enzyme engineering for improved deconstruction of poly(ethylene terephthalate) (PET) plastics

In the last ~20 years, a multitude of natural enzymes have been discovered that can catalyze the breakdown of the common plastic poly(ethylene terephthalate) (PET). While enzymatic PET recycling is an attractive alternative end-of-life route for this waste plastic, the enzymes are not yet optimized for efficient and economical industrial use. Here, we discuss recent advances in engineering these PET-degrading enzymes, which include PET, bis(2-hydroxyethyl) terephthalate (BHET), and 2-hydroxyethyl terephthalic acid (MHET) hydrolases, toward industrially-relevant engineering goals. We place emphasis on trends from past efforts in rational and semi-rational design and emerging areas in directed evolution/high throughput screening and computational design for engineering these enzymes.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2026

Multilevel Analysis of Electrochemically Mediated Methanolysis of Poly(ethylene terephthalate) (PET)

Here, this study presents a multilevel analysis of electrochemically mediated methanolysis as a promising method for reducing the environmental impacts of plastic recycling, with a focus on depolymerizing poly(ethylene terephthalate) (PET) into dimethyl terephthalate (DMT). Instead of conventional chemical PET depolymerization, this electrochemical approach provides distinct technical advantages in process control and efficiency. At the process level, key operational parameters, including applied current and reaction time, were systematically investigated to optimize PET conversion and DMT selectivity. The electrochemical approach was directly compared to equivalent chemical methanolysis systems and demonstrated superior performance in terms of PET conversion and DMT selectivity. Building on these findings, a technoeconomic assessment identified the current economic bottlenecks and revealed that improvements in process design, DMT selectivity, PET conversion, and energy efficiency are key to reducing the overall process cost and enabling future implementation. While further optimization is required for market competitiveness, these results establish a performance baseline for the electrochemically mediated PET methanolysis process and underscore the importance of combining process-level innovation with systems-level evaluation in the development of sustainable recycling technologies.

chemical recycling↗
DOE OSTI2023

Dihydroxyterephthalate—A Trojan Horse PET Counit for Facile Chemical Recycling

Abstract Here, low‐energy poly(ethylene terephthalate) (PET) chemical recycling in water: PET copolymers with diethyl 2,5‐dihydroxyterephthalate (DHTE) undergo selective hydrolysis at DHTE sites, autocatalyzed by neighboring group participation, is demonstrated. Liberated oligomeric subchains further hydrolyze until only small molecules remain. Poly(ethylene terephthalate‐ stat ‐2,5‐dihydroxyterephthalate) copolymers were synthesized via melt polycondensation and then hydrolyzed in 150–200 °C water with 0–1 wt% ZnCl 2 , or alternatively in simulated sea water. Degradation progress follows pseudo‐first order kinetics. With increasing DHTE loading, the rate constant increases monotonically while the thermal activation barrier decreases. The depolymerization products are ethylene glycol, terephthalic acid, 2,5‐dihydroxyterephthalic acid, and bis(2‐hydroxyethyl) terephthalate dimer, which could be used to regenerate virgin polymer. Composition‐optimized copolymers show a decrease of nearly 50% in the Arrhenius activation energy, suggesting a 6‐order reduction in depolymerization time under ambient conditions compared to that of PET homopolymer. This study provides new insight to the design of polymers for end‐of‐life while maintaining key properties like service temperature and mechanical properties. Moreover, this chemical recycling procedure is more environmentally friendly compared to traditional approaches since water is the only needed material, which is green, sustainable, and cheap.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Engineering PHL7 for Improved Poly(Ethylene Terephthalate) Depolymerization via Rational Design and Directed Evolution

Enzymatic depolymerization of poly(ethylene terephthalate) (PET) has emerged as a promising approach for polyester recycling, and, to date, many natural and engineered PET hydrolase enzymes have been reported. For industrial use, PET hydrolases must achieve high depolymerization extent and exhibit excellent thermostability. Here, we engineered a natural PET hydrolase, Polyester Hydrolase Leipzig #7 (PHL7), through rational design and directed evolution using a high-throughput screening platform. Four new enzymes were engineered with enhanced properties compared with the parent enzyme, wild-type PHL7 (PHL7-WT), and other benchmark PET hydrolases, under the tested conditions. In bioreactors, the exemplary engineered enzyme, PHL7-Jemez, exhibited improved ability to depolymerize amorphous PET film compared with PHL7-WT at 2.9% and 20% substrate loadings, with 37% and 270% higher hydrolysis, respectively, after 48 h. This study develops several state-of-the-art PET hydrolases and demonstrates a directed evolution platform to engineer high-performance enzymes, which can accelerate enzyme discovery toward improved biocatalytic recycling.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2026

Engineering and Application of a Thermostable MHETase for PET Depolymerization

Enzymatic hydrolysis of poly(ethylene terephthalate) (PET) releases mono(2-hydroxyethyl) terephthalate (MHET) as a major product, the accumulation of which can prolong reactor residence times and complicate downstream monomer separations. The use of a MHETase enzyme can enable MHET hydrolysis to the monomers, terephthalic acid and ethylene glycol, but industrial PETases typically operate at thermophilic temperatures and the well-known MHETase from Ideonella sakaiensis is a mesophilic enzyme, thus warranting the development of thermophilic MHETases. Here, we characterize thermostable MHET-active enzymes from a natural diversity screen by applying a hidden Markov model based on the previously reported, archaeal ferulic acid esterase, PET46. We identified enzymes with higher thermostability than PET46 and quantified their MHETase activity in reactions at 70 °C. The crystal structure of MHT077, the homologue with the highest MHETase activity and an apparent melting temperature (T m,app ) of 94.6 °C, informed site saturation mutagenesis in the active site and lid-domain interface. MHT077 exhibited a ∼100-fold slower unfolding rate at 65 °C than PET46, indicating substantially greater kinetic stability. In parallel, we applied evolution-informed design, a probabilistic model that leverages coevolutionary patterns in large multiple sequence alignments, to improve the activity and thermostability of five ferulic acid esterases. One design, EV-MHT043–5 was identified with a comparable thermostability (T m,app = 96.1 °C) and a 3-fold improvement in its MHETase activity relative to the wildtype enzyme, MHT043. Combination variants of beneficial mutations were screened and afforded a variant, MHT077 LFK , which reduced MHET accumulation in bioreactor experiments with postconsumer PET waste. Overall, this study expands the known MHET-hydrolyzing protein scaffolds available for enzymatic PET recycling.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Chapter 4: Chemical Recycling of PET

The circular economy of poly(ethylene terephthalate) (PET) today is dominated by collection, sorting, cleaning, melting, and re-processing of transparent bottles via mechanical recycling. This has a better environmental impact as assessed by Life Cycle Assessment (LCA) (e.g. uses less non-renewable energy and produces less greenhouse gases) than production of virgin resin and is the preferred method of recycling wherever possible. However, not all PET products can be recycled this way and there is forecast to be a large shortfall between supply of high quality recycled PET (rPET) and the demands of large users who have made commitments to use more recycled resin over the next 5 - 10 years. Consequently, there is renewed interest, and increased activity, in chemical recycling, where waste PET is depolymerized, and the monomer(s) are purified and repolymerized into resin equivalent to that from petroleum-derived raw materials. The LCA is likely to be not as favorable as traditional mechanical recycling, but will likely be better than virgin PET and the process can be applied to a broader range of lower value wastes and thus promises to dramatically increase the overall recycling rate. In this chapter we will review the processes used in chemical recycling of PET, with the VolCat process from IBM as a detailed case study, followed by descriptions of the alternative technologies and emerging players in the field.

chemical recycling↗
DOE OSTI2025

Protocol for engineering poly(ethylene terephthalate) hydrolases via directed evolution using a high-throughput screening assay

Poly(ethylene terephthalate) (PET) hydrolases, which depolymerize PET to its monomers, have gained attention for their potential to facilitate bio-industrial recycling of this waste plastic. Here, we present a protocol for screening large, random mutagenesis enzyme libraries simultaneously for enhanced activity, solubility, and stability. We outline steps for library construction, screening using plate-based split GFP and model substrate assays, and determination of enzyme thermostability. We then detail procedures for validation assays on PET substrates and characterization of final variants.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2026

Upcycling waste PET into functional multiblock copolymers through controlled macromolecular design

Poly(ethylene terephthalate) (PET) oligomers derived from glycolysis depolymerization were converted into multiblock copolymers through diisocyanate-mediated coupling with dihydroxy-terminated oligomers, enabling precise control over copolymer sequence distribution, connectivity, and mechanical performance. Here, we demonstrate that telechelic PET oligomers isolated directly from depolymerized consumer waste can serve as reactive building blocks for the formation of segmented multiblock copolymers, eliminating the need to revert to monomeric feedstocks. Dihydroxy-terminated PET oligomers (Mw ≈ 8 kg mol−1) were coupled with poly(ethylene oxide) (PEO, Mw ≈ 4 kg mol−1) to form PET-PEO multiblock copolymers with high molar mass (Mw ≈ 160 kg mol−1). We further show that the timing of end-capping reactions provides a key control parameter that governs the competition between chain extension and termination, thereby dictating the resulting multiblock architecture and molecular-weight evolution. Evaluation of their mechanical properties reveals that virgin PET exhibits high modulus (∼3 GPa) and strength (43 MPa) but limited ductility (<10% elongation). In contrast, PET–PEO multiblock copolymers retain comparable tensile strength (44 MPa), albeit while exhibiting dramatically enhanced ductility (>90% elongation), forming tougher materials with efficient stress transfer between the rigid PET domains and the flexible PEO segments. When incorporated into PET/PEO blends at low loadings, the multiblock copolymers serve as effective compatibilizers, yielding materials with an intermediate modulus (1.1–1.2 GPa) and improved elongation compared to uncompatibilized blends. Furthermore, the presence of PEO blocks increases water uptake and gas permeability relative to virgin PET, reflecting the tunability of molecular transport through the copolymeric blocks. To our knowledge, this represents the first report of PET–PEO multiblock copolymers derived from post-consumer PET for gas transport applications. These results demonstrate that multiblock copolymer formation from telechelic PET oligomers provides a versatile platform for tailoring the mechanical and transport behavior of polyester-based materials through controlled macromolecular design and establishes a generalizable strategy for transforming consumer plastic waste into functional segmented polymers without requiring complete depolymerization to monomers.

Watson-Sanders, Shelby [Department of Chemistry, U↗
DOE OSTI2025

Machine Learning-Guided Identification of PET Hydrolases from Natural Diversity

The enzymatic depolymerization of poly(ethylene terephthalate) (PET) is emerging as a leading chemical recycling technology for waste polyester. As part of this endeavor, new candidate enzymes identified from natural diversity can serve as useful starting points for enzyme evolution and engineering. In this study, we improved upon HMM searches by applying an iterative machine learning strategy to identify 400 putative PET-degrading enzymes (PET hydrolases) from naturally occurring homologs. Using high-throughput (HTP) experimental techniques, we successfully expressed and purified >200 enzyme candidates and assayed them for PET hydrolysis activity as a function of pH, temperature, and substrate crystallinity. From this library, we discovered 91 previously unknown PET hydrolases, 35 of which retain activity at pH 4.5 on crystalline material, which are conditions relevant to developing more efficient commercial processes. Notably, four enzymes showed equal to or higher activity than LCC-ICCG, a benchmark PET hydrolase, at this challenging condition in our screening assay, and 11 of which have pH optima <7. Using these data, we identified regions of PETases statistically correlated to activity at lower pH. We additionally investigated the effect of condition-specific activity data on trained machine learning predictors and found a precision (putative hit rate) improvement of up to 30% compared to a Hidden Markov Model alone. Our findings show that by pointing enzyme discovery toward conditions of interest with multiple rounds of experimental and machine learning, we can discover large sets of active enzymes and explore factors associated with activity at those conditions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Photostability of Ambient-Processed, Conjugated Polymer Electrochromic Devices Encapsulated by Bioderived Barrier Films

Polymer-based electrochromic devices (ECDs) are a promising technology for enabling low-voltage, disposable displays, yet are currently limited by photo-oxidative bleaching of the active materials. Here, renewable barrier films composed of cellulose and chitin are presented as an alternative to poly(ethylene terephthalate) (PET) for encapsulating ECDs. To assess barrier film effectiveness, lateral ECDs composed of poly(3,4-propylenedioxythiophene-(CH 2 OEtHx) 2 ) (P(ProDOT)) active layers were constructed and encapsulated with a multilayer barrier consisting of chitin nanofibers and cellulose nanocrystals spray cast onto a cellulose acetate substrate (oxygen transmission rate (OTR) = 29 cm 3 m –2 day –1 ), a commercially available PET film (OTR = 8.5 cm 3 m –2 day –1 ), and a high-performance PET-Al 2 O 3 multilayer barrier film (OTR < 1 cm 3 m –2 day –1 ). The photodegradation of the P(ProDOT) active layer was determined by measuring the evolution of the colorimetric contrast (ΔE*) and switching speeds as a function of light exposure (100 mW cm –2 , AM 1.5 G light). Photodegradation was found to proceed at a similar rate for all encapsulated devices (roughly 10 times more slowly than unencapsulated devices), highlighting the opportunity for replacing petroleum packaging with bioderived barrier films. Analysis of the switching kinetics, the shifts in optical absorbance, and evidence of chemical degradation indicate that both photochemical breakdown of the electrolyte and cross-linking of the P(ProDOT) active material are key drivers for loss of device performance when oxygen flux to the active material is limited. Furthermore, pathways toward better understanding photodegradation are then proposed with sustainability in mind for future ECD design.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Biochemical and structural characterization of an aromatic ring–hydroxylating dioxygenase for terephthalic acid catabolism

Significance More than 400 million tons of plastic waste is produced each year, the overwhelming majority of which ends up in landfills. Bioconversion strategies aimed at plastics have emerged as important components of enabling a circular economy for synthetic plastics, especially those that exhibit chemically similar linkages to those found in nature, such as polyesters. The enzyme system described in this work is essential for mineralization of the xenobiotic components of poly(ethylene terephthalate) (PET) in the biosphere. Our description of its structure and substrate preferences lays the groundwork for in vivo or ex vivo engineering of this system for PET upcycling.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2025

Closed‐Loop Recyclable Vitrimer Plastics from PET Waste: A Design for Circularity

Plastics are essential to modern society, but their low recycling rates and inefficient end-of-life management pose a significant environmental challenge. Herein, the efficient strategy for upcycling postconsumer poly(ethylene terephthalate) (PET) waste into robust, closed-loop recyclable vitrimer plastics and composites is presented to address this issue. The catalyst-free aminolysis utilizes readily available amines to deconstruct diverse PET wastes into macromonomers, which are upcycled into vitrimers, exhibiting superior mechanical properties and exceeding the ultimate tensile stress and Young's Modulus of virgin PET by 80% and 150% respectively. These vitrimers exhibit excellent healability, shape memory, thermal reprocessability, and closed-loop chemical recyclability, enabling quantitative macromonomer recovery even from mixed plastic waste streams and glass/carbon fiber reinforced vitrimer (G/CFRV) composites. Furthermore, the vitrimer resin yields robust GFRV and CFRV composites with tensile strengths exceeding those of traditional epoxy composites by 100% and 80%, respectively, while maintaining complete chemical recyclability of both constituent materials. A preliminary technoeconomic analysis confirms the costeffectiveness and competitiveness of the facile PET deconstruction approach, which is potentially adaptable to other condensation polymers. Further, this study presents a facile approach to upcycling plastic waste into circular plastics and composites, offering a sustainable solution to global plastic waste management and fostering a circular economy.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2025

High-performance reversible adhesive from PET waste for underwater, structural, and pressure-sensitive applications

Developing versatile, tough, and sustainable adhesives that function effectively in both wet and dry environments is a major challenge. Here, we report a bioinspired design for versatile, tough, and reversible adhesives upcycled from consumer poly(ethylene terephthalate) (PET) waste. Our approach uses solvent-free, room-temperature dynamic cross-linking of deconstructed PET macromonomers with a diacetoacetate cross-linker, generating a dynamic, vinylogous urethane–bonded, amphiphilic adhesive. Tunable cross-linker concentration and amphiphilicity yield versatile adhesives suitable for underwater, structural, and pressure-sensitive applications on diverse substrates. Our adhesive exhibits high lap-shear strength and work of debonding under both wet and dry conditions, outperforming common commercial adhesives. The dynamic bonds enable thermal repair, on-demand multicycle debonding/rebonding, facile removal, and chemical recycling. Our strategy of transforming plastic waste into versatile, tough, and reversible adhesives offers a sustainable solution for both plastic waste management and next-generation adhesive design while also providing a commercially viable pathway for valorizing plastic waste.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

In‐Situ Product Removal for the Enzymatic Depolymerization of Poly(ethylene terephthalate) via a Membrane Reactor

Poly(ethylene terephthalate) (PET) is a common single-use plastic and a major contributor to plastic waste. PET upcycling through enzymatic depolymerization has drawn significant interests, but lack of robust enzymes in acidic environments remains a challenge. This study investigates in-situ product removal (ISPR) of protons and monomers from enzymatic PET depolymerization via a membrane reactor, focusing on the ICCG variant of leaf branch compost cutinase. More than two-fold improvements in overall PET depolymerization and terephthalic acid yields were achieved employing ISPR for an initial PET loading of 10 mgPET ml buffer −1 . The benefit of ISPR was reduced for a lower initial loading of 1 mgPET ml buffer −1 due to decreased need for pH stabilization of the enzyme-containing solutions. A back-of-envelop analysis suggests that at a modest dilution ratio, ISPR could help achieve savings on caustic base solutions used for pH control in a bioreactor. Our study provides valuable insights for future ISPR developments for enzymatic PET depolymerization, addressing the pressing need for more sustainable solutions towards plastic recycling and environmental conservation.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

A Multi-Streamline Approach for Upcycling PET into a Biodiesel and Asphalt Modifier

The non-degradable nature of petroleum-based plastics and the dependence on petroleum-based products in daily life and production are dilemmas of human development today. We hereby developed a plastic waste upcycling process to address these challenges. A multi-stream fraction strategy was developed to process poly (ethylene terephthalate) (PET) plastics into soluble and insoluble fractions. The soluble fraction was used as a sole carbon source for microbial fermentation to produce biodiesel precursor lipids with an appreciable bioconversion yield. The insoluble fraction containing fractionated polymers was used as the asphalt binder modifiers. The downsized PET additive improved the high-temperature performance of the asphalt binder by 1 performance grade (PG) without decreasing the low-temperature PG. Subsequent SEM imaging unveiled alterations in the micromorphology induced by PET incorporation. Further FTIR and 1 H NMR analysis highlighted the aromatic groups of PET polymers as a crucial factor influencing performance enhancement. The results demonstrated the multi-stream fraction as a promising approach for repurposing plastic waste to produce biodiesel and modify asphalt. Finally, this approach holds the potential to tackle challenges in fuel supply and enhance infrastructure resilience to global warming.

09 BIOMASS FUELS↗
DOE OSTI2026

Selective Sequential Depolymerization of Mixed Plastics Mediated by Photothermal Conversion

Chemical recycling of plastics into monomers is a promising strategy to achieve a circular economy. However, selective depolymerization methods for mixed plastics are still underdeveloped. Herein, we report a selective and sequential depolymerization strategy for mixed plastics, including poly(L-lactide) (PLLA), polystyrene (PS), and poly(ethylene terephthalate) (PET), using photothermal conversion. We were able to selectively depolymerize PLLA into L-lactide in the presence of PS and PET. Then, PS was selectively depolymerized to styrene, followed by the depolymerization of PET into its monomer. Our protocol was carried out in one pot without any additional purification of the unreacted plastics at each stage. This method was successfully applied to mixtures of post-consumer waste plastic.

carbon black↗