Polyethylene terephthalate (PET) pollution has significant environmental consequences; thus, new degradation methods must be explored to mitigate this problem. We previously demonstrated that a consortium of three Pseudomonas and two Bacillus species can synergistically degrade PET in culture. The consortium more readily consumes bis(2-hydroxyethyl) terephthalate (BHET), a byproduct created in PET depolymerization, compared to PET, and can fully convert BHET into metabolically usable monomers, namely terephthalic acid (TPA) and ethylene glycol (EG). Because of its crystalline structure, the main limitation of the biodegradation of post-consumer PET is the initial transesterification from PET to BHET, depicting the need for a transesterification step in the degradation process. Additionally, there have been numerous studies done on the depolymerization reaction of PET to BHET, yet few have tested the biocompatibility of this product with a bacterial consortium. In this work, a two-step process is implemented for sustainable PET biodegradation, where PET is first depolymerized to form BHET using an orange peel ash (OPA)-catalyzed glycolysis reaction, followed by the complete degradation of the BHET glycolysis product by the bacterial consortium. Results show that OPA-catalyzed glycolysis reactions can fully depolymerize PET, with an average BHET yield of 92% (w/w), and that the reaction product is biocompatible with the bacterial consortium. After inoculation with the consortium, 19% degradation of the glycolysis product was observed in 2 weeks, for a total degradation percentage of 17% when taking both steps into account. Furthermore, the 10-week total BHET degradation rate was 35%, demonstrating that the glycolysis products are biocompatible with the consortium for longer periods of time, for a total two-step degradation rate of 33% over 10 weeks. While we predict that complete degradation is achievable using this method, further experimentation with the consortium can allow for a circular recycling process, where TPA can be recovered from culture media and reused to create new materials. 
                        more » 
                        « less   
                    
                            
                            Envisioning a BHET Economy: Adding Value to PET Waste
                        
                    
    
            Poly(ethylene terephthalate), the fifth most produced polymer, generates significant waste annually. This increased waste production has spurred interest in chemical and mechanical pathways for recycling. The shift from laboratory settings to larger-scale implementation creates opportunities to explore the value and recovery of recycling products. Derived from the glycolysis of PET, bis(2-hydroxyethyl) terephthalate (BHET) exhibits versatility as a depolymerization product and valuable monomer. BHET exhibits versatility and finds application across diverse industries such as resins, coatings, foams, and tissue scaffolds. Incorporating BHET, which is a chemical recycling product, supports higher recycling rates and contributes to a more sustainable approach to generating materials. This review illuminates the opportunities for BHET as a valuable feedstock for a more circular polymer materials economy. 
        more » 
        « less   
        
    
                            - Award ID(s):
- 2132183
- PAR ID:
- 10539008
- Publisher / Repository:
- ACS
- Date Published:
- Journal Name:
- Sustainable Chemistry
- Volume:
- 4
- Issue:
- 4
- ISSN:
- 2673-4079
- Page Range / eLocation ID:
- 363 to 393
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
More Like this
- 
            
- 
            The consumption of synthetic polymers has ballooned; so has the amount of post-consumer waste generated. The current polymer economy, however, is largely linear with most of the post-consumer waste being either landfilled or incinerated. The lack of recycling, together with the sizable carbon footprint of the polymer industry, has led to major negative environmental impacts. Over the past few years, chemical recycling technologies have gained significant traction as a possible technological route to tackle these challenges. In this regard, olefin metathesis, with its versatility and ease of operation, has emerged as an attractive tool. Here, we discuss the developments in olefin-metathesis-based chemical recycling technologies, including the development of new materials and the application of olefin metathesis to the recycling of commercial materials. We delve into structure–reactivity relationships in the context of polymerization–depolymerization behavior, how experimental conditions influence deconstruction outcomes, and the reaction pathways underlying these approaches. We also look at the current hurdles in adopting these technologies and relevant future directions for the field.more » « less
- 
            Abstract The accumulation of plastic waste, due to lack of recycling, has led to serious environmental pollution. Although mechanical recycling can alleviate this issue, it inevitably reduces the molecular weight and weakens the mechanical properties of materials and is not suitable for mixed materials. Chemical recycling, on the other hand, breaks the polymer into monomers or small‐molecule constituents, allowing for the preparation of materials of quality comparable to that of the virgin polymers and can be applied to mixed materials. Mechanochemical degradation and recycling leverages the advantages of mechanical techniques, such as scalability and efficient energy use, to achieve chemical recycling. We summarize recent progress in mechanochemical degradation and recycling of synthetic polymers, including both commercial polymers and those designed for more efficient mechanochemical degradation. We also point out the limitations of mechanochemical degradation and present our perspectives on how the challenges can be mitigated for a circular polymer economy.more » « less
- 
            Ionic liquids (ILs) are a promising medium to assist in the advanced (chemical and biological) recycling of polymers, owing to their tunable catalytic activity, tailorable chemical functionality, low vapor pressures, and thermal stability. These unique physicochemical properties, combined with ILs’ capacity to solubilize plastics waste and biopolymers, offer routes to deconstruct polymers at reduced temperatures (and lower energy inputs) versus conventional bulk and solvent-based methods, while also minimizing unwanted side reactions. In this Viewpoint, we discuss the use of ILs as catalysts and mediators in advanced recycling, with an emphasis on chemical recycling, by examining the interplay between IL chemistry and deconstruction thermodynamics, deconstruction kinetics, IL recovery, and product recovery. We also consider several potential environmental benefits and concerns associated with employing ILs for advanced recycling over bulk- or solvent-mediated deconstruction techniques, such as reduced chemical escape by volatilization, decreased energy demands, toxicity, and environmental persistence. By analyzing IL-mediated polymer deconstruction across a breadth of macromolecular systems, we identify recent innovations, current challenges, and future opportunities in IL application toward circular polymer economies.more » « less
- 
            The global utilization of single-use, non-biodegradable plastics, such as bottles made of polyethylene terephthalate (PET), has contributed to catastrophic levels of plastic pollution. Fortu- nately, microbial communities are adapting to assimilate plastic waste. Previously, our work showed a full consortium of five bacteria capable of synergistically degrading PET. Using omics approaches, we identified the key genes implicated in PET degradation within the consortium’s pangenome and transcriptome. This analysis led to the discovery of a novel PETase, EstB, which has been observed to hydrolyze the oligomer BHET and the polymer PET. Besides the genes implicated in PET degradation, many other biodegradation genes were discovered. Over 200 plastic and plasticizer degradation-related genes were discovered through the Plastic Microbial Biodegradation Database (PMBD). Diverse carbon source utilization was observed by a microbial community-based assay, which, paired with an abundant number of plastic- and plasticizer-degrading enzymes, indicates a promising possibility for mixed plastic degradation. Using RNAseq differential analysis, several genes were predicted to be involved in PET degradation, including aldehyde dehydrogenases and several classes of hydrolases. Active transcription of PET monomer metabolism was also observed, including the generation of polyhydroxyalkanoate (PHA)/polyhydroxybutyrate (PHB) biopolymers. These results present an exciting opportunity for the bio-recycling of mixed plastic waste with upcycling potential.more » « less
 An official website of the United States government
An official website of the United States government 
				
			 
					 
					
 
                                    