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Mixed polyester recycling can enable a circular plastic economy with environmental benefits

The mixed and varied nature of fossil-based and bio-based plastic waste requires complex and costly separations to enable compatibility with recycling technologies. A circular plastic economy based on mixed polyesters through cleaving ester bonds to produce monomers, while re-utilizing bio-based monomers to produce high-quality sustainable plastics, charts an exciting solution. However, the feasibility of such a circular economy solution remains underexplored. Here, in this study, we conducted a techno-economic analysis and life-cycle assessment of three polyester depolymerization recycling processes-methanolysis, glycolysis, and acid hydrolysis-for a mixed feedstock (polyethylene terephthalate [PET], polylactic acid [PLA], and polybutylene adipate terephthalate [PBAT]). Methanolysis outperforms glycolysis and hydrolysis economically and environmentally due to more efficient downstream separations, generating products with a 31% decrease in selling price and 21%-46% reduction in acidification, carcinogenic toxicity, fossil-fuel depletion, global warming potential, particulate formation, and smog formation compared to conventional polyester manufacturing. This study highlights the viability of a circular plastic economy for mixed polyesters via a single chemical recycling process.

09 BIOMASS FUELS

Optimal Design of Food Packaging Considering Waste Management Technologies to Achieve Circular Economy

Plastic packaging plays a fundamental role in the food industry, avoiding food waste and facilitating food access. The increasing plastic production and the lack of appropriate plastic waste management technologies represent a threat to the environmental and human welfare. Therefore, there is an urgent need to identify sustainable packaging solutions. Circular economy (CE) promotes reducing waste and increasing recycling practices to achieve sustainability. In this work, we propose a CE framework based on multi-objective optimization, considering both economic and environmental impacts, to identify optimal packaging designs and waste management technologies. Using mixed-integer linear programming (MILP), techno-economic analysis (TEA), and life cycle assessment (LCA), this work aims to build the first steps in packaging design, informing about the best packaging alternatives and the optimal technology or technologies to process packaging waste. For the economic analysis, we consider the minimum increase in price (MIP) when adding recycling to the cost of each packaging solution, while for the environmental analysis, the greenhouse gas emissions impact was considered. A case study on ground coffee packaging is used to illustrate the proposed framework. The results demonstrate that the multilayer bag option is the most convenient when considering both the chosen economic and environmental impacts.

Life Cycle Analysis

Analyses of circular solutions for advanced plastics waste recycling

A circular plastics economy can leverage the lightweight, strong and durable characteristics of macromolecular materials, while simultaneously reducing the negative environmental impacts associated with polymer waste. Advanced recycling technologies provide an opportunity to valorize plastics waste and extend the lifespan of these materials by converting waste into new monomers, polymers or specialty chemicals. Although many advanced technologies appear promising, assessments of economic and environmental sustainability are often not conducted in a standardized fashion and neglect factors such as plastics waste transportation, sorting and pretreatment. These shortcomings can lead to inaccurate or misleading predictions, reduce opportunities for optimization and limit industrial relevance. In this Review, we highlight select industrial case studies to underscore the notable consequences of underestimating the complexity of real-life consumer plastics waste. In addition, the current challenges associated with the assessment of the industrial viability of laboratory-scale processes are explored. Here, by discussing relevant analysis frameworks and system boundaries, along with potential analytical pitfalls, future research will be guided beyond chemical considerations and toward impactful circular solutions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH

Production of bio-based lactones as monomers for a circular polymer economy

To create a circular plastics economy, new polymers are being developed that can be chemically recycled. Circular polyesters are of particular interest and to this end, lactones are ideal monomers. Here, this Review examines catalytic routes to convert diols, hydroxy acids, and dicarboxylic acids to lactones, focusing on the development of scalable, atom-economic, and energy-efficient conversions of bio-derived feedstocks. Free energy analysis is used to inform process choices, such as reactor type, reaction phase, and use of solvent. Catalyst design principles are summarized for both direct (bio-substrate to lactone) and indirect (bio-substrate to intermediate to lactone) routes. Finally, we summarize literature that shows that many lactone precursors are readily accessible from various metabolic and chemo-catalytic pathways. Transitioning to bio-based monomers offers an opportunity to reduce reliance on fossil carbon resources, but requires advanced catalytic processes informed by mechanistic insights.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH

Ecologically inspired metrics for transitioning to a sustainable and resilient circular economy with application to multilayer plastic films

Current Circular Economy (CE) frameworks applied to product chains exhibit notable shortcomings. These include neglecting the resilience and robustness of design, requiring detailed economic and environmental data for impact assessment, and relying on qualitative rather than quantitative metrics capturing certain CE design aspects. In the current contribution, we addressed these shortcomings by developing an Ecologically inspired (Eco-inspired) Framework using the mathematical foundations of Ecological Network Analysis (ENA). While ENA metrics have previously found application in designing circular economies, particularly in Industrial Symbiosis (IS) networks, our adaptation tailors these metrics for use in product-level CE, recognizing the inherent distinctions between product-level CE and IS. Our Eco-inspired Framework comprises three key categories to provide holistic and granular-level metrics for designing product-level CE. The first set of metrics assesses circularity and resource efficiency. The second set gauges network intensity and robustness as complementary indicators ensuring a CE is both sustainable and resilient. The third group of metrics evaluates enhancement potential of CE strategies through introducing quantitative metrics for measuring the degree of closed-loop strategies and average circularity level of a CE design. The three comprehensive set of indicators within the Eco-inspired Framework uniquely captures various facets of circular design, whether originating from technological innovations and recovery improvement at the end of life (EoL), shifts in human consumption patterns, alterations in product design, or changes in business models. The framework’s application is tested in designing a CE for multilayer Polyethylene-Polyamide (PE-PA) films. Using the Eco-inspired Framework, we identified the best strategy for designing a resilient and sustainable CE for PE-PA films. A diverse set of EoL strategies along with a reduction in product consumption can improve circularity and resilience by 650% and 255%, respectively, and mitigate greenhouse gas emissions by 90%. The framework minimizes trade-offs between sustainability and circularity goals and offers insights on how to enhance each strategy for achieving a resilient and sustainable CE for products.

54 ENVIRONMENTAL SCIENCES

Catalytic Upgrading of Pyrolysis Condensables from Postconsumer Polyolefins Using HZSM-5

The conversion of plastic wastes to monomeric olefins is an attractive means for achieving a plastic circular economy. In our study, a fluidized bed reactor converts post-consumer waste high-density polyethylene (HDPE) and polypropylene (PP) to mostly condensed pyrolysis waxes and some oils, preventing carbon loss to gases. The pyrolysis condensables were upgraded to light olefins (C 2 –C 5 ) at carbon yields greater than 76 wt % using the HZSM-5 zeolite catalyst at a post pyrolysis process that employed a micropyrolyzer. These results were comparable to olefin monomer yields from direct ex situ catalytic pyrolysis of the original waste plastics without condensing the vapors, highlighting the potential applicability of this approach in plastic waste recycling. Our results suggest that a centralized catalytic upgrading facility fed by pyrolysis condensables sourced from distributed thermochemical processing plants is a promising pathway to a circular economy. Such an approach enables utilization of available catalytic cracking infrastructure while focusing on setting up distributed thermochemical processing plants close to material recovery facilities. As a result, the energy-dense pyrolysis waxes are more suitable for transportation, contributing to the overall scalability and economic viability of the proposed distributed approach.

10 SYNTHETIC FUELS

Solventless, Ambient-Pressure Production of Bio-Based Lactones Over Earth-Abundant, Mixed Metal Oxide Catalysts for Circular Polyesters

Transitioning to a circular plastics economy will require use of renewable feedstocks, energy-efficient processes, and closed-loop recyclable polymers, such as polyesters. A key challenge lies in sustainably sourcing monomers used to make recyclable polyesters. This work presents a catalytic platform utilizing earth-abundant Cu(x)Ca(1-x)O mixed metal oxides for the oxidative dehydrocyclization of bio-based diols to lactones, which are advantaged for energy-efficient ring-opening polymerization. Operating below 200 degrees C, at ambient pressure, and without solvent, the process uses air as the sole oxidant, achieving high yields of lactones across a broad substrate scope of C4-8 diols in the liquid phase. The oxidative dehydrocyclization reaction is thermodynamically downhill due to water formation and energy-efficient compared to incumbent, non-redox pathways utilized in fossil carbon-based industrial processes for lactone production. Mechanistic studies reveal facile redox cycling of Cu2+-O(Ca2+)-Cu2+ interfacial sites unique to the developed catalyst. Techno-economic analysis and life cycle assessment estimate 40% lower energy demand and 15% lower GHG intensity per mass of butyrolactone produced compared to the fossil carbon-based route. Liquid-phase oxidative dehydrocyclization offers a promising approach for scalable lactone production from renewable, bio-based diols to enable circular polyesters.

36 MATERIALS SCIENCE

Polymer Deconstruction and Redesign Strategies for Plastics Recycling

Advancing plastics recycling requires both the selective deconstruction of existing polymers and the design of new materials that enable efficient reuse without loss of performance. This perspective highlights an integrated approach that is rooted in polymer chemistry, catalysis, and process engineering which can enable a circular plastics economy. Here, we outline recent advances in catalytic, solvolytic, and enzymatic pathways for plastic deconstruction, and examine the molecular design principles driving next-generation recyclable-by-design and bio-based polymers. Despite these advances, major knowledge gaps remain in understanding the evolution of polymer morphology and catalyst structure during deconstruction, assessing deconstruction processes with realistic polymers, and offering redesigned polymers with competitive cost and environmental advantage over conventional plastics. United States Department of Energy (U.S. DOE) national laboratories offer unique capabilities to address these challenges through in situ and operando characterization, high-throughput experimentation, environmental studies, technoeconomic and life cycle assessment, scale-up support, and collaboration networks. Advances made in understanding plastic deconstruction mechanisms and structure-property correlations of redesigned polymers inform emerging research directions including autonomous experimentation, real-time feedback-enabled process optimization, and protein engineering for enzymatic depolymerization.

36 MATERIALS SCIENCE

How should reproducibility be approached in plastic recycling?

With the growing importance of developing new and improved methodologies for plastic recycling, conducting reproducible research and ensuring that results are transferable across labs are increasingly important. This Voices article reflects on how academia and industry view the path forward for strengthening reproducibility to advance science and enable a circular plastics economy.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH

Universal Approach for the Depolymerization of Polyamides via Photothermal Conversion

Polyamides (PAs) exhibit excellent chemical stability and mechanical resistance, yet these same characteristics lead to their widespread accumulation in the environment as pollution. In this work, we developed an inclusive and operationally simple photothermal strategy to recycle PAs, overcoming the high energy barriers necessary to break down these materials. PAs can be depolymerized using photothermally mediated ring-closing depolymerization and acidic hydrolysis to afford cyclic and linear monomers using carbon black as a photothermal agent (PTA) under visible light irradiation. We showed that polyamide 6 is efficiently depolymerized to ε-caprolactam with 74% yield in 10 min. Similarly, in 1 h, the photothermal acidic hydrolysis of polyamide 6,6 afforded hexamethylene diamine and adipic acid with 97 and 96% yields, respectively. This method was further applied to a variety of aliphatic and aromatic PAs and mixed PA waste. Both photothermally promoted processes effectively depolymerize pigment-containing postconsumer waste by leveraging existing black pigments as PTAs. Here, photothermal conversion provided a general and rapid route for PA depolymerization under visible light irradiation, enabling high monomer yields with inexpensive reagents and a general tolerance to additives, demonstrating this approach’s potential for a circular plastic economy.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH

Recent advances in chemical recycling and upcycling of plastic waste into valuable materials, chemicals, and energy: a comprehensive review

The global plastic waste crisis has increased in severity in recent years: annual plastic production is projected to reach 500 million metric tons by 2025, and plastic waste accumulation is expected to surpass 12 billion metric tons. Despite these growing volumes, only ∼9% of plastic waste is currently recycled; the majority is either landfilled, incinerated, or mismanaged, contributing to escalating greenhouse gas emissions—from 1.7 Gt carbon dioxide equivalent (CO 2 -eq.) in 2015 to an estimated 6.5 Gt CO 2 -eq. by 2050—and physical environmental pollution. This review provides a comprehensive overview of advanced plastic upcycling strategies to address this issue and recover value from diverse plastic waste streams. Recent developments in solvent-based dissolution, chemical depolymerization, and thermochemical conversions are examined for major plastic types, including polyolefins, polycondensation polymers, and PVC. Underlying reaction pathways, catalyst designs, and processing parameters that govern product selectivity, efficiency, and conversion yields are discussed in depth. Emerging techniques such as microwave-assisted depolymerization, tandem catalysis, and co-processing approaches are highlighted for their potential to enhance efficiency under milder conditions. Emphasis is also placed on the production of high-value products such as monomers, naphtha-range hydrocarbons, and syngas, and discussion is provided on catalyst stability, contaminant removal, scalability, life cycle effects on the environment, and technoeconomic viability. Finally, the review outlines future research directions focused on catalyst innovation, integrated process design, supportive policy frameworks, and interdisciplinary collaboration. All recommendations are aimed at accelerating large-scale implementation of plastic upcycling technologies and advancing the global circular plastics economy.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH

Scaling the polymerization of polyaldehydes through continuous flow synthesis

Abstract A plug flow reactor was constructed to scale the synthesis of metastable, phthalaldehyde-based polymers to achieve production rates of 1–2 kg per day. The flow-induced mixing and in-line polymerization quench and precipitation sequences resulted in improved polymer purity and long-term stability compared to the same materials made from a conventional batch process. Cryogenic rheology was used to probe the complex fluid dynamics encountered during the polymerization of PPA homopolymers. It is envisioned that this continuous flow manufacturing approach could be extended to other low ceiling temperature or aldehyde monomer systems to help implement and support a plastic circular economy. Graphical abstract

Schwartz, Jared M.

Toward a sustainable circular economy of multilayer plastic films: Life cycle and techno-economic assessment with a focus on end-of-life treatment and multiple recovery cycles

This study presents a life cycle assessment (LCA) and techno-economic analysis (TEA) of end-of-life technologies for treating polyethylene–polyamide barrier film waste, focusing on quality degradation across recovery cycles. Novel treatment methods are experimentally validated, while others are drawn from literature and industry consultations. A displacement approach, assuming no quality loss, is first applied. Results show that solvent-based recycling via the solvent-targeted recovery and precipitation (STRAP) process outperforms alternatives across environmental indicators, reducing global warming potential (GWP) by 40% compared to landfilling. Incineration performs worst in most categories, particularly eutrophication (80% higher than landfilling), due to nitrogen emissions. Experimentally validated downcycling (pelletizing) proves more economically viable. The assumption of infinite recoverability is overly optimistic. To address this, we propose a mathematical framework accounting for a finite number of recovery cycles. This refined model shows reduced GWP and cost savings for solvent recovery, making its benefits less pronounced than initially estimated. Sensitivity and uncertainty analyses reveal strong dependence on recovered material quality and solvent recovery efficiency, underscoring the need for optimized process design. Finally, hotspot analysis identifies greenhouse gas emissions from the polyamide supply chain as the dominant GWP contributor. In conclusion, the results underscore potential trade-offs across pathways and show that solvent-based recovery’s sustainability depends heavily on process conditions.

36 MATERIALS SCIENCE

Thermal Oxo-degradation and Catalytic Upgrading of Plastic Waste to Light Olefins for a Circular Economy

The commercialization of conventional pyrolysis of plastic in an inert atmosphere has been hindered by large thermal requirements stemming from long reaction rates. The rate of thermal depolymerization of waste plastics can be accelerated by the addition of oxygen in a process known as thermal oxo-degradation (TOD). This study offers the prospect of TOD to upcycle postconsumer waste rapidly and efficiently. Using moderate temperatures and small amounts of air in a fluidized bed reactor, we demonstrated that waste high-density polyethylene and polypropylene are rapidly deconstructed to condensable products. These condensable products were catalytically upgraded in a micropyrolysis reactor using commercially available zeolite (HZSM-5) to monomeric olefins. The olefin yields proved to be greater than those achieved through the catalytic upgrading of condensable products from (nonoxidative) the pyrolysis of the same plastic wastes. The coupling of TOD with catalytic upgrading proves to be an energy-efficient pathway in a plastics circular economy for the production of light olefins from wastes.

Enthalpy

Minimum GHG emissions and energy consumption of U.S. PET and polyolefin packaging supply chains in a circular economy

There is a wide agreement on the urgency of transforming linear management of plastics towards a circular economy model. However, no clear pathways exist as to required recycling technologies involved and system-wide environmental impacts. This study explores such pathways in the U.S. for the most commonly used packaging plastics through a combination of mechanical and emerging advanced recycling technologies. A system optimization model aimed at minimizing environmental impacts was developed to determine optimal end-of-life (EOL) management and locations of existing and emerging U.S. recycling infrastructures. Our study includes material flows from virgin resin production through semi-manufacturing processes to existing EOL disposal and recycling processes. An optimized circular plastics packaging system achieved greenhouse gas (GHG) emission savings of up to 28% and cumulative energy demand (CED) savings of up to 46%, compared to the linear economy. Moreover, these savings of GHG emissions and CED impacts represent a reduction of 0.16% and 0.49% compared to annual U.S. GHG emissions and energy consumption in 2022, respectively. The optimal recycling rates and systems-level circularity ranged from 78–99% and 57–75%, respectively. Increased energy savings led to increased GHG emissions showing a potential trade-off between GHG emissions and energy. Analysis of 40 scenarios showed the importance of material collection distances, blend limit of mechanically recycled resins, process yields, and mandated recycling rates for achieving a sustainable circular economy of plastics.

09 - BIOMASS FUELS

Systems Analysis and Optimization of Circular PET Packaging Supply Chains in the United States: Environmental and Socioeconomic Impacts

Many actions are underway at global, national, and local levels to address the plastic waste problem and transition toward a circular economy of plastics. Studies evaluating environmental and socioeconomic impacts of such a transition are lacking. Here, the purpose of this study is to conduct a national systems analysis of polyethylene terephthalate (PET) packaging supply chains in the United States. Material flow data was combined with environmental and socioeconomic indicators to evaluate and compare the sustainability of the linear PET packaging supply chain, current (2019) supply chain, and possible future circular supply chain options in the United States. Environmentally optimal circular US PET packaging material flows showed 31% and 38% savings of GHG emissions and energy demand, respectively, with a circularity of 77% when compared with a linear supply chain. Additionally, the environmentally optimal system showed higher employment (29%) and wages (31%) than a linear system, but with a 5% decrease in revenue generation. A socioeconomically optimal circular PET supply chain showed increased employment (by 52%), wages (by 67%), and revenues (by 1%), with a circularity of 59% when compared with the linear system. However, it showed 14% higher GHG emissions than a linear system, indicating a trade-off between environmentally and socioeconomically optimal circular PET packaging systems. Overall, linear-to-circular material flow transition may not necessarily lead to increased revenues and decreased environmental impacts of the entire system, but it does benefit society due to increased employment and wages. Future systems analysis work should focus on improving data quality for environmental and socioeconomic dimensions.

PET

Recycling Disassembled Automotive Plastic Components for New Vehicle Components: Enabling the Automotive Circular Economy

As the automotive industry increasingly relies on plastic components to meet fuel efficiency and emissions targets, the challenge of managing end-of-life vehicle (ELV) plastics continues to grow. Currently, more than 80% of ELV plastics in the U.S. are landfilled due to limited economic incentives and technical barriers to recycling. This study examines a mechanical recycling pathway for thermoplastic components disassembled from ELVs and assesses their usability for reintegration into new vehicle parts. Four representative materials were chosen based on material labels embedded in recovered parts and aligned with their virgin industrial equivalents: polypropylene (PP), 10% talc-filled PP (PP-T10), 20% talc-filled PP (PP-T20), and a 20% glass-/mineral-filled polyamide (PA6 + GF7 + MF13). The materials underwent shredding, drying, and injection molding before being characterized by particle size analysis, density measurement, thermal analysis (TGA, DSC), mechanical testing, and heat deflection temperature (HDT) evaluation. The results in this work indicated that minor differences in crystallinity were observed and small differences between model materials and ELV materials could have contributed to these changes. Mechanical testing revealed that neat polypropylene suffered a 15–20% reduction in stiffness and tensile strength, but talc-filled polypropylene and glass/mineral-filled nylon retained >90% of their modulus, strength, and heat deflection temperature values relative to virgin controls. Differences between virgin and ELV materials could have been attributed to use life degradation, contamination during use life, or even chemical/processing differences in model materials and ELV materials. However, these findings suggest that mechanically recycled, disassembled ELV plastics can retain sufficient structural performance to support circularity efforts in the automotive sector.

automotive recycling

Assessment of Different Application Grades of Post-Consumer Recycled (PCR) Polyolefins from Material Recovery Facilities (MRFs) in the United States

The recycling of plastics has been gaining traction in the following years as many companies, organizations, and governments are pushing toward a more circular economy. However, plastic recycling rates are still small compared to those of plastic production, especially for polyolefins, such as high-density polyethylene (HDPE) and polypropylene (PP). With the goal of finding applications for recycled plastic resin, recyclers can face some challenges associated with the heterogeneity in the polymer properties of plastic waste streams, which could hinder the full potential of recycling due to the lack of a consistent feedstock. Here, this study assessed how an additional sorting step of recycled HDPE and PP streams, separating them into two categories based on the previous application, impacts the recycled polymer properties, such as physical, molecular, and thermal. It was demonstrated that manually separating HDPE articles previously processed by extrusion blow molding (EBM) or injection molding (IM) and PP articles by thermoforming (TF) or IM could yield recycled resins with more consistent properties, considering the significant differences between them. This highlights that an additional sorting step would allow recyclers to target more premium or currently unattainable plastic processing applications with postconsumer recycled (PCR) resins, which could significantly promote an increase in plastic recycling rates. Nevertheless, the development of new technologies is needed to automate this extra sorting step, as with the increase in scale manual sortation could not be feasible and cost-effective, reducing the attractiveness of using PCR resins in comparison to virgin ones.

36 MATERIALS SCIENCE