Authors
Francesco CaraceniFrancesco ArfelliR. SansiAndrea BallarinoCarlo BrondiDaniele CespiDebnarayan Jana
Topics
Polymer crystallization and propertiesToxic Organic Pollutants ImpactMicroplastics and Plastic PollutionThis article is licensed under CC-BY 4.0| pubs.acs.org/journal/ascecg Environmental Alkaline F. | Research Article Impacts of PET Chemical Recycling: A Case Study on Hydrolysis and Systemic Evaluation ∥ ∥ Caraceni, F. Arfelli, R. Sansi, A. Ballarino, C. D. and F. Passarini Brondi,* Cespi,* Cite This: ACS Sustainable Chem. Eng. 2026, 14, 4499−4509 Read Online || --- | --- || ACCESS | *sı Metrics & More Article Recommendations Supporting Information |ABSTRACT: Polyethylene terephthalate (PET) is one of thee l c imost widely used polymers, but its durability and versatilityt r agenerate significant end-of-life challenges. While mechanicald e hrecycling remains the predominant option, its limitations in qualitys i l bloss and ability to treat complex waste streams highlight the need u .p ) for complementary solutions. Chemical recycling offers theC e r T a (Upotential to regenerate virgin-quality PET and handle wasteh s yfractions not suitable for mechanical routes, yet its environmental4 e : 7 aperformance is still to be fully explored. This study presents 5 im :2 tcomprehensive insights into an innovative chemical recycling process for PET, consisting in microwave-assisted alkaline6 o 2 thydrolysis. An attributional Life Cycle Assessment (LCA) was0 w 2 o ,conducted to quantify the environmental impacts associated with the innovative system and to provide a comparison with virgin and1 nbiobased PET. Scenario analysis investigates the replacement of the fossil fraction of the electricity mix with renewable energy. An analysis of the complementarity between chemical and mechanical recycling in the European market has been carried out to implement a systemic approach. Results highlight substantial reductions in greenhouse gas emissions when renewable energy isp o 1 .6 radopted, but also show trade-offs in biobased PET scenarios. The combined use of chemical and mechanical recycling emerges as7 f 8 sessential to maximize circularity while minimizing environmental burdens, underscoring the need for systemic, multitechnology.1 e n 1 i .9strategies in PET waste management.l e 9 d 6 i uKEYWORDS: life cycle assessment, plastic recycling, chemical recycling, waste management strategies, systemic thinking, environmental sustainability, circularity evaluation waste has been incinerated or landfilled, underscoring the urgent need for sustainable alternatives. 13In this context, Life Cycle Assessment (LCA) has become ap / / :crucial methodology within circular economy (CE) stratp t t hegies. 14−16 LCA systematically assess environmental impactse ethroughout a product’s lifecycle, from raw material extraction to disposal, allowing the identification of environmental hotspots. 17,18 Meanwhile, CE strategies aim to establish a closed-loop system emphasizing resource reuse and waste minimization. 19,20 As chemical industries account for about 10% of global energy demand and 7% of GHG emissions, integrating LCA into CE is vital to meet long-term sustainability objectives. 21 Notable approaches include the use of biopolymers and the application of eco-design principlesReceived: November 6, 2025Revised: February 18, 2026Accepted: February 19, 2026Published: February 24, 2026■ INTRODUCTION Plastic materials are crucial in modern society, being widely used across sectors such as packaging, healthcare, construction, and electronics. 1,2 Their durability, adaptability, and cost efficiency have made them critical, enhancing daily life by improving both convenience and efficiency. 3,4 For example, plastic packaging extends the shelf life of perishable food, while single-use medical devices ensure sterility in clinical settings. 5−7 As a result, global polymer production has grown quickly, highlighting the central role of plastic material in economic development. In 2021, the EU plastics industry generated approximately 405 billion euros and employed over 1.5 million workers. 8 However, these same properties, durability and versatility, pose substantial environmental concerns. 9 Growing demand has led to an increase in single-use plastic products, generating a considerable amount of waste and pollution. 10,11 Production is projected to increase from 260 million tons in 2016 to an estimated 460 million tons by 2030, intensifying resource depletion and waste management challenges. 12 Despite the mitigation efforts, only around 9% of all produced plastics have been recycled; throughout its history, the majority of plastic© 2026 The Authors. Published by American Chemical Society https://doi.org/10.1021/acssuschemeng.5c12048 ACS Sustainable Chem. Eng. 2026, 14, 4499−4509 to increase product durability, recyclability, and resource efficiency. 22 On the policy front, the European Commission has introduced legislation requiring a minimum recycled content in plastic products by 2025 and 2030, seeking to reduce dependence on virgin plastics and support sustainability targets. 23,24 Polyethylene terephthalate (PET) represents plastics’ role as both essential materials and environmental burdens. PET’s high strength, low weight, and chemical resistance make it ideal for packaging and textiles, yet these same properties hinder its postdisposal degradation. 25,26 As such, effective recycling technologies are essential for sustainable PET management. Currently, Mechanical recycling is the most established approach, involving cleaning, shredding, and remelting PET waste into new products. 27 Although both energy and cost efficient, it degrades polymer quality, reducing molecular weight, and results in downcycling. Additionally, mechanical recycling struggles with complex plastic structures, such as multilayered PET. At the same time, PET textiles are frequently excluded or downcycled into inferior materials, discarded after a single recycling cycle. 28 Conversely, chemical recycling depolymerises PET into its monomers, terephthalic acid (TPA) and monoethylene glycol (MEG), using methods such as glycolysis, methanolysis, or hydrolysis. This yields PET of virgin-equivalent quality, suitable for all applications, including food packaging. Chemical recycling can also process contaminated and complex waste streams, or PET textiles, that mechanical methods cannot efficiently handle. 27 Consequently, chemical recycling offers a promising pathway to close the PET loop, reducing the reliance on virgin feedstocks, and enhancing PET circularity and sustainability. Nonetheless, chemical recycling presents notable environmental drawbacks. 29,30 While it enhances material circularity and reduces dependence on virgin inputs, due to higher complexity of the processes involved may bring to an increase of the environmental impact associated with the involved flows (i.e., materials and energy). This discussion underscores the need to define an appropriate methodological framework for the assessment of environ mental impacts associated with plastic recycling. For instance, mechanical and chemical recycling yield products with varying characteristics and quality levels. 31 These differences should be properly accounted for in environmental evaluations. Fur thermore, performing a comprehensive comparison requires detailed knowledge of the recycling process inventories. In this regard, chemical recycling remains relatively underdiscussed in the scientific literature and the availability and detail of inventory data could be further improved to enable more robust life cycle assessments. 32 The present work addresses this research gap by offering a valuable reference benchmark for the environmental impact assessment that may enrich the literature discussion. Concerning the already available comparative analyses, it was found that chemical recycling often underperforms relative to mechanical recycling in environmental metrics. Shen et al., for instance, evaluated four bottle-to-fiber (B2F) recycling routes, mechanical, semimechanical, back-to-oligomer (glycolysis), and back-to monomer (methanolysis), against virgin PET (v-PET) fiber. 30 Their findings revealed that mechanical and semimechanical processes had lower environmental impacts than glycolysis based recycling. Similarly, Helmes et al. reported that glycolysis-recycled PET shampoo bottles had higher impacts in areas such as climate change and resource depletion compared to mechanically recycled counterparts. 29 Notably, both studies focused on a single-cycle assessment, isolating each technology and overlooking the broader aim of reducing virgin material use. 33 This broader aim is analyzed by both Komly et al. and Stegmann et al., who pointed out the necessity of adopting a systems-based perspective that evaluates technologies within the full recycling ecosystem. 34,35 Rather than identifying one superior method, a balanced approach that integrates sustainability with circularity is more pragmatic. By combining mechanical recycling, suited for clean, homogeneous waste, with chemical recycling, capable of handling contaminated and complex streams like textiles, it is possible to optimize both material recovery and environmental outcomes. Addressing PET waste requires a holistic, system-oriented strategy that aligns complementary recycling methods with long-term environmental and circularity targets. 36 While such integrated system assessments are beginning to emerge in the U.S., they remain comparatively scarce in the European context. 37,38 In this domain, Ghosh et al. applied a material flow model integrating consequential life cycle assessment, techno-economic analysis, and a plastic circularity indicator to evaluate U.S. PET bottle end-of-life pathways, identifying an optimal configuration that minimizes GHG emissions and costs while maximizing circularity. 37 Similarly, Chaudhari et al. formulated a mixed-integer optimization model for the U.S. PET and polyolefin packaging that integrates recycling technologies with geospatially resolved collection and processing infrastructure, showing that appro priately configured systems can substantially reduce green house gas emissions and increase recycling rates relative to a linear baseline. 38 This study aims to provide detailed insights into chemical recycling of PET via a life cycle assessment (LCA) of an innovative process developed by the Swiss startup GR3N during the Horizon 2020 Project DEMETO (grant agreement no. 768573) and improved into the Microwave Assisted DEpolymerization (MADE) process. 39,40 The process utilizes microwave-assisted alkaline hydrolysis, enabling the recycling of diverse PET waste streams. LCA is employed to perform scenario analyses, identifying how addressing key environ mental hotspots alters the impact profile. In the base case, the depolymerization is carried out at 180−200 °C and 5−7 bar, without the use of any catalyst, achieving a conversion yield of 95% on the net PET content of the feedstock. On this basis, and accounting for all upstream losses (sorting, pretreatment, depolymerization and repolymerization), approximately 1.1 kg of pretreated PET feed (or 1.17 kg of sorted PET waste) are required per kilogram of recycled PET resin obtained from the overall chemical recycling process. It is worth noting that the process yield is not affected by polymer crystallinity or by the presence of contaminants. Lastly, the study investigates the potential synergy between mechanical and chemical recycling, highlighting their comple mentary capabilities in treating different PET wastes.■ METHODOLOGY This analysis assesses the environmental impacts of multiple PET recycling scenarios using an attributional LCA approach. Each technology and scenario is evaluated based on its specific contributions within a defined system boundary. Given PET’s varied applications and the cradle-to-gate scope of this study, a declared unit of 1 kg of recycled PET produced was adopted, rather than a functional unit, which would entail extending the system to include a new product use and end-of life stages. The LCA was performed using SimaPro (v10.2), applying the ReCiPe 2016 Midpoint (H) V1.11 method for Life Cycle Impact Assessment (LCIA), covering 18 environ mental categories. 41,42 In addition, the results were also calculated in terms of cumulative energy demand (version 1.12). Cases of multifunctionality were handled via system expansion; alternatively, physical allocation was applied where flow contributions could be reliably distributed among output products. Specifically, mass-based allocation was applied in the depolymerization stage to distribute the environmental burdens between MEG and TPA. The Baseline Scenario, depicted in Figure 1, serves as the baseline for further scenario modifications. System boundaries extend from the end-of-life stage of PET waste (cradle) to the production of new granulates (gate), focusing on reintegrating the recovered materials into the new production cycles. Specifically, these boundaries include the collection of PET waste, sorting of plastic, the chemical recycling process (as implemented by the MADE technology) and the polymerization of recycled granules. The chemical recycling process consists of the pretreatment and cleaning of PET waste, followed by alkaline hydrolysis, where PET is depolymerised into MEG and TPA using a solution of NaOH, MEG and other reactants produced through brine electrolysis. The monomers are subsequently purified by MEG distillation and TPA crystallization, then repolymerised into PET granules. Primary data were obtained from GR3N’s DEMETO pilot plant in Chieti, Italy, which processes 60 kg of PET scrap per hour, and scaled up with the GR3N engineering team to better represent the MADE process. Developed under the EU Horizon 2020 program, the facility demonstrates an innovative and sustainable PET and polyester chemical recycling process. Although primary data were used, their disclosure is restricted for confidentiality reasons (indicated in Supporting Informa tion Tables S1−S6 in the form of NDV = non-disclosable value). All remaining background data were modeled using the ecoinvent database (v3.11). 43 Concerning the input waste, authors decided to associate primary information to the proxies available in ecoinvent: 37.5% waste textiles, 37.5% waste plastic mixture to market, and 25% waste plastic mixture to incineration. Monte Carlo simulation with 100 runs was carried out with the SimaPro software, with a confidence interval of 95%, to determine how the intrinsic variability of the parameters and the quality of the data used in the model may affect the outcomes. The number of runs was selected by referring to literature. 44,45 The results of the Monte Carlo simulations have been reported in Tables S23−S28. Scenario Analysis The MADE recycling process has been compared with currently available processes aimed at producing PET of the same quality from fossil (i.e., Virgin PET) and biobased sources (i.e., Biobased PET). Then, a sensitivity analysis was conducted by assuming the replacement of the European electricity mix with a totally renewable mix and partially replacing the heat source, shifting from a scenario employing 100% natural gas to one employing 50% natural gas and 50% biomethane. Accordingly, the renewable energy scenario modifies the baseline recycling system to align with the EU’s 2050 carbon neutrality targets, focusing on the integration of renewable energy. 29 Concerning the electricity flow, the original process relies on the European grid. In this scenario, projected for 2050, electricity inputs were updated to reflect a 100% renewable electricity mix, which has been modeled by removing the fossil fraction from the mix and proportionally redistributing the renewable share. renewable energy mix used is reported in Table S11. The 50% of biomethane, instead, is predicted to derive from a dedicated plant located in proximity to the production system. Such a configuration, in line with GR3N projections, allows for the production of biomethane in situ, which can be used to directly feed the recycling plant. To generate the model for biomethane production, an ecoinvent proxy representing a real-case scenario was used (Biomethane, high pressure {CH}| biogas purification to biomethane by membrane technique | cut-off, U). This proxy was used to replace natural gas in heat, central or small-scale, biomethane {CH}| heat production, natural gas, at boiler condensing modulating < 100 kW | cutFigure 1. Flowsheet of the baseline scenario. It includes collection and sorting of PET waste, the chemical recycling process (according with MADE) and the polymerization of recycled PET granules.off, U. Emissions different from CO2 and fugitive CH4 have been removed from the inventory by assuming a high purity of the biomethane. The environmental impacts of biomethane production strongly depend on the feedstock (e.g., biogas or syngas), which may originate from waste, dedicated crops, or other organic streams. Depending on the treatment applied, these feedstocks can entail different environmental burdens. This aspect is further discussed in the results and discussion section. Another focus in the comparison is biobased PET (Bio PET), as its integration into the PET market is driven by increasing environmental awareness, evolving regulations, and technological progress. 46 Bio-PET, which is compatible with conventional PET recycling, is expected to see global production rise from 2.4 to 9.2 million tonnes. 29 To address this projected expansion Bio-PET production was also modeled to assess its environmental implications. While 100% biobased PET is not yet commercially available, emerging technologies are progressing and attracting limited market interest. 47 Accordingly, among several biobased MEG production routes, this study focuses on synthesis from bioethanol obtained from sugar cane. 48 As shown in Figure 2, this involves biomass fermentation into ethanol, followed by dehydration to ethylene, then conversion into ethylene oxide and subsequently MEG. 48−50 On the other side, the biobased TPA production model follows the methodology proposed by Volanti et al., which involves the synthesis of isobutanol, subsequent conversion to para-xylene, and final oxidation to TPA. 51 Although fully biobased PET technologies remain in early development, this study has been taken as reference since it models a theoretical scenario combining sugar cane-derived MEG and corn-derived TPA. Sugar cane-based MEG is one of the most established production methods, while corn-derived TPA was selected based on Volanti et al., who identified it as the only process currently operating at industrial scale. 51 This assumed combination reflects a hypothetical case, as no fully biobased PET is presently on the market. Inventories used in the modeling of Bio-PET are reported in Tables S7−S10.Distinction of Treatment Capacities of Mechanical and Chemical Recycling As previously discussed, mechanical recycling is limited in its ability to process the full stream of PET waste, hindering complete circularity. The fraction of PET that is too degraded or compromised must be substituted with virgin material, creating a systemic gap. Chemical recycling presents a potential solution, allowing for processing the whole fraction of PET waste types without the constraints of mechanical methods. However, as noted earlier, its environmental impacts, when assessed in isolation over a single cycle, may exceed those of mechanical recycling. 29 This points to the importance of finding a convergence between circularity and environmental impact. 33 Accordingly, this section underscores the importance of integrating complementary recycling technologies to manage PET waste comprehensively and sustainably. Three future scenarios for the European PET market, reported in Figure 3, were modeled relying on literature data. 52 Each incorporates varying shares of landfill, incineration, mechanical, and chemical recycling. The scenarios differ in the relative proportions of mechanical and chemical recycling, enabling assessment of their combined effectiveness. In all cases, recycling alone is insufficient to meet demand, implying continued virgin PET production. The system boundaries for this analysis focus solely on the waste management phase and differ from those in previous sections (see Supporting Information, Figures S1 and S2). A consistent cut-off method was applied to all waste treatment processes to allow a fair comparison. Chemical recycling boundaries cover feedstock pretreatment, depolymerization, monomer purification, and repolymerization into r-PET granules, based on the MADE process (Figure 1). Mechanical recycling, incineration, landfill, and virgin PET production were modeled using individual proxies from the ecoinvent database. 43 The complementary scenario (CS, Figure 3a) models the 2040 European PET market and outlines strategies to enhance circularity and sustainability. 52 Key measures include demand reduction, improved collection and sorting, and integration of mechanical and chemical recycling. In this scenario, 39% of PET is mechanically recycled, 26% chemically recycled, 26% incinerated, and 4% landfilled; the remaining 5% is exported, lost, or still in use. To meet total demand, 2.5 Mt of virgin PET is required. Two alternative 2040 scenarios were developed to explore the effects of reduced chemical recycling capacity. In the partially integrated scenario (PIS), chemical recycling drops to 13%. PET packaging originally processed chemically is shifted to mechanical recycling, raising its share to 44%. Since textiles are unsuitable for mechanical recycling, they are redirected to incineration (33%) and landfill (6%), increasing virgin PET demand to 3.1 Mt (Figure 3b). In the mechanical scenario (MS), chemical recycling is entirely excluded. Here, 49% of PET is mechanically recycled, 41% incinerated, and 6% landfilled, resulting in a virgin PET demand of 3.7 Mt (Figure 3c). In both PIS and MS, 4% of PET remains exported, lost, or in use. All scenarios assume a constant PET demand of 7.2 Mt and model a single recycling cycle. To evaluate environmental performance, the climate change potential impact (t CO2 eq) of each PET management option and virgin production was calculated. 42 In all scenarios, three additional subscenarios for mechanical recycling were included to reflect real-world inefficiencies. 28 InFigure 2. Schematic synthesis of biobased PET from bio-TPA and bio-MEG. 50Figure 3. Schematic representation of the complementary scenario (a), partially integrated scenario (b), mechanical scenario (c).order to consider the lower quality of PET resulting from mechanical recycling, corrective factors of 1.0, 0.8, and 0.5 were multiplied to the mechanically recycled PET, aiming at representing 100%, 80%, and 50% efficiency, respectively. These variations offer a more realistic view of the contribution of mechanical recycling across different performance levels. As LCA alone does not capture system circularity, the results were complemented with circularity indicators to provide a more comprehensive assessment. 53 The “percent actual recycled material derived from outflow” (R) was used as a key metric (eq 1)R =mass of recycled material derived from outflow total mass of outflow (1) This circularity indicator measures the effective recovery of materials from resource outflows through a combination of collection and recycling performances. 54 Therefore, the impact per recycled unit was calculated for all scenarios (CS, PIS and MS, and the cases APs) as follows (eq 2)= R impact per recycled unit total impact in ktCO2 eq(2) This metric reflects the GHG emissions generated per unit of PET recycled, allowing a comprehensive assessment of the circularity in each scenario and highlighting the value of integrating complementary technologies for PET waste treatment.■ RESULTS AND DISCUSSION The complete summary of the environmental impacts for the MADE chemical recycling is reported in Table 1. Figure 4 provides a normalized comparison of the three processes, enabling evaluation of their relative performance within a broader system perspective. The full environmental profile of Bio-PET and Virgin PET are available in the Supporting Information (Tables S13 and S14).Among them, Bio-PET consistently exhibits the highest impacts across all categories. This outcome is primarily attributable to the early stage development of the technology and the prototype-scale data used for inventory modeling, indicating that industrial-scale implementation could substan tially reduce its footprint. 55,56 Although hypothetical, the Bio PET process highlights environmental burdens significantly higher than both the Chemically recycled and the Virgin PET, emphasizing the need for further research and technological innovation. These results should be viewed as preliminary projections, with substantial opportunities for improvement. Key strategies include Scale Up in Bio-PET production, transitioning to second-generation biomasses that avoid competition with food crops, and implementing more sustainable agricultural practices (e.g., improved irrigation, organic fertilizers). Such measures could reduce the potential environmental impact due to biomass cultivation, making fully biobased PET a more viable and sustainable alternative for future markets. 57 In contrast, chemically recycled PET generally outperforms virgin PET, showing lower impacts in 12 of 18 impact categories. However, it presents higher impacts in eutrophica tion, both marine and freshwater (FE, ME), ecotoxicity, both marine and freshwater (FET, MET), human non-carcinogenic toxicity (HTnc), and water depletion (WD). Figure 5a reports the values of GW for the three processes analyzed, using both the current European electricity mix and the expected mix at 2050. The full environmental profiles for the three processes using renewable energy are available in the Supporting Information (Tables S12−S15 and Figures S3− S8). CED results are reported in Figure 5b and in Table S15 of the Supporting Information in their numerical form. The most relevant energy sources across the product life cycle are nonrenewable fossil energy and renewable biomass. The latter, as expected, contributes substantially to the Bio-PET scenario. Despite exploring scenarios in which the energy consumed is assumed to be replaced with renewable energy, the overall CED impacts do not decrease substantially (i.e., −20% in the baseline scenario, −4% in the Bio-PET scenario, and −2% in the traditional PET scenario). This is because the CED indicator accounts not only for the energy directly consumed in the processes under study, but also for the energy embodied in the materials and, more generally, in all the flows involved. The transition to renewable energy across all three processes does not result in significant reduction of environmental impacts. The most pronounced improvements occur in chemical recycling, reflecting its high energy intensity. In contrast, Virgin PET and Bio-PET production show only marginal changes, except in the Ionizing Radiation category, where impacts are notably affected. This difference stems from the fact that Virgin PET and Bio-PET impacts are largely driven by raw material production, whereas recycling impacts are primarily associated with energy use for waste trans formation, specifically purification, depolymerization, separa tion, and repolymerization steps. As anticipated in the description of the inventory, the choice of the proxy representing the biomethane production may significantly affect the outcomes of the sensitivity scenario, since the impacts of biomethane highly depend on its derivation. The selected ecoinvent proxy results in a CC value of 2.09 × 10−5 kg CO2 eq/m 3., much lower than the natural gas (0.679 kg CO2 eq), but higher than some cases available in the literature, in which the final balance assigned negative impacts (i.e.,Table 1. Environmental Profile of MADE Chemical Recycling for 1 kg of PET impact category acronym unit Total global warming GW kg CO2 eq 2.55E + 00 stratospheric ozone depletion OD kg CFC11 eq 7.11E − 07 ionizing radiation IR kBq Co-60 eq 2.14E − 01 ozone formation, human health POFh kg NOx eq 4.30E − 03 fine particulate matter formationPMF kg PM2.5 eq 1.98E − 03 ozone formation, terrestrial ecosystemsPOFe kg NOx eq 4.54E − 03 terrestrial acidification TA kg SO2 eq 4.91E − 03 freshwater eutrophication FE kg P eq 9.77E − 04 marine eutrophication ME kg N eq 1.77E − 04 terrestrial ecotoxicity TET kg 1,4-DCB 6.61E + 00 freshwater ecotoxicity FET kg 1,4-DCB 3.60E − 01 marine ecotoxicity MET kg 1,4-DCB 4.59E − 01 human carcinogenic toxicity HTc kg 1,4-DCB 5.80E − 01 human noncarcinogenic toxicity HTnc kg 1,4-DCB 5.58E + 00 land use LO m 2a crop eq 6.33E − 02 mineral resource scarcity MRD kg Cu eq 1.01E − 02 fossil resource scarcity FD kg oil eq 7.40E − 01 water consumption WD m 3 2.58E − 02credits) to these systems, especially if they derive from waste with no economic value and are employed to produce energy. 58,59 Accordingly, it should be noted that the selected proxy represents a conservative modeling choice. More favorable assumptions regarding feedstock origin and process ing could lead to lower impacts, meaning that a less conservative proxy would likely result in further environmental benefits associated with the use of biomethane. Notably, certain impact categories exhibit increases under a renewable energy mix, particularly those sensitive to land and water use. Nevertheless, the shift to renewable energy delivers overall improvements across most impact categories. Powering chemical recycling with clean energy enhances the sustain ability of the recycled material lifecycle, strengthening process competitiveness. Achieving such a transition depends on robust political support and regulatory frameworks. Policies promoting large-scale renewable adoption, such as the European Union’s renewable energy directive (Directive (EU) 2023/2413), are central. In September 2023, the European Parliament set a 42.5% renewable share target for 2030, encouraging Member States to reach 45%, with the long term objective of 100% by 2050. Extending similar measures globally would foster favorable conditions for renewable investments. Complementary actions, subsidies, incentives for infrastructure, and potential penalties for fossil fuel reliance could further accelerate the transition. At the same time, industry must overcome practical barriers, particularly the intermittency of certain renewables, through investment in storage solutions or hybrid systems to ensure reliability. Complementarity Analysis The final part of the study aimed to highlight the complementarity of chemical and mechanical recycling for a more sustainable and circular PET waste management. To achieve this, the total GHG emissions for each scenario (CS, PIS, MS) were calculated (Supporting Information, Tables S16−S22) in a system expansion logic. As previously mentioned, scenarios with different mechanical recycling efficiencies were also considered, accounting for varying efficiency levels and avoided product (AP) rates of 100%, 80%, and 50%. The AP approach is supported by ISO 14044, which identifies system expansion as the preferred procedure over allocation when an increased level of detail in the analyzedFigure 4. Comparison between MADE chemical recycled PET, Biobased PET and Virgin PET in the EU market. The results have been normalized with respect to the maximum value.Figure 5. Comparison and hotspot analysis related to the climate change (a) and CED (b) categories for the chemically recycled PET, the Bio based PET and the Virgin PET, both with European electricity mix (EU Mix) and with renewable energy (RE).system is not feasible. It is specified that this approach still falls within an attributional LCA framework, as it merely follows the ISO recommendations for handling multifunctionality. To shift the study from an attributional to a full consequential perspective, it would have been necessary to introduce market-mediated effects, marginal substitutions, or broader economic system responses, which were intentionally excluded as they lie outside the control and scope of the analyzed system. The adopted choice is therefore consistent with the attributional framework or at least a more conservative “consequential if under control” as reported in literature. 60 The total impact of each scenario is presented below in Table 2.The Complementarity Scenario consistently exhibits the lowest total system impacts, regardless of the AP rates considered. For instance, at 100% mechanical recycling efficiency, overall impacts rise sharply, with PIS showing a 61% increase and MS reaching 2.3 times the CO2 eq. emissions of CS. This growth underscores the consequences of reducing or eliminating chemical recycling. In PIS, halving chemical recycling shifts the system toward greater reliance on mechanical recycling and waste management (landfilling, incineration), moderately raising impacts. In MS, where chemical recycling is removed, higher dependence on mechanical recycling and virgin PET drives a far steeper rise in GHG emissions. Analysis of mechanical recycling efficiencies (AP = 100%, 80%, 50%) reveals a consistent trend: lower efficiency increases virgin PET demand and exacerbates burdens. While absolute values grow as efficiency declines, the pattern remains, reduced chemical recycling heightens reliance on virgin PET, elevating emissions and resource use. For instance, in CS, total system impact rises by 8881.1 kt CO2 eq (196%) when AP falls from 100% to 50% (from 4526.0 to 13407.1 kt CO2 eq). Similarly, in MS, total system impact rises by 11101.4 kt CO2 eq (108%) when AP falls from 100% to 50% (from 10298.8 to 21400.2 kt CO2 eq). These findings highlight the need to optimize recycling efficiencies while maintaining chemical recycling capacity. Circularity was assessed through the R indicator: CS reached 65%, compared to 57% for PIS and 49% for MS. Impacts per recycled PET unit are reported in Table S21. This analysis confirms the importance of integrating both mechanical and chemical recycling to balance circularity and environmental performance. Importantly, sustainability and circularity, though often complementary, do not always align. A process with lower emissions may not advance circularity goals, under scoring the necessity of evaluating both LCA indicators and circularity metrics together. The results also challenge the assumption that mechanical recycling is inherently superior. While advantageous in some respects, it cannot handle all PET types. Chemical recycling complements mechanical methods, enabling material loops that would otherwise remain open. Recognizing its necessity could inform targeted policy measures, such as subsidies for chemical recycling facilities and expanding extended producer responsibility (EPR) schemes to include plastic textiles. 61 Such measures would contribute to building a more resilient and effective recycling infrastructure, ultimately supporting a more sustainable and circular PET waste management system. Limitations and Future Research This study relies on several assumptions due to data gaps, modeling constraints, and methodological choices, which also indicate directions for future research. For the future electricity mix, assumptions were necessary owing to limited data. Since no previsions were available, current European providers and proportions were applied where possible. Assumptions regarding transformation losses and process compatibility were also required. Polymerization and sorting phases remained unchanged, so modifications primarily affected chemical recycling. Overall, the proposed energy mix is not a prediction of future systems but a demonstration of the critical role of renewables in achieving long-term sustainability. Future research should refine these scenarios as more accurate data become available. This study includes the following assumptions due to data gaps, modeling limitations, and necessary choices, which suggest directions for future research. In the Bio-PET production modeling, sugar cane was chosen for bio-MEG as it is the most established method 62 and corn derived TPA was used for the fully biobased PET since, to date of submission, was the only industrial-scale production route in Volanti et al. 51 However, it is again specified that the production of 100% Bio-PET is currently not commercially available at the time of writing this study. Further research should involve using primary production data as they become available. The study also relies on assumptions regarding PET waste management in 2040, particularly the allocation of packaging and textiles between landfill and incineration, due to limited data. More accurate PET market data would improve model reliability and support better-informed waste management strategies. Moreover, the analysis was restricted to a single recycling cycle, whereas a multicycle perspective would better reflect long-term impacts. 34 Unlike mechanical recycling, which increasingly depends on virgin PET, chemical recycling regenerates waste into high-quality PET, reducing virgin demand. Future research should develop multicycle models to fully capture these benefits. The CFF offers a suitable framework, as it integrates open- and closed-loop recycling while accounting for multiple cycles. 63 These limitations offer insights into avenues for refining strategies in the future.■ CONCLUSIONS Applying the LCA procedure to the GR3N recycling process enabled the assessment of its grave-to-cradle environmental impact and comparison with scenarios aligned with Europe’s long-term sustainability goals and the evolving PET market. This result corroborates that the environmental performance of chemical recycling remains inferior to that of mechanical recycling. However, it is relevant to recognize that the two processes yield different products, making a direct comparison intrinsically unfair. A more appropriate comparison should be done with virgin or biobased PET, as the resulting products exhibit equivalent properties. In this case, the chemicalTable 2. Carbon Footprint Value in ktCO2 eq. for Each Scenario, Climate Change Category (Method EF 3.1)total system impact (kt CO2 eq.)CS (a) PIS (b) MS (c)AP = 1 4.526 7.428 10.299AP = 0.8 8.078 11.266 14.739AP = 0.5 13.407 17.261 21.400recycling process demonstrates the lowest overall environ mental impact, even with respect to the fossil-based material. The study also examined the complementary roles of chemical and mechanical recycling within a single cycle in the European PET market. Results highlight the critical interplay between the two: reducing or eliminating chemical recycling substan tially raises emissions, as shown in the PIS and MS scenarios, due to increased virgin PET demand. Mechanical recycling efficiency further shapes overall performance. Together, these findings stress the need for a balanced recycling approach, where both technologies complement each other to achieve optimal sustainability outcomes. The analysis also showed that the process can achieve a small reduction in GHG emissions when powered by a 100% renewable electricity mix. In conclusion, PET waste management requires a systems thinking perspective. As a complex environmental challenge, it cannot be effectively addressed through reductionist approaches alone. 36 Traditional approaches, which optimize individual processes, may overlook the complex interdepen dencies between technologies and environmental goals, leading to partial solutions that fail to capture the full circular potential of PET recycling. By analyzing the combined roles of chemical and mechanical recycling, this study emphasizes that each technology has unique strengths and limitations, with chemical recycling providing an essential complement to mechanical recycling in processing waste streams that the latter cannot handle. This complementary relationship reduces reliance on virgin PET, increasing overall circularity and reducing the environmental footprint at the system level. Achieving a robust and sustainable PET waste management system requires implementing both recycling technologies, transitioning to renewable energy sources, and integrating biobased PET if it becomes a viable material.■ ASSOCIATED CONTENT *sı Supporting Information The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acssuschemeng.5c12048. Additional modeling details, production schemes, materials, methods, results and uncertainty analysis are available (PDF)■ AUTHOR INFORMATION Corresponding Authors C. Brondi − CNR STIIMA−Institute of Intelligent Industrial Technologies and Systems for Advanced Manufacturing, National Research Council, Milano 20133, Italy; Email: carlo.brondi@stiima.cnr.it D. Cespi − Department of Industrial Chemistry “Toso Montanari”, University of Bologna, Bologna 40129, Italy; Interdepartmental Centre of Industrial Research “Renewable Resources, Environment, Sea and Energy”, University of Bologna, Rimini 47922, Italy; orcid.org/0000-0002- 6348-6111; Email: daniele.cespi2@unibo.it Authors F. Caraceni − CNR STIIMA−Institute of Intelligent Industrial Technologies and Systems for Advanced Manufacturing, National Research Council, Milano 20133, Italy; orcid.org/0000-0002-3437-2094F. Arfelli − Department of Industrial Chemistry “Toso Montanari”, University of Bologna, Bologna 40129, Italy; orcid.org/0000-0003-4399-4052 R. Sansi − Department of Industrial Chemistry “Toso Montanari”, University of Bologna, Bologna 40129, Italy A. Ballarino − CNR STIIMA−Institute of Intelligent Industrial Technologies and Systems for Advanced Manufacturing, National Research Council, Milano 20133, Italy F. Passarini − Department of Industrial Chemistry “Toso Montanari”, University of Bologna, Bologna 40129, Italy; Interdepartmental Centre of Industrial Research “Renewable Resources, Environment, Sea and Energy”, University of Bologna, Rimini 47922, Italy; orcid.org/0000-0002-8248-2044 Complete contact information is available at: https://pubs.acs.org/10.1021/acssuschemeng.5c12048 Author Contributions ∥F.C. and F.A. contributed equally to the manuscript. Notes The authors declare no competing financial interest.■ ACKNOWLEDGMENTS The authors acknowledge GR3N for providing the primary data for the life cycle modelling and analysis. Their contribution was critical to the completion of this work. The authors also thank all collaborators for their valuable input and technical support throughout the study.■ REFERENCES (1) Fortunato, M. E.; Vitiello, R.; Taddeo, F.; Turco, R.; Russo, V.; Tesser, R. 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PublishedFeb 24, 2026
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