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Removal of Legacy Substances from polyvinylchloride (PVC) via a continuous and sustainable extrusion process

Periodic Reporting for period 3 - REMADYL (Removal of Legacy Substances from polyvinylchloride (PVC) via a continuous and sustainable extrusion process)

Reporting period: 2022-06-01 to 2023-11-30

Polyvinyl chloride, also called PVC or simply vinyl, is one of the most widely used polymers in the world. It can be found in products such as piping, shower curtains, window frames, cable insulation, flooring and even medical equipment. Due to the long useful life of many PVC products, old PVC products can contain hazardous additives that are no longer allowed in new PVC products, therefore recycling is challenging. The EU-funded REMADYL project is tackling this important problem with (semi)-continuous processes to remove the additives and deliver high-quality REACH-compliant PVC.

The presence of legacy substances (LS) is a persistent barrier for PVC recycling as there are currently no economically viable solutions for their removal. This seriously hampers the recycling of PVC. Indeed, although the material itself is intrinsically very well suited for recycling (almost 800.000 tons of PVC were recycled in 2019 within VinylPlus), however, (1) No viable methods exist to remove lead and plasticizers from PVC; (2) Mechanical recycling does not remove any of the hazardous substances from PVC and (3) Lead content in the PVC remains and is transferred into the new product

At the end of the project, the following key achievements have been reached:
* Three lab-scale processes for rejuvenating PVC have been developed and tested: (i) supercritical carbon dioxide (scCO2) cleaning technologies for phthalate removal from plasticized PVC; (ii) use of Layered double hydroxides (LDH) as scavengers for lead in the PVC melt; (iii) extraction and improving accessibility of the LS in the PVC matrix via Natural Deep Eutectic Solvents ((NA)DES) and green solvents.
* Detection and sorting process for PVC containing legacy substances: a lead monitoring and sorting prototype was developed and validated in industrial site.
* Pilot line development for a continuous extractive extrusion process for rejuvenating PVC: first steps for upscaling all processes were taken, a detailed report was composed pinpointing the lacking elements to further increase the TRL of the technologies.
* Demonstration of the re-use of rejuvenated PVC materials streams: the feasibility of using rejuvenated PVC in water proofing membranes was shown. The use of rejuvenated PVC was proven in injection moulding for cable grommets. The principals of inline sorting of Pb containing materials have been proven by IRIS and Deceuninck.
* Safe handing and re-use of the by-products: successful recovery of high purity metallic lead from comparable lead salts, and conclusive evaluation of contaminants and guidelines and methodology for the safe handling of by-products.
* Policy contribution at European, national and regional level: Special effort was put in place for the writing of the Joint Policy Brief with CREAToR project and to the establishment of the Circular Plastics Cluster born thanks to the support of the Horizon Results Booster Mod.B.
The LS of main concern are lead and DEHP. Therefore, to remove these legacy substances, REMADYL investigates three different extraction technologies: (i) supercritical carbon dioxide (scCO2) cleaning technologies for phthalate removal from plasticized PVC; (ii) use of Layered double hydroxides (LDH) as scavengers for lead in the PVC melt; (iii) extraction and improving accessibility of the LS in the PVC matrix via Natural Deep Eutectic Solvents ((NA)DES) and green solvents. Furthermore, a prototype was developed to detect and sort lead containing PVC.

The technical R&D work focussed on (i) the final optimization and upscaling of the extraction technologies, on (ii) the development and testing of the sorting prototype, (iii) the safe disposal of the byproducts and (iv) the demonstration of re-use of rejuvenated PVC in end-applications. More in detail:

• In WP1 a lead monitoring and sorting prototype was developed, based on LIBS point-detection technique, with sufficient high resolution. The prototype was successfully validated at the PVC recycling plant of Deceuninck.
• In WP2 batch extractions process were developed leading to high extraction rates (>70%) for DEHP in P-PVC, the use of pure extraction solvents for Pb in uPVC with extraction rates of 88 % and a filtering capacity of the LDH for lead of 40%.
• In WP3 scale-up of the scCO2 cleaning technology for DEHP removal from soft PVC was further investigated in a semi-continuous batch process with achieved extraction rates of 70%. Regarding Pb removal from rigid PVC, (i) the solid-liquid extraction process with green solvents was further optimized with extraction rates up to 91% and (ii) in-line continuous extractive extrusion was performed using LDH scavengers achieving a reduction of lead content of 60%.
• In WP4 the main advances have been made in the successful recovery of high purity metallic lead from comparable lead salts, as well as in the final evaluation of contaminants and guidelines and methodology for the safe handling of by-products.
• In WP5, the feasibility of using rejuvenated PVC in water proofing membranes was shown by Danosa. The use of rejuvenated PVC was proven in injection moulding for cable grommets by Promolding. The principals of inline sorting of Pb containing materials have been proven by IRIS and Deceuninck.
• In WP6 data collection continued to develop mass and energy balances on REMADYL technologies leading to the final LCA, LCC and s-LCA results showing the importance of green solvents and solvent re-use.

Regarding the dissemination and communication (WP7), our key achievements were presented in a dissemination event held live at ECOMONDO 2023 and streamed online. REMADYL has been presented at 26 international conferences and established further synergies with ongoing projects and initiatives. Special effort was put in place for the writing of the Joint Policy Brief with CREAToR project and to the establishment of the Circular Plastics Cluster born thanks to the support of the Horizon Results Booster Mod.B.
To tackle this major challenge, REMADYL have developed breakthrough (semi-)continuous processes based on extractive extrusion technology in combination with novel solvents and melt filtration, which has the potential of rejuvenating ‘old PVC’ into high purity PVC tuned towards the demands of various soft and hard PVC products. The process also has potential for other plastics applications, e.g. removal of (halogenated) flame retardants. The extracted phthalate plasticizers can be safely disposed and the lead can be re-used in batteries.

REMADYL is delivering a breakthrough support to the Circular Economy Package and resource efficiency targets for Europe as recovered PVC will reduce incineration and landfilling. The developments are expected to bring the following long-term impacts:
*Increased purity and/or desirable quality of Secondary Raw Materials
*Increased recycling rate for, and reduced landfill and incineration of, Secondary Raw Materials
*Reduced risk of retaining hazardous substances in recycled materials
*The implementation of the European Commission Strategy on Plastics in a Circular Economy and of the SPIRE PPP Roadmap
*Improving industries innovation capacity and creating market opportunities
*Contribution to climate protection: recycling generates lower CO2 emission than producing virgin PVC.
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