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in-built Triggered Enzymes to Recycle Multi-layers: an INnovation for USes in plastic-packaging

Periodic Reporting for period 3 - TERMINUS (in-built Triggered Enzymes to Recycle Multi-layers: an INnovation for USes in plastic-packaging)

Berichtszeitraum: 2022-03-01 bis 2023-07-31

TERMINUS addresses the challenge of unlocking recycling and reuse of flexible multi-layer and multi-compounds packaging materials used for food, beverages, cosmetics, pet food, fertilizers, any perishable goods in general. Known for its invaluable properties, multi-layer packaging is widely used in many packaging applications. However, these materials are non-recyclable given the conventional recycling methods, and therefore largely incinerated or landfilled.

A range of smart enzyme-containing polymers with triggered intrinsic self-biodegradation properties will be developed, acting as adhesives or tie layers in the design and manufacturing of multi-layer plastics for food and non-food applications. The technology will be applied to biodegradable PUR-based adhesives for adhesive lamination and extrusion coating lamination, and polymers and tie layers (PBS, PLA, PPC or PCL) in blown extrusion. Controlled biodegradation of these adhesives and tie layers would enable the separation of the different layers (e.g. PET, HDPE, LDPE, or Aluminum) of the packaging, which can then be recycled using conventional recycling methods.

TERMINUS will base its innovative and challenging objectives on a cross-disciplinary team of renowned organizations with expertise in enzymatic biodegradation of polymers, thermal protection of enzymes using nm organosilica and layered double hydroxide, cyclodextrins, UV and water triggered enzymatic activity, formulation of advanced polymers, manufacturing of multilayer plastic packaging, plastics recycling.

Two classes of enzymes have been selected (hydrolases and oxydases). Three processing tachniques for producing Terminus mulltilayers films have been involved (lamination, Blown coextrusion and lamination coating). After having solved the major identified bottlenecks, Terminus multilayers films have been produced at lab scale (g), at pilot scale (1kg) and finally at industrial scale (tenth of kgs). For on-demand separation/delamination, three demonstrators have been built up allowing themselves three different capabilities (g kg 10th kg) of Terminus multilayers films delamination. Delaminated films have been recycled according to the Recyclass protocol and the properties of Terminus recyclates have been assessed.
Since the beginning of the project (January 2019) a lot of works and activities have been carried out. All the guidelines to process model multilayers flexible films have been reviewed as well as for lamination process and for extrusion coatings. Hydrolases and oxidases enzyme have been selected regarding their capacities for enzymatic degradation for both adhesive and tie layers (Polyurethane and bioplastics based). Solvent based and solvent free specific polyurethane formulations have been designed with the aim to meet usual PUR tie layers properties (pot life, viscosity...). Finally, triggering and shielding activities have also started in order to make the rate of enzyme survival compatible with the processing thermomechanical constraints (time, temperature...). A preliminary LCA model has been built up as it will be an important issue of the project. As for circular economy, bibliographic survey has been made and metrics for circular economy assessment validated. Regarding this last point, Terminus project is one of the H2020 consortia founders participating in the Plastic Circularity Multiplier.

While period 2 was essentially devoted to identify the major bottlenecks by scaling up lab-scale to pilot-scale trials, period 3 has been mainly dedicated to solving these main bottlenecks (Size and size distribution of the inorganic containers, PUR formulations parameters, Adhesion promotion for final properties,..). Once done, it has been possible to produce terminus multilayers films at an industrial scale with the three designed technologies (Lamination, blown coextrusion, and coextrusion coating). These samples have been delaminated and separated in a prototype demonstrator and the separated streams of each individual layers have been recycled and characterized according to the Recyclass protocol. A whole environmental assessment connecting Life Cycle Analysis together with Circular metrices have been established for demonstrating and quantifying the circular improvement of Terminus technology.

Two Terminus workshops (scientific and industrial) have been organized as well as five breakfasts in five European different countries. Finally, Terminus has also participated to the innovation Forum for plastics who has taken the following lead on the Circularity Multiplier Cluster. All along the project, Terminus partners have been aware to disseminate the vast majority of information in open access. All this information can be found on the Terminus community on Zenodo data repository (https://zenodo.org/communities/terminus-h2020)
All the results of the Terminus project have allowed us to reach the whole level of demonstrating the initially proposed concept, meaning:
- Use of enzymes for designing specific additives for tie layers and adhesives used for laminated and coextruded plastic multilayers
- Shielding and triggering these adhesives to protect them of the thermal stresses
- Carrying out on-demand delamination at demonstration scale

Thus, the initial Terminus concept has been validated at lab scale, at pilot scale and finally at industrial scale. In parallel, a whole environmental and circularity assessment has been validated. Moreover, a Terminus Digital Product Passport has been originally proposed.

A lot of progresses beyond the state of the art have been accomplished during Terminus project:
- Moving non-recyclable to recyclable multilayers plastic films
- Demonstrating the capacity to control the whole cycle of life of a plastic multilayer
- Improving thermal survival of enzymes by using specific chemicals (NADES ) and/or inorganic containers
- Designing a specific Enzyme degradable Polyurethane adhesive
- Linking and connecting LCA with circular indicators
The project may result in major market opportunities for European industrials in several well-established markets ready for market opportunities: plastic packaging, industrial enzyme applications, PUR adhesives, biodegradable plastics, biotech plants and mechanical recycling. At least 15% of improvement of economic efficiency compared to current solutions (landfilling, incineration) is expected, with a reduction in landfilling for multi-layer plastic packaging of over 80%, as well as a reduction of overall plastic landfilling by 55%. Furthermore, a minimum decrease of 65% of the overall CO2 footprint will be achieved.

Increasing the recyclability of multi-layer packaging will significantly aid the efforts of reaching the target of recycling 55% of packaging waste by 2030, as set by the European Commission.
Objectives of TERMINUS project