Polymer-based multilayer packaging materials are commonly used in order to combine the respective performance of different polymers. By this approach, the tailored functionality of packaging concepts is created to sufficiently protect sensitive food products and thus obtain extended shelf life. However, because of their poor recyclability, most multilayers are usually incinerated or landfilled, counteracting the efforts towards a circular economy and crude oil independency. This review depicts the current state of the European multilayer packaging market and sketches the current end-of-life situation of postconsumer multilayer packaging waste in Germany. In the main section, a general overview of the state of research about material recycling of different multilayer packaging systems is provided. It is divided into two subsections, whereby one describes methods to achieve a separation of the different components, either by delamination or the selective dissolution–reprecipitation technique, and the other describes methods to achieve recycling by compatibilization of nonmiscible polymer types. While compatibilization methods and the technique of dissolution–reprecipitation are already extensively studied, the delamination of packaging has not been investigated systematically. All the presented options are able to recycle multilayer packaging, but also have drawbacks like a limited scope or a high expenditure of energy.

Plastic‐based multilayer packaging has an important function on the packaging market, but is currently not recyclable as the polymer layers used are usually thermodynamically immiscible. This work therefore follows the approach to prepare separable multilayer packaging using a packaging adhesive modified with thermally unstable adducts, and proposes a corresponding recycling process. For this purpose, typical multilayer structures (polyethylene (PE)// polyethylene terephtalate (PET), PET//aluminum, and PE//aluminum) were prepared by curing furan‐/maleimide‐functionalized polyurethane (PU)‐prepolymers with a three‐functional cross‐linking agent. Adhesions of up to over 3N per 15 mm test specimen were measured or substrate failures of PET films were observed. However, heating in dimethylsulfoxide, the retro‐Diels–Alder reaction takes place and the cross‐linked adhesive turns thermoplastic and dissolves in the solvent. Thus, the laminate separates and the pure PE, PET, and aluminum foils can be recovered without any PU residue.

Lacking recyclability of multilayer packaging can be overcome by using a thermoreversible crosslinking adhesive consisting of maleimide- and furan-functionalized polyurethane-(PU-)prepolymers, reacting in a Diels–Alder-reaction. Here, the furan-functionalized PU-prepolymer carries furan-side-chains to avoid the usage of an additional crosslinking agent. Thus, N‑(2‑hydroxyethyl)maleimide and furfurylamine are the only two chemicals contained in the adhesive that are not listed in the appendix of EU Regulation 10/2011. Using migration modelling, it could be shown that, at 23 °C, both chemicals have lag-times of only a few minutes if 45 µm PE is used as a barrier. However, if the residual content is below 30 mg/kg, the legally specified maximum amount of 0.01 mg/kg food is not reached. After determining the diffusion coefficients and the activation energy of diffusion through ethylene-vinyl alcohol copolymer (EVOH), it could be determined that the lag-time of the migrants can be extended to at least 9 years by the use of 3 µm EVOH. From a food law point of view, the use of the described adhesive is possible if the above‑mentioned measures are complied.

Multilayer packaging is an important part of the packaging market, but it is not recyclable with conventional methods since it is made of different thermodynamically immiscible materials. In this work, it was shown that it is possible to produce a PET//LDPE laminate in a pilot plant for lamination by using an adhesive consisting of maleimide- and furan-functionalized polyurethane prepolymers that cure through the Diels–Alder reaction. The material could then be delaminated in a small-scale recycling plant using a solvent-based recycling process by partially opening the Diels–Alder adducts through the influence of temperature. The PET and LDPE could be recovered without any adhesive residues before each material was regranulated, and in the case of the PE, a film was produced via cast film extrusion. The obtained PET granulate exhibited a slight, approximately 10%, decrease in molecular weight. However, since small amounts of LDPE could not be separated, compatibilization would still be required here for further use of the material. The obtained LDPE film was characterized by means of infrared spectrometry, differential scanning calorimetry, tensile testing, determination of the melt index, and molecular weight. The film showed lower crosslinking than usual for LDPE recycling and exhibited good mechanical properties. In this work, it was thus shown that upscaling of the laminate production with the modified adhesive and also its recycling at the pilot plant scale is possible and thus could be an actual option for recycling multilayer packaging.