Macro Chemistry Physics - 20hvbhioj

PERSPECTIVE
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The Frontier of Plastics Recycling: Rethinking Waste as a

Resource for High-Value Applications
Hannah Mangold and Bernhard von Vacano*
plastics like polyurethane (PU) (see, e.g.,

Following the circular economy hierarchy of reduce and reuse, recycling is the Table S3, Supporting Information, in Ref.
third layer to close the loops for materials and decouple their value from [4]). At end of life (EoL), an incineration
consumption. Polymeric materials (“plastics”) are in principle well suited for step, as one of the current preferred op-
recycling, as they can be reprocessed with relatively low energy input as a tions in terms of waste abatement, adds
another 2–3 kg CO2 /kg[7] to the respec-
material, cleaved back into their monomers or converted back to feedstock.
tive carbon footprint (which can, by con-
Today, these approaches still fall short in quantitatively diverting waste sidering substitution of other CO2 -emitting
towards reuse. This perspective describes the industry challenges for recycling processes for the generated energy, be re-
back into high value applications of polymers, and the portfolio of existing duced to below 1 kg CO2 /kg by energy
and emerging technology solutions. Sustainable design of products and recovery).[8,9] Overall, plastics contribute to
3.5% of global greenhouse gas emissions
polymers, recycling technologies, appropriate business models, and enabling
today.[4] It is therefore obvious that plas-
technologies converge at the frontier of plastics recycling, for a transformation tics value chains need to be transformed
of the industry towards circularity and greenhouse gas emission neutrality. to achieve climate neutrality:[10] a recent
comprehensive analysis showed that net-
zero greenhouse gas emission plastics are
1. Introduction possible with existing technologies, combining biomass-derived
feedstocks, carbon capture and utilization (CCU) and plastics
A life without polymeric materials, by virtue of their versatility, recycling.[11] Recycling is identified as the key lever to keep re-
performance, and efficiency, today cannot be imagined. With the newable energy consumption for CCU low as well as limit com-
consequential growth of plastic production[1] from fossil raw ma- petition for biomass demand and optimize economics.
terials and subsequent plastics-derived waste two challenges exist Establishing a circular economy[12] for plastics is the most con-
that are intrinsically connected: environmental pollution,[2,3] ex- sequential approach to finally decouple economic growth from
acerbated by uncontrolled waste management, and contribution consumption (waste) and emissions. Reduction and reuse of
to CO2 emissions.[4] polymeric materials must be prioritized in conjunction with en-
While plastic waste for a long time has been considered by forcing recycling at EoL, to achieve circularity and climate neu-
many a local and aesthetic problem, the growing amounts of un- trality. In certain cases, certified compostable biopolymers can
managed or poorly managed plastic waste have elevated the is- be an additional contribution, for example, in conjunction with
sue on a global scale, and need to be curbed as a source of sec- reducing food waste in organic recycling via the biosphere, re-
ondary microplastics[5] formed by environmental degradation. turning nutrients to the soil, and enabling larger volumes of
Biobased plastics from non-fossil renewable raw materials con- compost.[13] While reduction and reuse in itself call for research
tribute less than 1% to all global plastics production.[6] For the and innovation on all levels, our article focuses on technical
majority of plastics, refining crude oil and the subsequent chem- recycling[14] pathways: the waste material has to be seen as the
ical transformations to monomers require energy inputs that re- valuable resource it is, that can be recycled and brought back into
sult in emissions of CO2 during production from ≈1.5 kg CO2 /kg applications to replace as much fossil based virgin plastics as pos-
for polyolefins to more than 4 kg CO2 /kg for some engineering sible.
Out of the estimated 8 Gt of plastics ever produced by hu-
H. Mangold, B. von Vacano mankind by 2015, 2.5 Gt were considered still “in-use stock”,[1]
BASF SE maybe as part of a car (dashboard, bumper, tire), a household ap-
Carl-Bosch-Str. 38, Ludwigshafen 67056, Germany pliance or item (fridge, salad bowl), or in buildings (pipes, win-
E-mail: [email protected] dow frames, or insulation material), to name a few. This high-
The ORCID identification number(s) for the author(s) of this article lights the different lifespans polymeric materials experience in
can be found under https://doi.org/10.1002/macp.202100488 various applications, ranging from many decades in construc-
© 2022 The Authors. Macromolecular Chemistry and Physics published tions, a dozen of years in transportation, a few years in toys or
by Wiley-VCH GmbH. This is an open access article under the terms of other household articles, to only months in packaging (Figure 1).
the Creative Commons Attribution License, which permits use, Due to their specific properties, different polymers are used
distribution and reproduction in any medium, provided the original work
is properly cited.
in the respective applications (Figure 2). Short-lived packaging
applications are dominated by the polyolefins PE, PP, and PET
DOI: 10.1002/macp.202100488
Macromol. Chem. Phys. 2022, 223, 2100488 2100488 (1 of 17) © 2022 The Authors. Macromolecular Chemistry and Physics published by Wiley-VCH GmbH
www.advancedsciencenews.com www.mcp-journal.de
Figure 1. Indications of typical life span ranges of plastics use in different applications, adapted from data from Refs. [1,15].
Figure 2. Polymer types by application. Data for 28 EU countries plus Norway (NO) and Switzerland (CH), 2019. Reproduced with permission of
PlasticsEurope, Source: PlasticsEurope Market Research Group (PEMRG) and Conversio Market & Strategy GmbH.
Polyester. These materials reach EoL and return, assuming ap- by material redesign outside of the packaging sector will have a
propriate waste collection and sorting infrastructure, typically significant delay before they can become effective.
within 1 year for possible recycling. On the other hand, the dom- Establishing a circular economy[12] for plastics, with all its ben-
inating polymer PVC in construction, for example, will stay in its eficial contributions to breaking the wave of waste[16] and achiev-
application for decades before it would even theoretically be avail- ing climate neutrality,[11] requires respective economic loops at
able again as feedstock. This has two important consequences for scale. Looking at EoL plastics as an industrial resource, availabil-
establishing a polymer circular economy: with polymer use vol- ity, quality, and price are key factors that determine how value
umes having grown exponentially in the last decades,[1] the com- chains will be able to transition.
position of available waste streams today is skewed towards the One way of organizing the available EoL polymeric material
material types used in short-lived applications. From an innova- streams is by a variant of the well-known polymer pyramid[17] that
tion perspective, the use–time lag also means any interventions organizes commercially applied polymers (thermoplastics) into
Figure 3. Polymer pyramid, grouping some exemplary polymers by their microstructure (amorphous on the left side versus semi-crystalline on the
right). On the y-axis, increasing performance of the materials (e.g., mechanics, temperature resistance) is indicated, together with the typical mate-
rial value in dollars per kilogram. The size of the respective bubbles reflects the production volumes in 2015. (LDPE: low-density polyethylene, HDPE:
high-density polyethylene, PP: polypropylene, PS: polystyrene, PVC: polyvinylchloride, PA6: polyamide-6, PA66: polyamide 6,6, PET: polyethylenethereph-
thalate, x-PUR: crosslinked polyurethanes, PBT: polybutylenetherephthalate, PC: polycarbonate, UHMW-PE: ultrahigh molecular weight polyethylene,
TPU: thermoplastic polyurethane, PESU: polyethersulfone, PPS: polyphenylenesulfonate). *) x-PUR, not being a thermoplastic material, is included for
comparison.
Figure 4. Simplified cost structure for the competition of virgin plastics and recyclates for the same application.
groups based on their structural properties (amorphous versus rials, any recyclate application competes with virgin material at
semi-crystalline) and clusters them by performance into tiers of the respective performance tier. The economics of recycling dif-
commodity plastics, engineering, and specialty engineering poly- fer from the virgin material value chain: instead of the cost of
mers (Figure 3). Together with performance, the price of materi- feedstock, cost occurs for collection, sorting, and pretreatment.
als is increasing. Prices range from roughly 1–2 $/kg for com- The production cost of virgin materials is replaced by the cost of
modity polymers up to tens of dollars per kilogram for specialty the respective recycling process steps (Figure 4).
plastics. Economics dictate the use of the most efficient materi- For recycling, feedstocks need to be available in reliable
als; hence polymers are chosen for applications to be sufficient quantities and, in the absence of regulatory interventions, at
by performance while minimizing cost. This is also reflected in low enough cost. At the same time, the quality of the stream
the production volumes, decreasing from commodity to specialty (e.g., purity of polymeric materials, presence of contamina-
materials. tions) directly determines: i) the cost of the subsequent sorting
In the world of virgin polymers, materials from the bottom of and cleaning steps; ii) the intensity of the recycling process;
the pyramid, by constant innovation in tweaking properties, con- and iii) quality, achievable properties, and the possible price
tinuously push into the respective applications of the next perfor- level for applications. To enable cost- and energy-efficient recy-
mance tier, competing by their beneficial cost position and estab- cling, collection and sorting is a crucial pre-requisite. A prime
lished economies of scale. This also sets the framework for plastic example for efficient collection is the PET bottle system in
recyclates: in the absence of regulatory measures like mandates Germany, where the use of a deposit system for PET bottles
or subsidies for recycled content, or penalties for virgin mate- helps to collect >95% of PET bottles and leads to a high rate of
mechanical recycling as a relatively pure waste stream is readily approach,[26] but today still ahead of the state of the art. The only
available.[18] limitation of the NIR sorting technology is black plastic waste
Today´s established plastics markets (Figure 3) point to the as NIR light is absorbed by many of the commonly used black
fact that commodity plastics offer the largest availability, also be- colorants, especially carbon black, and not reflected for spec-
cause they constitute the majority of components, for example, troscopic fingerprinting. Beyond certain black fractions in con-
in packaging waste streams. For them, the challenge is to recycle sumer waste, this is an even more pronounced problem, for ex-
at competitive cost, maintain performance, and handle minority ample, for automotive waste, where many parts are of black color
impurities. High performance materials, on the other hand, are and contain carbon black. As separate chemically homogeneous
limited in volume, often diluted according to their very special- streams, sortable black plastics in principle could be beneficial
ized applications as minority components in products and much for recycling, as a black color can consistently be achieved and
less available. While their virgin production costs are also higher is insensitive to discoloration challenges of light colored recy-
and could offer an economic stimulus for recyclates, higher price clates. Innovative technologies are being developed to solve this
levels are only justifiable by uncompromised properties. To sig- problem such as mid infrared spectroscopy with hyperspectral
nificantly drive the circular plastics economy: imaging [27–29] terahertz radiation,[30] fluorescence imaging,[31]
LIBS,[32] or fluorescence decay time analyses.[33,34] For all these
• availability issues need to be addressed, for example, by creat- techniques, advanced data analysis supported by machine learn-
ing deposit–return systems, as has been established very suc- ing tools is crucial for efficient sorting. Implementing such new
cessfully for PET bottles in many countries,[19] by tracking and technologies in a commercial sorting process would lead to in-
tracing, better sorting, by designing applications for recycling creased recycling rates as the economic viability of many mechan-
as well as by promoting well-designed extended producer re- ical or chemical recycling processes depend on the availability of
sponsibility systems;[20,21] relatively pure plastic material streams.
• recycling processes need to maintain or ideally even upgrade On the other hand, novel black pigments are also developed,
material performance to access similarly demanding applica- that allow for NIR sorting. Lanxess, for example, has introduced
tions in their second life. a black pigment based on iron oxide that still allows 20% NIR
reflectivity of pigmented articles to enable NIR sorting.[35,36]
Today´s polymer recycling value chains face limitations in all Another option to fundamentally upgrade sorting capabilities
mentioned areas. Improvements are emerging, and innovation is the use of markers to be able to identify plastics more easily.
is needed to consistently convert plastic waste into a resource for An example are initiatives like the Digital Watermarks HolyGrail
high-value applications.[22] Polymers, virgin or circular, are used 2.0 which can simplify the sorting of end-of-life waste materials
for their performance. Novel approaches need to be rigorously and thus contribute to higher recycling quotas. The digital water-
analyzed in a comprehensive way, for economic, societal, and en- marks are the size of a post stamp but invisible to the human eye.
vironmental impacts, for example, by life cycle analyses (LCA). They include various information such as of the manufacturer,
Such thinking should guide our perspective on recycling (and de- material composition, and food or non-food application. This in-
sign for recycling [DfR]) in this contribution. formation can be analyzed by a high-resolution camera during
sorting. A successful validation of the first detection sorting unit
2. Sorting and Cleaning was already achieved for packaging waste. More than 120 com-
panies and organizations across the value chain of the packaging
2.1. Advances in Sorting Technologies industry are part of the initiative.[37]
Tracer based sorting, on the other hand, is based on using
Efficient and correct sorting can turn mixed plastic wastes which markers that are added to the polymers in very low concentra-
would otherwise be only suitable for combustion into high-value tions. Here, fluorescence markers based on perylene dyes,[38] or
resources. It most directly contributes to better availability of up-conversion based markers [39,40] are of special interest.
waste input for recycling as well as their quality. Sorting can be For all these sorting techniques, pre-treatment such as cutting
done on both product/object level (macro-sorting) and on shred- and cleaning is required, as for contaminated samples where the
ded plastic flakes (micro-sorting). While macro-sorting is often plastics’ surface is barely visible, no automated sorting is possi-
done manually or with the help of object recognition,[23] micro- ble.
sorting needs automated classification. Near-infrared (NIR) spec-
troscopy is the technique that is commonly used to distinguish
different plastic materials. NIR spectroscopy has been available 2.2. Cleaning and Pre-Treatment
for high-speed sorting lines to distinguish different polymer
streams for some years, but a series of improvements keep push- Cleaning plays a key role for all recycling technologies. It can im-
ing the boundaries for sorting. In addition, the company Tri- prove sorting and remove adhering contamination from use be-
namix has developed hand-held devices where a sample can be fore it is incorporated into the material during further process-
directly scanned on site to determine the polymer type and cor- ing, including possibly odor-bearing or harmful contaminants.
rect assignment to recycling streams [24,25] before entering mixed Equally, treatment of the resulting wastewater is crucial for an
streams, or for spot checks and process control. Even structurally efficient recycling process. Cleaning agents and processing aids
similar polymers, such as PA6 and PA66 or HDPE and LDPE are necessary in several process steps, for example, for washing,
can be distinguished with this technique. For automated sort- floating, and rinsing before a certain plastic can then be re-used.
ing, such advanced spectral analysis capabilities are a promising Today, this already is of special importance in the PET recycling
Figure 5. Overview of different recycling approaches that are based on physical processes and maintain the chemical polymer structure. a) Depicts
mechanical recycling by re-extrusion. b) A process using dissolution in suitable solvents.
process where a large volume of mechanically recyclable plastics rity and material quality of the input for remelting. A key prob-
is available. Standard washing procedures are done with water lem are components that are non-miscible in the majority matrix
containing caustic soda (NaOH) and a surfactant at elevated tem- in the melt.[14,45] They can create uncontrolled heterogeneities
perature (70–90 °C).[41] The effect of washing and drying of PET in the material, weaken the mechanical performance, and can
bottle scraps on certain adhering organic contaminants and cop- make processes like film blowing impossible, or deteriorate op-
per was investigated by Komolprasert et al.[42] For most organic tical appearance. Other contaminants include hazardous mate-
contaminants, the process was able to remove >99% of the initial rials, legacy additives that have been phased out or are banned
contamination. for specific use,[46] odor-bearing compounds, chemically active
New developments focus on a reduction of waste water and substances which, for example, catalyze polymer degradation,
energy consumptions by adding specific additives to the wash- or ingredients imparting undesired color. Therefore, technically
ing and subsequent wastewater treatment process. Also, special rather undemanding applications are still typical for many recy-
surfactants are available that can efficiently remove labels or glue clates. These include street posts, garbage cans, or wood substi-
from the plastic surface.[43] tutes in construction. High-value applications, on the other hand,
target closed-loop scenarios: in closed loops, the resulting recy-
3. Recycling Technologies clate is again used in the same application as the virgin material
before.
3.1. Maintaining the Polymer Structure To achieve this goal, mechanical recycling aims to improve re-
cyclate quality mainly by deliberate choice of the waste source
3.1.1. Mechanical Recycling and preprocessing. For sourcing, post-industrial waste is close to
ideal: well-defined materials from production residues, little to no
For thermoplastic polymers, which by volume constitute >75% contamination and no additional aging during the life cycle. Of
of all plastics used worldwide, melting and re-extrusion is the similar attractiveness are closed deposit systems, for example, as
most straight-forward way for recycling. In principle, reprocess- established for PET bottles in some countries.[19] Larger volumes,
ing uses the same machinery and workflows as for virgin plas- however, are still available in mixed waste streams. Preprocessing
tics conversion. Such mechanical recycling[44] (Figure 5a) pro- includes sorting, shredding, washing, and re-sorting steps. There
vides the bulk of all recycled polymeric materials today. Being are trade-offs to be considered: Shredding to smaller sizes, for ex-
a physical process, the polymer structure remains (largely) un- ample, makes washing more effective, but complicates sorting.
changed. However, the thermal stress of reprocessing adds to Selective sorting to increase quality inevitably decreases the yield
any damage to the molecular chains that the material already of the entire process or requires separate treatment of the dif-
has experienced due to aging: by its initial processing, oxidative ferent sorted fractions. During the process, recent developments
stress during use, UV exposure, or other factors. The quality of target further measures to improve purity and quality. Krauss
mechanical recycling outputs is directly dependent on the pu- Maffei combines two twin-screw extruders in their Edelweiss
technology,[47] where the first extruder can be used for moisture

removal and deodorization. During re-extrusion, melt-filtration
can be applied. Adding extraction agents like PEG,[48] applying
hot air or steam stripping together with degassing of the melt
has also been shown by researchers to remove volatile contami-
nants and some odor-bearing substances. Similarly, supercritical
CO2 extraction has been proposed, as it can be applied directly in
an extrusion step.
A specific purity challenge for mechanical recycling is to gen-
erate recyclates that can be used in food contact applications. In
those applications, strict rules for the composition of virgin ma-
terials are enforced, together with limits on possible migration of
substances into food, for example, in the European Union.[49] For
recycling processes, the input is also regulated to be from >95%
food-grade material. EU regulation EC No 282/2008 requires for
a safe process either: i) controlled closed loop schemes (as real-
ized, for example, for PET bottles); or ii) the scientific demonstra-
tion by challenge tests to prove the capabilities of a process to re-
move any possible contaminations from less controlled sources,
like sorting fractions out of mixed post-consumer wastes, which
need to be quality controlled and certified. The FDA has issued
similar guidelines.[50] Studies could show that mechanical PET
recycling with a subsequent solid-state polymerization step was Figure 6. a) Polymeric materials experience damage during their life cy-
capable of removing all model contaminants in challenge stud- cles. In mechanical recycling, such degraded polymer chains enter the cir-
ies between >90% and >99%, to achieve safe levels.[51] In an- cular value chain and typically downgrade material performance and pro-
other case, mechanical recycling of HDPE bottles was analyzed: cessability. b) Oxidative damage as measured by the carbonyl index,[54] a
Pre-sorted HDPE consumer waste milk bottles from the UK ratio of C═O versus aliphatic absorption bands in IR spectroscopy, show-
were manually and automatically re-sorted, ground, washed, and ing the nonlinear, accelerated aging of a mechanical recyclate due to the
pre-damaged material input. (Source: BASF)
dried, steam and gas stripped followed by re-extrusion under vac-
uum. While low-Mw model contaminants (such as toluene and
chlorobenzene) had been removed here as well with an efficiency hindered amines or phosphites, light stabilizers, UV absorbers,
of >99%, other surrogates showed markedly lower decontamina- and others. Plastic additive suppliers have put an increasing fo-
tion efficiencies, for example, well below 50% for benzyl salicylate cus on this aspect of mechanical recycling: Clariant, for example,
or methyl palmitate.[52] This highlights some of the challenges has introduced specific Additives with a “Circle” designation,[57]
for food-grade mechanical recycling, and calls for further devel- or Altana the brand RecycloByk.[55] BASF created the IrgaCycle
opments in waste management, sorting, sampling, analytics, and range of additive solutions,[55] with new blends that are tailored to
quality control as well as decontamination technologies. the needs of mechanical recycling and optimizing recyclate value.
Relying solely on physical reprocessing through the melt One example is the recycling of PP from post-consumer—
phase, mechanical recycling is dependent on feedstock quality. collected automotive battery cases, which are aged, contain par-
However, even pure EoL materials come with a history of use tially oxidized polymer chain fragments and additional acidic or
that has left traces in the molecular structure of the macro- metal ion contaminants. To mimic long term stability require-
molecules: Heat, chemical, and (UV) radiation induced stress ments, recyclate out of this input was reprocessed by injection
lead to degradation[53] and loss of molecular weight (Figure 6). molding into 2 mm plaques and aged in an oven at 140 °C. With-
Additives and stabilizers that had been added to the virgin mate- out restabilization, the tensile impact strength retained already
rial can be used up from the first service life, and recyclates are drops to only 10% after 6 weeks, whereas added optimized sta-
very likely to already show significant oxidation as well as have ac- bilizers maintain performance even after 12 weeks at the initial
quired impurities that further catalyze future oxidative damage. level (Figure 8a). The same effect is seen for process stabilization:
Because the oxidation reaction is a chain reaction, pre-damage without restabilization, reprocessing quickly degrades molecu-
promotes further degradation. All of this hinders the processabil- lar weight, as witnessed by a reduction in viscosity. In the re-
ity of recyclates, reduces their mechanical performance, severely stabilized case, the recyclate maintains high molecular weight
limits long term thermal stability and weatherability (Figure 5b), during 60 min of simulated reprocessing, and thus its material
leads to discoloration, or accelerated molecular decomposition value (Figure 8b). Similar effects have also been shown for other
during the next product life, which can yield leachable or volatile additives and polymer systems.[56]
degradation products and impart odor. For some polymers, such as PET, bifunctional reactive
For high quality recyclates, additives are needed.[55,56] Appro- molecules can be added as chain extenders for mechanical
priate stabilization allows to control the underlying autoxidation recycling.[14,56] They allow reaction between end-groups of
cycles (Figure 7). As for virgin materials, an effective combina- oligomers or polymer chains, lead to a build-up of molecular
tion of different types of additives is employed: Primary antiox- weight, and restore or improve mechanical properties. Another
idants (AOs) such as phenolic compounds, secondary AOs like class of additives, compatibilizers,[14] address impurities of
Figure 7. The role of additives in stabilizing polymers in mechanical recycling during processing as well as re-stabilizing for their new product life.
Figure 8. Experimental data on accelerated aging of recyclates from post-consumer pre-damaged PP from battery cases. a) The retained tensile impact
strength is shown for two different levels of added re-stabilization with IrgaCycle PS 032 G, for the initial state (equals 100%) and oven aging at 140 °C
after 6 and 12 weeks. b) Similarly, recyclate processing was simulated for up to 60 min in a Brabender mixer at 210 °C and the torque measured as an
indicator for melt viscosity and hence molecular weight retention. Shown are curves for PP recyclate without and with 0.5% renewed additive addition.
(Source: BASF)
immiscible polymer components[58] when they exceed pos- has been shown that in up to a few percent of PA such materials
sible (thermodynamic) miscibility or (practical) compatibility are already compatible with high-value film-to film mechanical
thresholds.[45] PA, for example, is generally considered a contam- recycling in the PE stream, this can also be achieved for higher
inant in PE streams, leading to the classification of typical PE/PA amounts of PA by using appropriate compatibilizers,[59] for
multilayer barrier packaging films as non-recyclable. While it example, anhydride modified polyethylene derivatives such as
Figure 9. Dissolution–precipitation method for mixed and contaminated waste including solvent recycling.
Fusabond E226 by Dow Inc. In this case, compatibilization is and needs to be addressed similarly as in the mechanical recy-
based on a modified version of the majority polymer which offers cling process described above. A drawback of solvent-based recy-
reactive sites for the minority polymer components to covalently cling is the high energy cost associated with solvent recovery and
bind, such as amide end-groups of the PA to, for example, maleic the need for complete solvent removal from the target polymer.
acid anhydride moieties. In recent research activities, block-co- Also, the identification of environmentally-friendly and non-toxic
polymers from novel synthetic approaches that combine struc- solvents or solvent mixtures needs to be addressed; computa-
tural features of relevant polymer phases occurring in plastic tional methods can help here.[65] Polystyrene (PS) is one example
waste have been demonstrated as highly effective compatibiliz- where solvent-based recycling has been researched intensively
ers. Exemplarily, technology developed at the University of War- and where commercial processes are available, for example, by
wick, UK, allowed creating olefinic copolymers with, for example, Fraunhofer (CreaSolv technology), Polystyvert,[66] or Recycling
acrylates or vinyl esters.[60] Similarly, work on PE/PP block-co- Avenue.[67] Here, the removal of toxic brominated flame retar-
polymers[61] at Cornell University, USA has led to the creation of dants (BFR) plays an important role and levels below 1000 ppm
the startup Intermix Polymer Systems. can be achieved.[68] A pilot scale example is the PSLoop plant with
Together with advances in sorting, pretreatment, and process- 3.3 kt/a which uses the Creasolv technology to recycle PS foam
ing, additive technologies will be key to unlocking high value or rigid waste streams which contain the hazardous substance
applications. Mechanical recycling has comparably low energy hexabromocyclododecane (HBCD), introduced in the past as ef-
intensity due to the small loop size, is already operating at fective flame-retardant additive for PS-based insulation for build-
scale and a prioritized EoL option, within the limits of polymer ings. In subsequent steps the PS foam is dissolved, solid impuri-
chain degradation and contamination that are still being pushed ties are separated by filtration, then an additional solvent is added
further. which transforms the PS into a gel, while the bromine containing
impurities are separated with the liquid. Elemental bromine can
be recovered on top of the purified polystyrene which is re-used as
3.1.2. Solvent-Based Recycling granulated polymer.[69] Other commercial processes are available
for polyolefins, and the separation of multilayer films, such as
For mixed and contaminated waste streams where direct re- APK who focus on the recovery of LDPE and PA[70] or Sulayr who
processing in the melt leads to deteriorated properties or haz- target the separation of PE and PET from multilayer films.[71] The
ardous additives cannot be eliminated, solvent-based recycling solvent-based method has been shown to work well for relatively
(Figure 5b) is a viable option. Here, the polymer structure is re- simple multilayer films with one or two targeted components
tained, too (in a purely physical process), however other polymers that can be recovered. More complex films with multiple differ-
and impurities can be separated from the target polymer.[62,63] ent layers[72] are likely more challenging. In some cases, certain
The separation process is based on a selective dissolution of the current multilayer laminates might even only be recycled chem-
target polymer in a specific solvent. Insoluble impurities, addi- ically. Design-for-recycling approaches (see Section 3) play a key
tives, and other polymers are mechanically separated (e.g., by role to improve recyclability.
filtration) to produce a purified polymer that is recovered from As mentioned above, efficient solvent recovery and recycling
solvent by precipitation. Precipitation can be induced, for exam- is crucial for these solvent-based processes. The energy costs as-
ple, by using an anti-solvent, fast solvent evaporation, or cooling sociated with the dissolution process and the solvent recovery by
down. Solvent treatment and recirculation create a closed-loop distillation, or separation of solvents if an anti-solvent is used,
recycling process in which mixed plastic waste can be recycled are the main costs of the process and also lead to CO2 emissions.
sustainably and high quality recyclates are recovered. Figure 9 Therefore, the amount of solvent used in the process must be
shows a schematic depiction of the process. minimized, and a detailed LCA of the entire process needs to be
The properties of the recycled polymer are expected to be com- considered to ensure that the respective solvent/polymer system
parable with the virgin product,[64] however a lowering of the av- is the right choice for getting a high quality recyclate with a low
erage molecular weight in the drying process might be observed CO2 footprint.
Figure 10. Overview of different recycling approaches that are based on reactive, chemical processes, and change the chemical structure of the polymers:
a) Remonomerization or b) conversion of polymeric input into basic chemical building blocks as feedstock for the chemical industry.
3.2. Chemical Recycling ent solvolysis techniques (shown in Figure 11), such as hydroly-
sis, the reaction with water to obtain terephthalic acid (TPA) and
Chemical recycling, which means the destruction of the polymer ethylene glycol (EG), methanolysis, the reaction with methanol
structure, is used if waste streams are too mixed or contaminated to obtain dimethyl terephthalate (DMT) and EG, or glycolysis,
for mechanical recycling, or if virgin-like quality of the recyclate the reaction with EG to obtain bis-HET, are used, which in turn
polymer is needed. However, the energy consumed by the chem- yield different products that can either be directly used in re-
ical process is generally higher than for mechanical recycling, polymerization or are further reacted to the monomers TPA and
therefore mechanical recycling should be used whenever and, EG.
considering polymer degradation over cycles, as long as possi- These reactions are usually carried out at elevated temperature
ble. Still, especially for waste streams that were previously only and pressure. On top of the reaction process, several purification
energetically valorized by combustion, chemical recycling is an steps are necessary to remove impurities, additives, or colorants
invaluable method to use plastic waste as a raw material source and obtain the purified and separate monomers. Examples for
and achieve a zero plastic waste goal. pilot scale or commercial processes include Eastman and Loop
Chemical recycling can be divided into two subgroups, first Industries who use methanolysis, Gr3n and INEOS who use hy-
re-monomerization processes (Figure 10a), where the polymer is drolysis, and Ioniqa, Jeplan, SABIC, and perPETual who use gly-
recycled into its constituent monomers that can then be polymer- colysis. For these processes both bottles/packaging and textiles
ized again, or high-temperature conversions such as pyrolysis have been used as the main feedstock material. Eastman recently
and gasification, where a mixture of smaller molecular fragments announced to start production in 2023 with a scale of 110 kt/a
is obtained (Figure 10b). In general, re-monomerization is used of post-consumer and post-industrial waste, which demonstrates
for polycondensation polymers that can be readily depolymerized that there is a huge market for PET depolymerization. Moreover,
by solvolysis processes whereas a process to obtain pyrolysis oil enzymatic processes for depolymerization enable hydrolysis at
is better applicable for polymers which contain less heteroatoms, low temperatures.[73,74] This is also possible by using metal oxide
especially polyolefins. The commercial success of all processes catalysts and UV light as the Swiss start-up Depoly has shown.[75]
described below depends largely on costs and availability of se- Current developments for most processes focus on optimization
lected waste streams, and also on political regulations that make of catalyst re-use and recovery, and also the purification steps that
recycling processes more attractive. are necessary to remove contaminants from the depolymerized
products in order to have a depolymerization process with a low
environmental impact.[76]
3.2.1. Re-Monomerization by Solvolysis Polyurethanes (PU) exist in many different forms with a wide
range of properties, for example, from extremely flexible to ex-
For depolymerization technologies of polycondensation type tremely rigid. Usually, the polyol component is varied to obtain
polymers, polyethylene terephthalate (PET) is the most inten- the desired properties. Therefore, a pre-sorting or a selection
sively investigated polymer due to its large volumes. Here, differ- of a specific waste-stream is often necessary to obtain a more
Figure 11. Main depolymerization pathways for PET: hydrolysis, methanolysis, and glycolysis, yielding the respective products shown above, and ethylene
glycol for all routes.
Figure 13. Split-phase glycolysis of polyurethanes.
adipic acid (AA) and hexamethylene diamine (HMD), and there-

fore needs more elaborate separation processes. On a commer-
cial scale, Aquafil uses an acidic hydrolysis at high pressures to
obtain virgin-quality caprolactam which is then re-polymerized
Figure 12. Mattress made from recycled polyol; flasks contain shredded and sold as ECONYL fiber. As waste streams, old fishing nets
mattress sample (right) and recycled polyols (left).[79]
and textiles are used, which provide a source of relatively clean
PA. The yearly production is about 25 kt.
specified waste input which can then yield the required poly-
ols. So far, recycling quotas for polyurethanes have been low due
to their variety in application. Therefore, several companies and 3.2.2. Re-Monomerization by Pyrolysis
consortia have recently focused on progress in PU depolymeriza-
tion technologies, such as the EU funded projects PolynSPIRE[77] From a thermodynamic point of view, polymerization reactions
and PUResmart.[78] BASF has recently demonstrated the foam- equilibria can be shifted via the temperature. For a lot of common
ing of a new mattress with polyols recovered from old mattresses polymers, for example, polyethylene or polypropylene, the poly-
(see Figure 12).[79] For these chemical recycling routes, glycolysis merization is highly exothermic and thus thermal depolymer-
is the most widely used process. The reason for this is the gly- ization arguably difficult.[81] Other addition polymers, like poly-
cols having a relatively high boiling point, therefore no pressure methyl methacrylate (PMMA) and polystyrene (PS), can be de-
needs to be applied for reactions at elevated temperatures (usu- polymerized in a thermochemical process.[22] PMMA can be re-
ally in the range 160–250 °C). verted back to its MMA monomer at temperatures ≈400–500 °C
Usually diethylene glycol (DEG) is used as solvolysis agent. If a in the absence of oxygen. Different process technologies such as
large excess of glycol is used, the reaction mixture splits into two fluidized bed, molten metal bath, or use of a twin-screw extruder
phases, where the lower layer contains the glycol and the remain- exist. An example of recent development is the MMAtwo project
ing PU hard phase, while the upper layer contains the recovered funded by the EU where the goal is to recycle 27 kt/a of PMMA
polyols (see Figure 13). Thus, the polyols can be separated and EoL products. Depolymerization to a high-quality MMA product
worked up in the next step, for example, with an extraction pro- (purity 99.8%) with a yield of 64–85 wt% has been achieved on a
cess. pilot level with twin-screw extruder technology.[82]
Re-monomerization of polyamides can also be done by solvol- Polystyrene cracking is mainly done in a fluidized bed re-
ysis processes like hydrolysis.[80] Polyamide 6 is more straightfor- actor to obtain its monomer styrene and other decomposition
ward to recycle as it is made from only one raw material, capro- products. Agilyx has developed a commercial process based on
lactam, while polyamide 66 is derived from two raw materials, thermal pyrolysis and collaborates with several PS producing
companies (such as INEOS and Trinseo) to expand recycling of value chains,[11] there is very likely a role to play for all the differ-
PS post-consumer products. ent approaches in chemical recycling. The relative contributions
are still to be determined. For zero net GHG emissions, high tem-
perature processes either need to be electrically heated by green
3.2.3. Pyrolysis and Gasification electricity in the future, or will need carbon-capture and storage
or utilization (CCS, CCU) if a fraction of the input is incinerated
If none of the above-described recycling techniques is applica- for process heat generation, or offsetting via biomass input.[11]
ble to a waste stream, thermochemical processes can be used Another important lever to lower the energy needs of chemi-
that provide a mix of short-chain hydrocarbons or gases as prod- cal recycling approaches could be catalysis, as has been pointed
uct which can be re-fed into the polymer production cycle at an out in specific examples throughout the previous sections. The
earlier stage than in the case of monomer recycling. Two main specific opportunities and challenges in conjunction with plastics
techniques exist: pyrolysis, which is carried out at temperatures waste feedstocks have recently been highlighted from a catalysis
above 300 °C under the exclusion of oxygen, and gasification, perspective[85–87] and open up many development options.[81,88,89]
where controlled amounts of oxygen or water steam are added Main challenges in using catalysts are potentially the high costs
at temperatures between 700 and 1600 °C. For both processes it and poisoning of the catalysts by unknown by-products in the
is possible to use mixed and contaminated plastic waste, however waste material and, in many process implementations, the nec-
the nature and amount of heteroatoms in the plastics determines essary separation from the recycled product.
the level of possible corrosion in the plants and how tedious fur- To find out which recycling process should be used for which
ther cleaning steps of the product streams are. In the pyrolysis waste stream a detailed LCA[90] needs to be considered. This can
process, a mix of short-chain hydrocarbons (pyrolysis oil) and sometimes even yield surprising results, for example for com-
gases is obtained, but mainly the oil can be re-used, after fur- modity plastics pyrolysis or gasification has been claimed to out-
ther processing to remove heteroatom-containing components. perform mechanical recycling as a high sorting effort is needed
Therefore, polymers without heteroatoms, such as polyolefins, in the latter case and therefore a high amount of material today
EPDM, or rubbers, provide the ideal feedstock for pyrolysis. ends up in incineration (energy recovery).[90] However, this de-
The products obtained in gasification are even smaller chem- pends strongly on the quality of the incoming material stream,
ical building blocks, mainly CO and hydrogen. These gases also the quality requirements of the recycled product, and the consid-
need to be cleaned before re-use in synthetical routes. Gasifica- eration of offsets due to the specific energy recovery situation. For
tion means a partial oxidation of the feedstock due to less oxygen engineering and high-performance plastics (shown in Figure 3 in
being added than in combustion processes. The big advantage of the upper half of the pyramid) sorting often is highly beneficial: it
gasification is the broadest acceptance of feedstocks[83] and tol- reduces environmental impact of the polymer waste significantly
erance of heteroatoms, making it an option for otherwise non- if thus mechanical or depolymerization technologies can be used
processable residues from smaller loop recycling schemes. His- to provide recycled polymer for similar applications as the virgin
torically used for coal, and recently pursued for biomass, gasifica- one. This shows that a detailed LCA might sometimes challenge
tion for plastics still also encounters specific process challenges, the current recycling hierarchy which prefers smaller loops as
for example, related to its low thermal conductivity or the stick- shown in Figure 14 and described above.
yness of plastics residues during heating.[83] Due to the nature
of the gaseous products, gasification also needs to be directly 4. Design for Recycling
collocated with an integrated chemical production site at scales
that need significant investments. Upgrading existing coal-based As discussed earlier (see, e.g., Figure 4), the key factor for any re-
gasifiers is a smaller hurdle: Eastman Chemicals has announced cycling process is access to suitable, clean enough plastic waste
to upgrade their gasification capabilities at the Kingsport, Ten- as feedstock, at scale and at commercially viable cost levels. The
nessee site in the U.S. to co-feed mixed plastics waste. They state availability of such streams is directly dependent on the way poly-
that using gasification for the otherwise hard-to-recycle plastic meric materials are used. By deliberate design choices before in-
they obtain molecules with 20–50% reduced GHG emissions ver- troduction of products or, for example, packaging formats, high
sus via syngas produced conventionally from coal.[84] value uses at EoL can greatly be facilitated. This is what DfR is
Chemical recycling that regenerates and purifies building aiming at.[91] One obvious prerequisite is to avoid introducing
blocks, monomers, or even feedstock has the big advantage of substances or components into EoL streams that harm future
no loss of quality in the resulting recycled polymeric materi- use. Examples of such hurdles today based on design choices
als and a capability to quantitatively remove unwanted contam- in the past include, for example, problematic legacy flame retar-
ination. Being identical in chemical composition, new polymers dants like HBCD[46] from PS insulation foams that now severely
from such recycled feedstock show exactly the same performance complicate waste collection and contaminate recycling.[92] This
and characteristics as virgin grade material, and can be used in is, on the one hand, the result of advancing knowledge on the
all applications, including, for example, food contact. As initially hazard of such substances in the time span between production
stated, their commercial viability will depend on the cost, for ex- and EoL, which is especially long in the construction industry
ample, of purified pyrolysis oil versus fossil-derived naphtha, de- in this specific case. On the other hand, the design process it-
tails of regulatory acceptance, CO2 pricing, and economic instru- self, which in the linear economy focuses on performance and
ments to incentivize recycled over virgin plastics. For a circular price, in the past has only rarely considered EoL design objec-
economy of plastics, that in addition to eliminating waste also tives. Such design objectives depend on the waste collection and
supports the transformation to carbon neutrality for the plastics processing scenarios. Designing for a product-specific take-back
Figure 14. Different pathways for plastics recycling in a circular economy. In general, the smaller the circle, the less energy is consumed in the recycling
process, and the easier it is to reach GHG emission neutrality in this loop. While this paper focuses on the technical cycle, the biological cycle based on
renewable resources and compostable plastics is also a way to achieve a circular economy.[13] (Reproduced with permission of BASF SE).
would be used. However, lacking critical barrier properties, for ex-

ample, for oxygen or lacking mechanical strength, either much
higher film thicknesses and as such polymer amounts have to
be used, or alternative barriers must be applied that do not add
a significant share of foreign material, for example, by gas-phase
deposited inorganic thin films. Alternatively, well-recyclable high
barrier polymers such as PA6 could be used exclusively for a
complete construct in some applications, but likely impose other
compromises, such as cost or loss of properties in other perfor-
mance dimensions. Reaching sufficient performance always re-
Figure 15. Conceptual sketch of different design-for-recycling approaches
mains critical and besides improved recyclability, low weight, and
following a monomaterial strategy on the systems level, using a simplified
multilayer barrier (packaging) film as an example. highly efficient protection of perishable ingredients such as food,
need to be optimized jointly in a life-cycle assessment to address
sustainability.[95] Designing for full recyclability in the polyolefin
scheme allows different choices than having to assume intro- stream can also be addressed by restricting other materials to stay
duction into a general mixed-waste stream. A general avoidance within practical or theoretical compatibility limits described in
of potentially hazardous substances in materials or products, guidelines,[96,97] or potentially by already incorporating compat-
which is at the core of “Safe and Sustainable by Design” (SSbD) ibilizer additives in respective laminates needed for their high
approaches,[93] in this respect also directly supports DfR, or a value mechanical recycling.[59]
more comprehensive “Safe, Sustainable and Recyclable by De- As an alternative to monomaterial designs, laminates or as-
sign” (SSRbD) paradigm. Recent regulatory developments, such semblies of different materials can be converted into monoma-
as in the European Union the “Green Deal” with the included terials if they can be disjoined (Figure 15) by a selective trigger
Chemical Sustainability Strategy,[69] are pushing for a “toxic-free” during pre-treatment. Debonding-on-demand adhesives[98] are
environment, which in the longer term also should limit future such an enabling technology, that could provide a way out of con-
surprises by hazardous materials in EoL streams. flicting performance—recyclability design spaces, for example in
Another general guideline for DfR is to reduce material multilayer laminates for packaging: pure films are obtained, if
complexity on the systems level, where possible: in all above- the laminating adhesive de-bonds in a controlled way,[99] ideally
mentioned recycling processes, impurities of specific incompat- in a process step that is already available, or only needs small
ible materials hinder recycling, increase processing efforts, and adaptations in the current workflow, for example, during wash-
thus cost and/or potentially deteriorate recyclate quality. One ap- ing/pretreatment (see section 2.2).
proach is to follow “monomaterial” concepts (Figure 15). Multi- The concept of monomaterial design is not restricted to the
layer packaging films today are hard to recycle.[94] Typically, they packaging sector. In the sports footwear space, Adidas has show-
consist of polyolefin base materials co-laminated with a barrier cased the FUTURECRAFT.LOOP,[100] a running shoe where all
film and, for example, an outer PET-based decorative layer.[95] parts are made from TPU (outer sole, midsole, knitted textiles).
In a monomaterial packaging instead, a single polyolefin film Adhesives are not needed, because the thermoplastic material
can be thermally fused. Whole shoes can be recycled into new sibility of circular feedstocks while maintaining necessary per-
TPU components for new shoes at EoL. Such approaches are formance. The likely dependence of new circular polymers on
likely to be emerging for other materials as well, especially poly- non-technical circumstances such as business model innovation
mers which have been shown to be amenable for high quality points to the importance of additional enablers. One key area for
recycling. The ability to remove foreign materials (including dirt circular economy and sustainable chemistry is digitalization.[110]
from the use phase or pigments from colored design elements) Digital platforms can help to create a marketplace for recycled
will likely be important to sustain multiple loops in high-quality materials, making material availabilities and qualities transpar-
applications. Pure PET, PA6 but also PLA[101] with “dual” loops ent. To this end, there are activities by startups (e.g., EME – Excess
both for mechanical recycling and depolymerization (as well as Materials Exchange from The Netherlands, MikaCycle in France
alternative composting under limited circumstances in the case or Scrapo in the U.S.) and publicly funded projects, for example,
of PLA) could be candidates. Reuse of polymers themselves or DiLink[111] supported by the German Federal Ministry of Educa-
their building blocks could even shift the economics and total tion and Research. Similarly, transparency along the value chain
CO2 -emission intensity in favor of easily recyclable, but initially is enabled by digitalization, to track components of products, in-
more expensive and potentially more energy intensively pro- formation about the composition, and specification of materials
duced polymeric materials. This is also a rationale for molecular as well as recycled content in the next life cycle. Without the need
DfR, envisioning new inherently circular polymers that replicate for a central authority, blockchain technology has been proposed,
the performance of incumbent ones but with built-in abilities for example in the BASF pilot project reciChain in Brazil and
for reuse of the building blocks.[81] Several recent examples have Canada,[112] or by the Dutch startup Circularise together with a
been demonstrated: to replace PE, Häußler et al. propose poly- consortium of plastics producers like Covestro, Domo and Bo-
carbonate with octadecandiol-blocks (PC-18) or polyesters from realis and plastics users such as Arçelik or Porsche. With Cir-
octadecanoic diacid and octadecandiol (PE-18,18). PC-18 and PE- cularise´s solution, a recycler would be enabled to query criti-
18,18 are shown to have comparable properties to PE, to repli- cal parameters of incoming materials for high value recycling,
cate some key features of PE crystallinity, while allowing straightfor example, confirming absence of critical ingredients. A cus-
forward depolymerization by solvolysis.[102] In another example, tomer, on the other hand, might verify the recycled content of a
both crosslinked as well as thermoplastic PUs based on poly-𝜖- product. This approach likely works best with larger parts that
caprolactone (PCL) polyols have been explored by Magnin et al., can be disassembled and identified—the link between the digital
allowing controlled degradation via the PCL block by chemical representation and the physical part needs to be established via
or enzymatic hydrolysis. Degradation products are reassembled a unique part number, optical barcode, or embedded radio fre-
by condensation to second-generation PU.[103] Abel at al. demon- quency identification (RFID) tag to realize the full value. Alterna-
strate high Mw thermoplastic polyacetals such as poly(1,3 diox- tively, microscale or molecular barcoding and tracing technolo-
olane) that can reach tensile properties of isotactic PP. Depoly- gies could be highly synergistic to identify disintegrated parts,
merization of PDXL to the monomer has been demonstrated ideally even after shredding. Such solutions might be based on X-
at 140 °C in the presence of acid catalysts.[104] Helms et al. in- ray fluorescence,[113] optically fluorescent microparticles,[114] or
troduced poly-diketoenamines (PDK), based on the dynamic co- unique DNA labels.[115] More research is required to develop vi-
valent diketoenamine bond that allows recovery of the building able and robust enough adaptations for plastics circularity. In-
blocks (bis-triketones and aromatic or aliphatic polyamines). The dependent of technical implementation, the general value of at-
challenging economics of new polymers without existing value taching information to products to facilitate repair, reuse, and
chains, and based on synthetically more complex building blocks, recycling at EoL is also recognized by regulators: The European
have been explored by Vora et al. explicitly for the PDK exam- Union (EU), for example, is pushing within the EU Green Deal
ple: while not viable at all in a linear economy, with an estimated and the Circular Economy Action Plan for a digital product pass-
minimum selling price (MSP) for PDK resin of 45 $/kg and es- port (DPP).[116] Intimately connected with any digital representa-
timated life cycle GHG emissions of 86 kg CO2 /kg, the circular tion of a physical stream for recycling is the need to analyze the
PDK resin, due to the ease of recycling and based on the regen- composition and quality, as a data source for the “digital twin” or
erated monomers, could become competitive to existing mate- simply for quality control and quality assurance. Recycling, with
rials at 1.5 $/kg and with only 1.8 kg CO2 /kg life cycle GHG the heterogeneity of waste streams at different length scales, as
emissions.[105] From an industrial perspective, this highlights the well as unknown potential contaminants, poses challenges for
challenges and opportunities of similar circular materials: With sampling (from the bulk scale of a pile of waste to lab scale),
their high embedded value, initial cost and capital bound in the and analytical chemistry (ensuring quantification of major com-
material stock is very high and has to be borne somewhere in ponents as well as detection of hazardous trace materials).[117] De-
the value chain, while at the same time the incentive for reuse velopment and validation of sampling methods, improved char-
is equally high. This might require as much innovation in cir- acterization methods that can assess quality-relevant parameters
cular economy business models[106–108] as further technical de- such as aging, as well as respective standards for input and output
velopments, possibly including seemingly visionary, for example, quality in recycling will be decisive to scaling high-value recyclate
“rental materials” or leasing approaches.[109] applications, independent of the recycling route.[117]
5. Enabling a Plastics Circular Economy 6. Conclusions

In the previous sections, we have highlighted the progress of re- Emerging technologies enable us to recycle an increasing share
cycling technologies themselves, as well as DfR to improve acces- of plastic waste into high-value applications, for example, in a
Figure 16. Schematic summary of recycling technology options for closed-loop recycling back to high value products. The various types of plastics
introduced in the polymer pyramid in Figure 3 are accessible for different technologies discussed in this paper. A hierarchy of the recycling methods
is sketched, indicating a preference for methods with lowest energy-consumption and highest chemical structural value preservation, as long as the
necessary performance for high value applications can be met. Virgin-equivalent quality can be achieved with chemical recycling approaches, like re-
monomerization or thermochemical conversion to feedstock via pyrolysis or gasification.
closed loop back into the same application as in the first life. important that regulators define recycling technology-neutral to
Intrinsic polymer degradation through repeated processing and include different sustainable recycling technologies, evaluated,
aging, as well as inevitable extrinsic heterogeneity and contami- for example, via LCA. The set-up of extended producer respon-
nations in the waste feedstocks are the fundamental challenges, sibility systems can further promote collecting plastic wastes in
as both directly compromise performance and application value. sufficient volumes and quality to enable efficient recycling pro-
For engineering plastics defined by their specific performance, cesses. Such regulatory developments, the dynamics of techno-
any property losses directly question their applicability. Perfor- logical progress as well as the intrinsic link of circularity and
mance plastics, with higher price points and typically higher CO2 greenhouse gas emission neutrality will keep shaping the plas-
burdens from virgin production, as well as smaller volumes, tics industry.
on the other hand offer a potential value proposition for more
complex recycling technologies compared to commodity plastics.
Waste availability and purity are the key factors dominating eco- Acknowledgements
nomics. Both are directly addressed by improved sorting, DfR,
and new circular business models. Enabling technologies such H.M. and B.v.V. contributed equally to this article. The authors thank K.
Wittstock, A. Stammer, J. Hamprecht, C. Seitz, C. Krüger, G. Türkoglu, O.
as additives, debonding on demand, improved melt processing Reich, H. Herbst, M. Bender, and S. Schunk for valuable input and com-
in mechanical recycling, but also advances in chemical recycling ments, as well as the very helpful anonymous reviewers.
are necessary to avoid property degradation. New polymer types
can offer advantages at EoL but face high barriers for market in-
troduction. The digital transformation of the recycling chain will
Conflict of Interest
support further progress towards plastics circularity. A true trans-
formation for circularity for all plastics, including engineering The authors declare no conflict of interest.
materials, will require collaboration across the value chain, from
feedstock provision, material production, application, and use—
and finally return in an as controlled a way as possible. Regulatory Keywords
support will be required to make landfilling and incineration of
circular economy, design for recycling, engineering plastics, plastics, recy-
plastic waste unattractive and to promote plastics recycling. Also,
cling, sustainability
political mandates for recycled content of plastics can help in-
crease market demand for recycling. Mechanical and chemical Received: December 14, 2021
recycling technologies are complementary in many aspects and Revised: February 10, 2022
will jointly contribute to reaching ambitious targets for plastics Published online: March 4, 2022
circularity, especially for high value applications (Figure 16). It is
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Hannah Mangold studied chemistry at Freiburg University, Germany, and completed her Ph.D. at
the Max Planck Institute for Polymer Research in Mainz on the topic of organic photovoltaics. She
joined BASF R&D in 2014 and has been working in diverse fields such as photophysics of luminescent
materials, as well as product development for display materials in the corresponding business unit.
She is now a team leader in process research and chemical engineering, where her focus is on polymer
recycling.
Bernhard von Vacano studied chemistry and physics as an elective subject, in Tübingen (Germany),
at the University of Wales in Bangor (UK), the Max-Planck Institute for Quantum Optics in Garching
(Germany) and received his Ph.D. in physical chemistry from Marburg University (Germany). Having
joined BASF in 2008 in the company´s polymer physics department, he has since held various posi-
tions in R&D and is currently a senior research fellow in the area of advanced materials, responsible for
global technology scouting, strategic university collaborations, and a program for sustainable materi-
als and circular economy.

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PERSPECTIVE

The Frontier of Plastics Recycling: Rethinking Waste as a

plastics like polyurethane (PU) (see, e.g.,

technology,[47] where the ﬁrst extruder can be used for moisture

Figure 13. Split-phase glycolysis of polyurethanes.

adipic acid (AA) and hexamethylene diamine (HMD), and there-

would be used. However, lacking critical barrier properties, for ex-

5. Enabling a Plastics Circular Economy 6. Conclusions

[26] M. L. Henriksen, C. B. Karlsen, P. Klarskov, M. Hinge, Vib. Spectrosc.

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