Chemically Recyclable Thermoplastic Elastomers: Preparation, Properties, and On-Demand Depolymerization
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Chemically Recyclable Thermoplastic Elastomers: Preparation, Properties, and On-Demand Depolymerization
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  • Yingying Liu
    Yingying Liu
    State Key Laboratory of Advanced Optical Polymer and Manufacturing Technology, College of Chemical Engineering, Qingdao University of Science and Technology, Qingdao 266042, China
    More by Yingying Liu
  • Yong Shen*
    Yong Shen
    State Key Laboratory of Advanced Optical Polymer and Manufacturing Technology, College of Chemical Engineering, Qingdao University of Science and Technology, Qingdao 266042, China
    *Email: [email protected]
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    Orcidhttps://orcid.org/0000-0002-8624-2662
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Precision Chemistry

Cite this: Precis. Chem. 2026, XXXX, XXX, XXX-XXX
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https://doi.org/10.1021/prechem.5c00441
Published March 5, 2026

© 2026 The Authors. Co-published by University of Science and Technology of China and American Chemical Society. This publication is licensed under

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Abstract

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Great advancements have been achieved in the past decade for chemically recyclable polymers that can be selectively depolymerized back to their monomers to address the end-of-life issue of plastics. Nevertheless, the technologically important thermoplastic elastomers (TPEs) with on-demand depolymerization property have received less attention largely due to their intrinsically complicated multiblock architectures and challenges involved in the selective chemical recycling of different monomers. This review highlights the recent achievements of chemically recyclable TPEs by focusing on their preparation, mechanical properties, and on-demand depolymerization and recycling. A variety of TPEs are introduced according to their backbone, including copolyesters, polyurethanes, and polyolefins. The dynamically cross-linked elastomers with chemical recyclability are also briefly discussed. Finally, the current challenges and possible future directions for chemically recyclable TPEs are also addressed.

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© 2026 The Authors. Co-published by University of Science and Technology of China and American Chemical Society

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Published as part of Precision Chemistry special issue “Precision Chemistry for Polymer Recycling”.

1. Introduction

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Thermoplastic elastomers (TPEs) possess the good mechanical strength and high elasticity of traditional cross-linked vulcanized rubbers, as well as the ease of thermal molding and processing ability of thermoplastics. (1,2) They have been widely used in the automotive industry, electronic products, medical devices, sports equipment, clothing, footwear, and headwear, etc. (3,4) The global TPEs market size reached $26.86 billion in 2019, and is expected to continuously grow to $39.42 billion by 2027. (5) Generally, TPEs are block copolymers composed of glassy or semicrystalline blocks with a high glass transition temperature (Tg) or a melting point (Tm) and soft rubbery blocks with a Tg below ambient temperature. (6,7) By adjusting the compositions and molecular weights of the block copolymers, microphase separation occurs between the thermodynamically incompatible hard and soft segments. (8,9) The hard blocks, as physically cross-linking points, distribute within the continuous rubber matrix of soft blocks, thereby imparting the block copolymers with excellent mechanical strength and elasticity.
The commercially available TPEs are currently produced from petroleum feedstock, including styrenic block copolymers, polyolefin-based copolymers, block copolyesters, thermoplastic polyurethanes, and polyamide-based copolymers. (10,11) These TPEs are not degradable in nature due to their stable backbone and cause severe pollution if they are not properly treated after their service life. To address the growing concerns over resource and environment problems, great efforts have been devoted to developing sustainable TPEs from biosourced feedstock or biodegradable TPEs with cleavable backbones. Several excellent reviews have been published to summarize the recent progress in the biorenewable or biodegradable TPEs. (12−18) Despite the great successes of biodegradable TPEs, their degradation to CO2 and H2O cannot recover any material value and is economically undesirable. Recycling represents a more attractive strategy to create a circular plastics economy. TPEs can be mechanically recycled through thermal remolding or melt reprocessing due to their reversible cross-linking networks. However, their physical recycling faces challenges including complex, costly, and time-consuming sorting and purification processes and considerable performance deterioration after multiple reprocessing cycles due to chain scission, oxidation, or irreversible cross-linking. (19) As such, physical recycling is considered a “downcycling” strategy. The TPEs will reach their end-of-life stages after limited reprocessing cycles.
Compared to physical recycling, chemical recycling offers an additional opportunity to recover the material value when they are no longer suitable for mechanical reprocessing. Especially, chemically recyclable polymers have emerged as a research frontier, since they can be depolymerized back to their original monomers or converted to valuable chemicals under controlled conditions at the end of their service life. Great advancements have been achieved for the chemically recyclable polymers in the past decade, including polyesters, polythioesters, polycarbonates, polyamides, and other heterocyclic polymers. (20−23) Polyolefins that are prepared by ring-opening metathesis polymerization (ROMP) can also achieve chemical recycling. (24−26) However, most studies reported the design and preparation of thermoplastics; the technologically important TPEs with chemical recyclability have been largely underexplored. On the one hand, the intrinsically complicated multiblock architectures of TPEs require the sophisticated selection of different monomers to synthesize hard and soft segments. The thermal and mechanical properties of TPEs are greatly dependent on their compositions, topologies, monomer sequences, and molecular weights and dispersities. On the other hand, it is more challenging to achieve the chemical recycling of TPEs than thermoplastics, since two or more monomers need to be selectively and efficiently recovered.
Nevertheless, great efforts have been devoted to addressing the chemical recycling of TPEs. For example, several tri- or multiblock elastomers with intrinsic chemical recyclability have been developed based on ring-opening polymerization (ROP) or ROMP of cyclic monomers with near-equilibrium polymerization thermodynamics. These TPEs can undergo ring-closing depolymerization (RCD) under specific conditions to achieve the selective recovery of pristine monomers. (27−30) The recovered cyclic monomers are capable of repolymerization to offer TPEs with virgin performances, realizing a closed-loop life cycle of “polymer–monomer–polymer”. On the other hand, dynamically cross-linked elastomers introduce dynamic bonds to construct reversible cross-linking networks, such as imine and borate ester bonds, as well as coordination, hydrogen bonding, and ionic interactions. (31,32) This strategy not only maintains the physical reprocessing capability of the linear elastomers but also enhances their service performances, including high-temperature resistance, solvent resistance, mechanical strength, and elasticity. It is worth noting that dynamically cross-linked elastomers can also undergo depolymerization under specific conditions for chemical recycling.
In this review, we highlight the latest advancements in chemically recyclable TPEs. Different types of TPEs, including block copolyesters, thermoplastic polyurethanes, and polyolefin-like elastomers, are introduced by focusing on their preparation and on-demand chemical recycling. Following these sections, the preparation and properties of dynamically cross-linked elastomers are discussed with a particular emphasis on their chemical recycling. Finally, the current challenges and potential opportunities for the development of chemically recyclable TPEs are briefly addressed. Table 1 gives an overview of the reported chemically recyclable TPEs to better present the state of the art.
Table 1. Overview of the Reported Chemically Recyclable TPEs
TPEMna (kg/mol)fhard (%)Tgd (°C)Tmd (°C)E (MPa)eσb (MPa)eεb (%)eelastic recovery (%)frefs
PLLA-b-PδCL-b-PLLA90.90.33–35, 5715915.8 ± 3.120.4 ± 1.0956 ± 10591.8 (33,34)
PδVL-b-PαMeVL-b-PδVL104.60.41–516014.2 ± 0.914.9 ± 0.51061 ± 1196 (35)
PδVL-b-PβMVL-b-PδVL92.40.56–5542n.r.i39.4 ± 0.41986 ± 3696.3 (36)
PPDO-b-PβMVL-b-PPDO90.00.24–50.3, −17.680.4n.r.21.1 ± 0.51054 ± 4593.5 (37)
P(5C-TMC)-b-P(MePr-TMC) -b-P(5C-TMC)53.80.32n.r.n.r.n.r.11.7 ± 1.3472 ± 1187.3 (38)
PLLA-b-P(THF-co-CHO)-b-PLLA1090.58–78, 641780.21 ± 0.0116.0 ± 3.0277 ± 36n.r. (39)
P(CL2000-grad-SHPL500)121n.r.n.r.49,265157 ± 2.858.8 ± 4.01959 ± 5392 (40)
P[CL48-stat-(4Ph-BL)52]383n.r.n.r.n.r.31.3 ± 1.734.5 ± 3.6812 ± 4299.3g (41)
PβMVL-TPU102.20.40b–33n.r.7.2 ± 0.237 ± 31000 ± 2098.8h (42)
PδCL-TPU99.40.32b9.8n.r.6.0 ± 0.360.4 ± 2.6899 ± 697 (43,44)
PγBL-TPU70.10.15c–23n.r.n.r.18.3 ± 1.52298 ± 7595.9 (45)
PE4082.40.4c–50.610915 ± 112.0 ± 0.71030 ± 30n.r. (46)
rOBC7.7 (7.7 mol % of 1-octene)129.4n.r.–44.795.1n.r.24.8 ± 1.71950 ± 83n.r. (47)
polyolefin-like elastomer P4158.3n.r.–21411.9 ± 0.231.5 ± 3.11495 ± 28698 (48)
PE(v)-b-PTMC-b-PE(v)1850.13–14, 115n.r.7.1 ± 0.725.9 ± 1.1822 ± 4296.9 (49)
a

The Mn values of TPEs were measured by size exclusion chromatography (SEC) except for PPDO-b-PβMVL-b-PPDO, which was measured by 1H NMR.

b

Weight percentage of the urethane-rich hard segments in the polyurethane.

c

Molar percentage of the urethane-rich hard segments in the polyurethane.

d

Tg and Tm were measured by differential scanning calorimetry (DSC).

e

E, σb, and εb represents Young’s modulus, ultimate tensile strength, and elongation at break, respectively.

f

Calculated from 10 cycles at 100% strain unless otherwise noted.

g

Calculated from 20 cycles at 100% strain.

h

Calculated from 20 cycles at 50% strain.

i

These data were not reported in the references, n.r. = not reported.

2. Chemically Recyclable Block Copolyester-Based TPEs

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Aliphatic block copolyester-based TPEs derived from various cyclic monomers have attracted extensive attention due to the abundant commercially available cyclic monomers, potential biodegradability, and tunable structures and properties. (50) A series of triblock copolymers composed of a hard-end block of polylactide (PLA) and a biorenewable midblock, such as poly(ε-decalactone) (PDL), poly(6-methyl-ε-caprolactone) (PεMCL), and poly(γ-methyl-ε-caprolactone) (PγMCL), has witnessed rapid development over the past two decades. (51−53) Despite biorenewability and biodegradability, these TPEs usually end up in nature as water and carbon dioxide after their service life. It is more attractive to develop chemically recyclable TPEs that can be depolymerized back to their original monomers or converted to valuable building blocks to recover material value. One promising strategy to prepare chemically recyclable block copolyester-based TPEs is sequential ROP of cyclic lactones or lactides with a moderate ceiling temperature.
δ-Caprolactone (δCL) is a biosourced monomer with a low ceiling temperature of 42 °C at [M]0 = 1 mol L–1. The corresponding PδCL is capable of depolymerizing back to δCL at 130 °C under vacuum, catalyzed by stannous octoate (Sn(Oct)2). Given its low Tg of −39 °C, PδCL is a promising candidate as a soft segment of chemically recyclable TPEs. For example, our group achieved the one-pot sequential ROP of δ-caprolactone (δCL) and l-lactide (l-LA) to produce well-defined PLLA-b-PδCL-b-PLLA triblock copolymers. The phase separation morphology and mechanical properties of PLLA-b-PδCL-b-PLLA triblock copolymers can be precisely regulated by their volume fraction of hard segment (fhard). (33) As fhard gradually increased from 0.22 to 0.45, the transition of the phase separation morphology from a poorly ordered sphere to a lamellar phase was observed from the small-angle X-ray scattering (SAXS) curves. When the fhard was in the range of 0.33–0.45, these triblock copolymers exhibited thermoplastic elastomer properties. For example, PLLA-b-PδCL-b-PLLA with a Mn of 90.9 kg mol–1 and a fhard of 0.33 exhibited an excellent tensile strength of 20.4 MPa and elastic recovery of 91.8%.
In contrast to the simple recycling of PδCL homopolymer, initial attempts to recover δCL and l-LA by directly heating PLLA-b-PδCL-b-PLLA triblock copolymers in bulk using Sn(Oct)2 as the catalyst failed due to the high ceiling temperature of l-LA and poor depolymerization selectivity of PLLA. Although several latter studies reported new catalysts and optimized conditions to achieve the selective depolymerization of PLLA, (54−56) the direct depolymerization of PLLA-b-PδCL-b-PLLA can only afford a mixture of δCL and l-LA. Tedious separation and purification are required before the recovered monomers can be reused to produce new TPEs, thus reducing the environmental benefit. As an alternative, we proposed a tandem alcoholysis and depolymerization strategy for the chemical recycling of PLLA-b-PδCL-b-PLLA triblock elastomers. As shown in Figure 1, the PLLA block was completely converted to ethyl lactate by alcoholysis with ethanol in the presence of Sn(Oct)2 as the catalyst. It is worth pointing out that the PδCL block remained as a polymer despite with a reduced Mn and a broadened distribution. As such, ethyl lactate can be easily recovered with a high yield (∼92%) through vacuum distillation (1600 Pa) at 45 °C. Subsequently, the depolymerization of PδCL midblock was achieved at 140 °C, and almost quantitative clean δCL (∼95% yield) was recovered by distillation under reduced pressure (200 Pa). Notably, ethyl lactate is a valuable chemical and can be used as a food additive and environmentally benign solvent. (57)

Figure 1

Figure 1. Illustration of preparation and chemical recycling of PLLA-b-PδCL-b-PLLA triblock elastomer. (34)

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In the case of PLLA-b-PδCL-b-PLLA triblock elastomers, only a portion of the components was chemically recycled back to δCL, and additional l-LA was required to prepare new TPEs and close the life cycle. It is highly attractive to develop TPEs that can be depolymerized back to recover both monomers and thus achieve an ideal “polymer–monomer–polymer” closed-loop life cycle, which is more in line with the circular plastics economy. In addition to δCL, other six-membered cyclic lactones also have moderate ring strain and a low ceiling temperature (Tc). The corresponding polyesters can be depolymerized under mild conditions to recover the original monomers, and the recycled monomers can be repolymerized to afford virgin-quality polyesters. Moreover, the crystallinity and entanglement molar mass (Me) of the polyesters can be finely tuned by the position and length of the alkyl substituents, (50) which facilitates the regulation of the structure and properties of triblock copolyester-based elastomers. Therefore, six-membered cyclic lactones show great potential in the development of TPEs with closed-loop recyclability based on their ROP and RCD. In 2024, Chen and Xu reported the synthesis of PVL-b-PαMeVL-b-PVL triblock elastomers through the one-pot sequential ROP of α-alkyl-δ-valerolactone (αMeVL) and δ-valerolactone (δVL). (35) The triblock elastomers with a Mn of 144 kg/mol and a fhard ∼0.5 exhibited an ultimate tensile strength of 29.7 MPa, an elongation at break of 1041% and a toughness of 135 MJ m–3. The TPEs were capable of depolymerizing back to recover a mixture of δVL and αMeVL by vacuum distillation in the presence of ZnCl2 or phosphomolybdic acid as a catalyst. In order to avoid the tedious separation and energy cost of using column chromatography, a large excess amount of δVL was mixed with the recovered monomers to achieve a [δVL]/[αMeVL] ratio of 92:8, which then underwent ROP to produce the PVL macroinitiator. A pentablock elastomer PVL-b-PαMeVL-b-PVL-b-PαMeVL-b-PVL was then prepared by sequential ROP of δVL and αMeVL. Although it seems that the chemical recycling of PVL-b-PαMeVL-b-PVL was achieved, only a small portion of the new TPEs was composed of the recovered monomers.
Recently, our group successfully synthesized a series of triblock copolymers by sequential ROP of β-alkyl-δ-valerolactone (βMVL) and δ-valerolactone (δVL). (36) Compared to PαMeVL (Me = 7.7 kg mol–1), PβMVL has a lower entanglement molar mass (Me = 4.3 kg mol–1), which makes it a better candidate as the soft midblock to impart the TPEs with superior mechanical properties due to more efficient chain entanglement. As such, the obtained PδVL-b-PβMVL-b-PδVL (Mn = 102.5 kg mol–1, fhard = 0.63) behaved as a supertough thermoplastic elastomer, showing a ultrahigh ultimate tensile strength of 48.2 MPa, an elongation at break of 2007%, a high toughness of 391.2 MJ m–3, and a high elastic recovery of 95.5%, a resilience of 75%, and a low residual strain of 3.5%, which surpass most previously reported chemical recyclable or commercial styrenic block copolymers based TPEs (SBS YH-791 and SEBS YH-506T from Baling Petrochemical Company).
It is worth noting that the PδVL-b-PβMVL-b-PδVL triblock elastomers were capable of bulk depolymerizing back to recover original monomers in the presence of 4 wt % Sn(Oct)2 as the catalyst at 130 °C under reduced pressure (70–80 Pa). Two strategies have been proposed to achieve the closed-loop recycling of the TPEs. As illustrated in Figure 2, the recovered βMVL and δVL can be separated by column chromatography and then sequentially repolymerized to obtain a new triblock elastomer PδVL-b-PβMVL-b-PδVL with the same performances as the original TPE. As an alternative, the cumbersome and energy-consuming separation process of the two monomers was abandoned. The recovered monomer mixture was directly copolymerized to afford an amorphous soft segment. δVL was subsequently added for ROP to produce a triblock copolymer PδVL-b-P(βMVL-co-δVL)-b-PδVL with good elastomeric performances. It is obvious that the regenerated TPE possessed a different composition and structure from the original one. Therefore, such recycling is more like a upcycling process rather than a closed-loop recycling.

Figure 2

Figure 2. Illustration of the sequential ROP of βMVL and δVL toward PδVL-b-PβMVL-b-PδVL triblock copolymers and their chemical recycling. Adapted from ref (36). Copyright 2025 Wiley-VCH Verlag.

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The upper service temperature of TPEs can be improved when a polymer with a high Tm value is used as the hard block. For example, closed-loop recyclable TPEs with good performance were recently prepared by sequential ring-opening copolymerization of biobased βMVL and p-dioxanone (PDO). (37) The obtained triblock elastomer PPDO-b-PβMVL-b-PPDO (Mn = 90.0 kg mol–1, fhard = 0.24) exhibited an excellent tensile strength up to 21 MPa, a high elongation at break up to 1054%, and a high elastic recovery up to 93.5%. Notably, the TPE possessed a wide operational temperature range from −45.2 to 81.3 °C, facilitating a step forward in practical application.
In 2025, Wang et al. proposed a “polycondensation–depolymerization–repolymerization” strategy for the synthesis of closed-loop recyclable and structurally diverse aliphatic polycarbonates and poly(thioether-alt-ester)s. (38,58) The thermal and mechanical properties of polycarbonates can be widely adjusted by changing the types and positions of substituents on cyclic carbonate monomers. Based on this, a triblock copolymer was prepared by one-pot sequential ROP of trimethylene carbonate (TMC) with a spiro-cyclopentyl substituent (5C-TMC) and TMC substituted with methyl and propyl groups (MePr-TMC). (38) The obtained triblock copolymer P(5C-TMC)-b-P(MePr-TMC)-b-P(5C-TMC) exhibited elastomeric performances, which can be completely recovered as diols/dialkyl carbonates by alcoholysis or directly depolymerized to recover the corresponding cyclic carbonate monomers. The monomers can be separated by column chromatography and then repolymerized to afford a new triblock elastomer.
Although the above examples demonstrate the concept of closed-loop recyclable TPEs, tedious and costly separation of the monomer mixture by column chromatography or additional monomers is still required to achieve chemical recycling. At present, it remains a challenge to develop a simple method to separately recycle two monomers with high selectivity and purity so that they can be reused for sequential ROP to produce new block copolymers. On the other hand, if the block copolymers can be prepared directly from the monomer mixtures, there is no need to separate the monomers.
Switchable polymerization as an innovative synthetic strategy enables the polymerization switching between different monomers by external triggers, such as catalysts, solvents, and temperature, thereby efficiently synthesizing structurally complex multiblock copolymers from a variety of monomer mixtures in a “one-pot, one-step” method. (59−61) The TPEs prepared by switchable polymerization can avoid the cumbersome and costly monomer separation involved in the recycling process, which is desirable for achieving the ideal “polymer–monomer–polymer” closed-loop life cycle. In 2024, Matson and Byers reported a switchable polymerization between the ROP of lactide (LA) and the copolymerization of tetrahydrofuran/cyclohexene oxide (THF/CHO) using an iron-based redox-switchable catalytic system. A well-defined triblock copolymer PLLA-b-P(THF-co-CHO)-b-PLLA was prepared directly from the mixture of l-LA, THF, and CHO. (39) PLLA-b-P(THF-co-CHO)-b-PLLA with a Mn of 109 kg mol–1 behaved as a TPE, exhibiting an ultimate tensile strength of 16 MPa and an elongation at break of 277%. Although only THF and l-LA were recovered with a moderate yield of 78% and 80%, respectively, this study provides a new strategy for the design and preparation of closed-loop recyclable TPEs.
In addition to switchable polymerization triggered by external factors, block elastomers can also be prepared by utilizing the large difference in polymerization activity between two monomers. In 2025, Zhu and co-workers prepared a gradient block copolymer P(SHPL-co-εCL) by a one-pot copolymerization directly from a mixture of εCL and highly active α-spirocyclohexyl propiolactone (SHPL). (40) The gradient P(SHPL-co-εCL) segment served as a soft block, while the PCL-rich segment and the P3HSHP-rich segment acted as hard-end blocks. Notably, the gradient copolymer P(CL2000-grad-SHPL500) exhibited impressive elastomer characteristics, with an ultimate tensile strength of 58.8 MPa, an elongation at break of 1959%, and a high elastic recovery (>90%). Although this study did not achieve the recycling of elastomers, it provides an insight that there is no need to achieve a strict block structure for TPE applications. Recently, Tang et al. reported a solvent-dependent sequence-controlled copolymerization of 4-phenyl-2-oxabicyclo [2.1.1]hexan-3-one(4Ph-BL) and ε-caprolactone (ε-CL) to produce block and statistical copolyesters. (41) As shown in Figure 3, the unique kinetic differences of 4Ph-BL and ε-CL make it easy for these two monomers to copolymerize to form block copolyester PCL-b-P(4Ph-BL) in non-coordinating solvents, such as dichloromethane and toluene. In contrast, coordinating solvents such as tetrahydrofuran, 2-methyltetrahydrofuran, 2,5-dimethyltetrahydrofuran, 1,4-dioxane, and 1,2-dimethoxyethane promoted intramolecular and intermolecular transesterification, resulting in statistical copolyesters P[CL-stat-(4Ph-BL)] with different degrees of randomness. P[CL48-stat-(4Ph-BL)52] (Mn = 383 kg mol–1) with 48% ε-CL incorporation behaves as a TPE, showing a high excellent tensile strength of 34.5 MPa and elongation at break of 812%, outstanding elastic recovery of ≥99.3%, high resilience of ≥92.0%, and low residual strain of ≤0.7%. Of note, both statistical and block P(4Ph-BL)-based copolymers can achieve a closed-loop life cycle catalyzed by yttrium complex Y(CH2SiMe3)3(THF)2 (Y1). After P[CL48-stat-(4Ph-BL)52] (Mn = 87.0 kg mol–1, D = 1.82) was heated at 250 °C for only 1 h, the pure mixed monomers with 98% conversion for 4Ph-BL and 94% conversion for ε-CL were recovered.

Figure 3

Figure 3. Solvent-dependent sequence-controlled copolymerization of 4Ph-BL with ε-CL to produce block or statistical copolyesters and their chemical recycling. (41)

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3. Chemically Recyclable Thermoplastic Polyurethane Elastomers

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Polyurethane elastomers are typically synthesized through the step-growth polymerization of polyols with diisocyanates or polyisocyanates. Compared with physical recycling that can only produce low-value materials, the chemical recycling by alcoholysis and acidolysis can efficiently recover polyols and realize their reuse for the production of value-added polyurethane materials. (62,63) Although the recovered polyols can be employed to synthesize new polyurethanes, their substitution for virgin polyols is limited to a maximum of 10–20 wt % without compromising the quality of the final polyurethane products. (64,65) Due to these limitations, the development of polyurethane elastomers with intrinsic recyclability using closed-loop recyclable polyester polyols presents an attractive strategy considering the immense economic and practical potential. In 2014, Hillmyer and Zhang et al. reported a large-scale, economically viable method to synthesize bioderived β-methyl-δ-valerolactone (βMδVL), which underwent controlled polymerization to produce closed-loop recyclable polyesters (PβMδVL). (66) α,ω-Hydroxy telechelic PβMδVL polyol can be used as a replacement of petroleum-derived polyols to successfully produce PβMδVL-based thermoplastic polyurethane (TPU) elastomers with thermal and mechanical properties comparable to those of commercial TPU elastomers. (42) It was demonstrated that the rapid depolymerization of PβMδVL enabled efficient chemical recycling of the TPU elastomers to recover the βMδVL monomer with a high yield of 97%. Subsequent studies revealed that the copolymerization of high-Tc monomers with βMδVL enhanced the thermodynamic stability of α,ω-hydroxy telechelic copolyesters, which can then react with isocyanates and water (chain extender) to produce thermoplastic polyurethane-ureas (TPUU) elastomers with a high ultimate tensile strength σb of 54 MPa and an elongation at break εb of 740%. (67) When 50% of the original monomers were replaced with recycled βMVL, the mechanical properties of the reproduced elastomer TPUU-R (σb = 54 MPa, εb = 720%) were almost the same as those of the original TPUU, demonstrating excellent chemical recyclability.
In 2022, our group reported a cascade ROP and step-growth polycondensation strategy to produce chemical recyclable PδCL-based TPU elastomers, which can be recycled back to δCL with an almost quantitative yield. (43) Recently, a series of TPU elastomers with high mechanical properties and excellent hydrolysis resistance was prepared using poly(alkyl-δ-lactone) polyols as precursors, which were prepared by ROP of alkyl-δ-lactones bearing C3, C6, and C9 n-alkyl substituents at the δ-position (Figure 4). (44) The TPU elastomers exhibited an ultimate tensile strength of up to 60.4 MPa, an elongation at break of 899%, an elastic recovery of 98%, a resilience of 92%, and a residual strain of less than 2%. Meanwhile, the TPU elastomers remained intact after being immersed in acidic or alkaline aqueous solutions for up to five months. In addition to alkyl-δ-lactones, γ-butyrolactone (γBL) was also used to prepare chemical recyclable PγBL-based TPU elastomers. (45)

Figure 4

Figure 4. Illustration of the preparation of chemically recyclable polyurethanes from biosourced alkyl-δ-lactones as well as their chemical recycling to recover pristine monomers. Reproduced from ref (44). Copyright 2025 Elsevier.

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Although the above TPU elastomers achieved near-complete recovery of polyester polyols, it remains a great challenge to recycle components such as isocyanates and chain extenders. The highly active isocyanates generated from the dissociation of urethane bonds rapidly react with residual initiators and chain extenders to form a cross-linked network. The recycling of the remaining components, especially the high-value isocyanates, is an important direction for future research.

4. Chemically Recyclable Polyolefin-Like Elastomers

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Polyolefin elastomer (POE) is generally synthesized by the copolymerization of ethylene and α-olefins (such as 1-butene, 1-hexene, 1-octene, etc.) using metallocene catalysts. (68,69) It possesses excellent mechanical properties, as well as outstanding low-temperature resistance and processability. As a modifier or blend component, POE has been widely applied in various fields, including automotive parts, wires and cables, household goods, sports equipment, hot-melt adhesives, and seals. (70,71) When ethylene and α-olefins undergo copolymerization to form an olefin block copolymer (OBC) that exhibits a more defined multiblock structure, superior mechanical properties and an improved upper service temperature are achieved compared to POE. (72) Despite the low cost and wide applications, the chemical inertness of the carbon–carbon backbone of POE and BOC makes them difficult to degrade or recycle at the end of their service life.
The introduction of cleavable moieties such as ester bonds into the backbone of polyolefin-like elastomers offers a novel strategy for their chemical recycling. In 2023, Miyake et al. synthesized α,ω-hydroxyl-terminated telechelic hydrogenated poly(cyclooctene) and hydrogenated poly(3-hexylcyclooctene) oligomeric building blocks as hard and soft segments by ruthenium-mediated ROMP of cyclooctene and 3-hexylcyclooctene, respectively, in the presence of cis-hexadec-6-ene-1,16-diol as a chain-transfer agent (Figure 5a). (46) These hard and soft building blocks were subsequently subjected to dehydrogenative polymerization to produce ester-linked multiblock polyolefin-like copolymers. The mechanical properties of these polyolefin-like copolymers could be tailored by adjusting the molar ratio of hard to soft blocks, thereby achieving the transition from thermoplastics to elastomers. PE40 (82.4 kg/mol, Đ = 2.4, and 40 represented the molar percentage of the hard segment) exhibited typical elastomeric characteristics, with a tensile strength of 12.0 MPa and an elongation at break of 1030%. Additionally, PE40 demonstrated a high Tm of 109 °C and excellent thermal stability with a 5% weight-loss temperature (Td,5%) of 413 °C. Notably, the hydroxyl-terminated telechelic hard and soft oligomers could be efficiently recovered by ruthenium-catalyzed hydrogenolysis depolymerization. Especially, as shown in Figure 5b, the ester-linked polyolefin-like copolymers were completely depolymerized in toluene at 160 °C under 40 bar H2 over 24 h, achieving a 99% conversion from ester bonds to hydroxy groups. Furthermore, the hard and soft segments could be readily separated due to differences in their solubilities, with a yield greater than 90%. The ester-linked polyolefin-like copolymers could be regenerated by subsequent dehydrogenation polymerization. Multiple tests demonstrated that after two “hydrogenolysis depolymerization–dehydrogenation polymerization” closed-loop recycling processes, the recovered building blocks remained intact, and the molecular weight and mechanical properties of the regenerated polyolefin-like copolymers were nearly identical to those of the original copolymers, highlighting the stability and reproducibility of this recycling process. Moreover, the closed-loop recycling process for the ester-linked polyolefin-like copolymers from mixed plastic wastes was also demonstrated, indicating that the “catalytic dehydrogenation–hydrogenation reaction” holds significant potential for developing closed-loop recyclable polyolefin-like elastomers.

Figure 5

Figure 5. (a) Synthesis of hard and soft building blocks. (b) Preparation and closed-loop recycling of polyolefin-like multiblock elastomers. (46)

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In 2024, Gao, Chen, and Tang et. al reported a tandem coordination copolymerization and polycondensation strategy to synthesize a series of ester-linked polyethylene (PE)-based copolymers. (47) AB-type telechelic PE-based building blocks end-capped with hydroxyl (A) at one end and ester (CO2Et) functionality (B) at the other terminal were synthesized via coordinative chain-transfer polymerization (CCTP) of ethylene and 1-octene in the presence of alkyl zinc reagent Zn[(CH2)6OTIPS]2 (TIPS = triisopropylsilyl) as the functionalized chain-transfer agent. Hard and soft telechelic building blocks can be prepared by tuning the 1-octene incorporation. Consequently, ester-linked OBC elastomers were then prepared by polycondensation between hard and soft telechelic building blocks. The polyolefin-like elastomer rOBC7.7 (129.4 kg mol–1, Đ = 2.8, 7.7 mol % of 1-octene) demonstrated a tensile strength of 24.9 MPa and an elongation at break of 1953%. Meanwhile, this elastomer also exhibited excellent thermal properties with a Tm of 95.1 °C and a Td,5% up to 427.5 °C. Complete depolymerization of these OBC elastomers was achieved by alcoholysis to afford hard and soft building blocks, which can be separated based on their big difference in solubility. The recovered building blocks were then subjected to polycondensation catalyzed by Ti(OnBu)4 to regenerate the OBC elastomers, enabling their closed-loop recycling.
Olefin metathesis polymerization exhibits high tolerance to various functional groups and can be used to prepare degradable polyolefin-like polymers by introducing cleavable moieties into their main chains. For example, ROMP or ring-opening metathesis copolymerization (ROMCP) of cyclic monomers with cleavable moieties shows high efficiency and controllability to prepare degradable polymers. Zou and Chen et al. presented a one-pot, two-step tandem olefin metathesis polymerization (TOMP) system, combining the ring-closing metathesis (RCM) of diene comonomers with ROMCP of cyclic monomers to prepare polyolefin-like elastomers with in-chain ester bonds, (73) which can be easily degraded by alcoholysis in the presence of KOH to produce a mixture of α- and α,ω-substituted polyethylenes. The recovered oligomers then underwent polycondensation again to regenerate polyolefin-like elastomers. Although the mechanical properties of the regenerated elastomer were slightly lower than those of the original ones, this study provides a new strategy to develop closed-loop recyclable polyolefin-like elastomers.
In addition to the above multiblock polyolefin-like elastomers, Sha and Jia recently reported a very rare example of homopolymer-based chemically recyclable polyolefin-like elastomers through ROMP of a fully biobased cyclic olefin derived from isomannide and undecenoic acid (Figure 6a). (48) An unsaturated polyolefin structure with low crystallinity, consisting of “hard segments” (solid crystallites) and “soft segments” (noncrystalline domain), was obtained by judicious design of the monomer, which is crucial for achieving elastomeric properties in a homopolymer system. The obtained polyolefin-like elastomer P4 (158.3 kg mol–1) with a high molecular weight but a low crystallinity exhibited excellent tensile strength of 31.5 MPa, elongation at break of 1495%, and elastic recovery of 98%. As shown in Figure 6b, based on ring-closing metathesis depolymerization, the prepared polyolefin-like elastomers can be efficiently depolymerized to recover cyclic olefin monomer along with other cyclic polymerizable oligomers with an overall high yield of 90% under mild conditions (concentration of repeat units = 20 mM, 50 °C, 1 h) in the presence of 1 mol % Grubbs second-generation catalyst (G2). The recovered monomers can be repolymerized via ROMP to regenerate the original homopolymer, enabling closed-loop recycling (Cycle 3). The same homopolymer can also be synthesized directly from an α,ω-bifunctional diene monomer via acyclic diene metathesis (ADMET) polymerization (Cycle 1). Isomannide and α,ω-dicarboxylic acid can be recovered in high yield (∼93%) through alkaline hydrolysis and subsequently used in polycondensation to reproduce a polyolefin-like elastomer (Cycle 2).

Figure 6

Figure 6. (a) Synthesis of homopolymer-based polyolefin-like elastomers and (b) their chemical recycling through three cycles. (48)

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5. Chemically Recyclable Dynamically Cross-Linked Elastomers

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Compared with traditional chemically cross-linked rubbers, TPEs exhibit relatively weaker physical cross-linking, resulting in significant reductions in terms of high-temperature resistance, solvent resistance, and mechanical properties. The recently emerging dynamically cross-linked strategy can not only effectively improve the mechanical properties and solvent resistance of elastomers but also maintain their physical reprocessability. Dynamic covalent bonds such as borate bond (74−76) and imine bond, (77,78) as well as noncovalent interactions such as coordination bond, (79,80) hydrogen bond, (81) ionic interaction, (82) and mechanical interlocks, (83) have been employed in the development of high-performance, reprocessable elastomers. Nevertheless, we will only introduce recent developments on chemically recyclable dynamically cross-linked elastomers in the following section.
Mechanical interlocking networks (MINs), featuring versatile interlocked topology, stability, structural integrity, and dynamic properties, have emerged as a promising platform to develop mechanically robust yet adaptable materials. In 2022, Yan and Zhang et al. combined dynamic vinylogous urethane bond with mechanically interlocked structures to prepare a class of elastomers with dual-dynamic network. (83) Specifically, the elastomers were prepared through the catalyst-free condensation reaction between presynthesized acetoacetate-modified [2] rotaxanes and two commercially available monomers of 1,14-diamino-3,6,9,12-tetraoxatetradecane (monomer A) and tris(2-aminoethyl) amine (monomer B). In contrast to the elastomers without mechanically interlocked cross-linking points, the dual-dynamic network elastomers exhibited significantly enhanced mechanical properties, including Young’s modulus (18.5 vs 1.0 MPa), toughness (3.7 vs 0.9 MJ/m3), and damping capacity (98% vs 72%). In addition to excellent physical reprocessability, the dual-dynamic network elastomers can also undergo depolymerization and chemical recycling based on the transamination reaction of vinylogous urethanes. When the fragments of dual-dynamic network elastomers were immersed in an acetonitrile solution containing 5 equivalents of n-butylamine at 80 °C for 5 h, the cross-linked networks of these elastomers were degraded to n-butylamine-modified [2] rotaxane monomers. The n-butylamine-modified [2] rotaxane monomers were collected by precipitation, and excess n-butylamine with acetonitrile solution was removed. Fresh amine monomers A and B were then added to react with the modified [2] rotaxanes to afford the regenerated dual-dynamic network elastomers. The thermal and mechanical properties of the regenerated elastomers were consistent with those of the original elastomers, supporting effective depolymerization and the chemical recycling of these elastomers.
The chemical recycling of dynamically cross-linked elastomers still suffers from large excess use of solvents and/or harmful reagents, incomplete cleavage of dynamic covalent bonds, tedious separation, and purification of degradation products. How to achieve controllable depolymerization and closed-loop recycling or upcycling of dynamically cross-linked elastomers remains a big challenge.
In 2022, Gregory and Williams et al. developed a series of triblock elastomers PE(v)-b-PTMC-b-PE(v) by a one-pot, sequential ROP of trimethylene carbonate (TMC) and ring-opening alternating polymerization of phthalic anhydride (PA) with vinyl-cyclohexene oxide (vCHO) (Figure 7a). The alternating copolymer of PA and vCHO was simplified as PE(v). (49) The prepared triblock elastomer P3 (185 kg mol–1, fhard ∼ 0.13) had an ultimate tensile strength of 25.9 MPa, an elongation at break of 822%, and an elastic recovery of 96.9%. To further enhance the mechanical properties of the elastomer, hydrogen bonding and Zn2+-COOH coordination interaction were introduced into the hard segments to afford the hydrogen-bonding cross-linked elastomer P3COOH and Zn2+-COOH coordination cross-linked elastomer P3Zn, respectively. P3COOH and P3Zn both exhibited significantly improved tensile strength while maintaining elongation at break as P3. The tensile strength of P3COOH and P3Zn was 39.3 and 62.3 MPa, respectively. Meanwhile, P3Zn exhibited good reprocessability as supported by the unchanged mechanical properties even after being hot-pressed and molded at 200 °C five times. Furthermore, as shown in Figure 7b, the depolymerization of the elastomer could be achieved to recover TMC monomer with a yield of 75% by using 0.15 equiv of 1,5,7-triazabicyclo [4.4.0] dec-5-ene (TBD) (relative to TMC repeating units) as the catalyst in dry acetonitrile at 80 °C for 3 h. Alternatively, cyclic carbonates can be separated and recycled with a yield of 82–92% by the addition of 3 equivalents of diol (relative to TMC repeating units) during the depolymerization process. As analogues of TMC, the recovered cyclic carbonates can also undergo ROP to afford polycarbonate. 1H NMR spectroscopy indicated that the remaining polyester segment was converted to ring-opened epoxides and the phthalate ester of the diol.

Figure 7

Figure 7. (a) Preparation and (b) chemical recycling of PE(v)-b-PTMC-b-PE(v) and P3Zn triblock elastomers. (49)

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6. Conclusion and Perspective

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The development of chemically recyclable TPEs with high performances is of particular importance to address the end-of-life issue of plastics and to create a circular life cycle. Compared with conventional physical recycling, which is highly sensitive to the impurities and other polymers, chemical recycling of TPEs offers a new opportunity to recover the material value when they are no longer suitable for mechanical reprocessing. This review highlights the latest advancements in chemically recyclable TPEs that can be depolymerized back to recover monomers or converted to building blocks, which can be reused to produce TPEs with comparable performances to the original ones. According to the classification of chemically recyclable TPEs, block copolyesters, thermoplastic polyurethanes, polyolefin-like elastomers, and dynamically cross-linked elastomers are sequentially introduced, focusing on the discussion of their preparation and on-demand chemical recycling. The chemically recyclable block copolyester-based TPEs and TPU elastomers are typically prepared from polyester building blocks by ROP of cyclic lactones with a moderate ceiling temperature. Their chemical recycling is achieved by depolymerizing back to the cyclic lactone monomers. This strategy benefits from the mild depolymerization conditions, easy recovery of monomers, and no need to use solvents. In contrast, chemically recyclable polyolefin-like elastomers are typically prepared by incorporating cleavable bonds into their backbone, such as an ester bond. As such, polyolefin-like elastomers are chemically recycled back to their constituted polyolefin building blocks. The incorporation of dynamically cross-linked points significantly enhances the mechanical strength and elasticity of the elastomers while maintaining their physical recyclability. Nevertheless, due to the challenges to achieve the controlled depolymerization of networks and facile recovery of fragments, studies addressing the chemical recycling of dynamically cross-linked elastomers are largely underexplored.
Over the past decade, chemically recyclable TPEs have attracted significant attention and become a rapidly advancing research field. As the next generation of TPE materials, these chemically recyclable TPEs hold broad application prospects and deserve further exploration to address the following challenges.
(1)

It is attractive to continuously develop TPEs with intrinsic chemical recyclability to create an ideal closed-loop life cycle. Most of the above-reported chemically recyclable TPEs only achieve the recovery of partial components, especially for the thermoplastic polyurethane elastomers. Even for the cases of fully recyclable block copolyester-based TPEs, tedious, costly, and time-consuming separation and purification of monomers by column chromatography are required to close the “material–monomer–material” loop. Utilizing monomers with big differences in solubility or boiling point may facilitate their separation by extraction, recrystallization, or distillation. Another promising strategy is to achieve the selective recovery of different monomers by the selective depolymerization of soft and hard blocks. As an alternative promising strategy, switchable polymerization presents an opportunity to prepare TPEs directly from the monomer mixture so that monomer separation is not necessary.

(2)

More efforts should be devoted to developing a more efficient chemical recycling strategy for polyolefin-like elastomers and dynamically cross-linked elastomers. Although polyolefin-like elastomers exhibit excellent thermal stability and mechanical properties comparable to those of commercial POE or OBC elastomers, the current chemical recycling strategy to recover polyolefin oligomers suffers from a large excess use of solvent, harmful reagents (such as strong acids or bases), or high-pressure hydrogen. The same problems exist for the chemical recycling of dynamically cross-linked elastomers. There is an urgent need to develop a milder, greener, and solvent-free chemical recycling strategy to promote their practical applications.

(3)

It is crucial to investigate the chemical recycling of these TPEs in the real world. The current studies in the laboratory use single or pure TPEs for their chemical recycling, which is not consistent with reality. Future research on the chemical recycling of these materials in a mixed plastics stream is necessary to evaluate their economic and ecological accessibility.

(4)

Last but perhaps the most important thing to keep in mind, it is necessary to prepare TPEs with comparable properties to their commercial analogues before considering their recycling. Otherwise, “wastes” rather than useful materials are produced at the beginning. In addition to the frequently investigated thermal stability, mechanical strength, and elastic recovery, fatigue resistance, high- and low-temperature resistance, chemical stability, creep and stress relaxation, weather resistance, processability, and production cost should be evaluated. The comprehensive evaluation and comparison provide a data foundation for the potential application of chemical recyclable TPEs in the future.

Author Information

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  • Corresponding Author
  • Author
    • Yingying Liu - State Key Laboratory of Advanced Optical Polymer and Manufacturing Technology, College of Chemical Engineering, Qingdao University of Science and Technology, Qingdao 266042, China
  • Notes
    The authors declare no competing financial interest.

Acknowledgments

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The authors appreciate the financial support by the National Natural Science Foundation of China (Nos. 52322304 and 22475117), the Natural Science Foundation of Qingdao (24-4-4-zrjj-17-jch), and the Postdoctoral Innovation Project of Shandong Province (SDCX-ZG-202400254).

A Vocabulary Section:

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Chemical recycling

A process that polymer is depolymerized to recover pristine monomers or converted to valuable chemical raw materials.

Thermoplastic elastomer (TPE)

A type of polymer material that combines the physical properties of traditional cross-linked vulcanized rubber with the processing properties of a thermoplastic.

Closed-loop recyclable TPE

A type of TPE that can be depolymerized back to their pristine monomers under controlled conditions at the end of their service life. The recovered monomers can be repolymerized to produce virgin-quality TPE, thus establishing a “polymer–monomer–polymer” closed-loop life cycle.

Dynamic cross-linked elastomers

A type of elastomer material that is cross-linked by dynamic covalent bonds or supramolecular interactions. The dynamic cross-linked elastomers combine the chemical resistance and mechanical strength of thermosets with the reprocessability of thermoplastics.

Volume fraction of hard block (fhard)

A critical parameter describing the composition of a block copolymer (such as TPE), which can be calculated according to fhard = ρsoftblock/[ρhardblock (1/ωhardblock – 1) + ρsoftblock], where ω is the weight percent of hard block and ρ represents the density at room temperature.

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  • Abstract

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    Figure 1

    Figure 1. Illustration of preparation and chemical recycling of PLLA-b-PδCL-b-PLLA triblock elastomer. (34)

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    Figure 2

    Figure 2. Illustration of the sequential ROP of βMVL and δVL toward PδVL-b-PβMVL-b-PδVL triblock copolymers and their chemical recycling. Adapted from ref (36). Copyright 2025 Wiley-VCH Verlag.

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    Figure 3

    Figure 3. Solvent-dependent sequence-controlled copolymerization of 4Ph-BL with ε-CL to produce block or statistical copolyesters and their chemical recycling. (41)

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    Figure 4

    Figure 4. Illustration of the preparation of chemically recyclable polyurethanes from biosourced alkyl-δ-lactones as well as their chemical recycling to recover pristine monomers. Reproduced from ref (44). Copyright 2025 Elsevier.

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    Figure 5

    Figure 5. (a) Synthesis of hard and soft building blocks. (b) Preparation and closed-loop recycling of polyolefin-like multiblock elastomers. (46)

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    Figure 6

    Figure 6. (a) Synthesis of homopolymer-based polyolefin-like elastomers and (b) their chemical recycling through three cycles. (48)

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    Figure 7

    Figure 7. (a) Preparation and (b) chemical recycling of PE(v)-b-PTMC-b-PE(v) and P3Zn triblock elastomers. (49)

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