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At least 37 records · Page 2

Predicting Selective Laser Printing Print Quality of Polymer Powders through Melt Flow Index

Selective Laser Sintering (SLS) uses a precisely controlled laser to fuse polymer powder to build complex 3D shapes. While SLS covers a wide application space, the processing knowledge of polymer powder is limited, restricting the number of commercial powders available. This study serves to expand the processing knowledge of polypropylene and polyethylene in parallel with a “mature” SLS feedstock, nylon, through melt flow index (MFI) characterization. Differential Scanning Calorimetry (DSC) was used to explore the sintering window of the polymers. Polyethylene and polypropylene exhibited a relatively narrow sintering window between 4 – 5 °C, whereas the sintering window of nylon was much wider, between 23 – 24 °C. This suggests that the print quality between polyethylene and polypropylene would be similar; however, X-ray computed tomography revealed a higher volume of print defects, voids, and de lamination in polyethylene than in polypropylene. MFI analysis provided additional insight into the difference in print quality, as the MFI of polyethylene was 7.16 g/10 min, 9.95 g/10 min for polypropylene, and 17.23 g/10 min for nylon. MFI is inversely correlated to melt viscosity, and a low melt viscosity is desired for proper coalescing between the layers and particles. These results suggest that MFI is a promising tool, in conjunction with traditional thermal analysis, for screening candidate powder feedstocks for SLS and optimization of print parameters for novel powders.

36 MATERIALS SCIENCE

Latent Catalysis as a Platform for Accessing Diverse Material Properties in Vat Photopolymerization 3D Printing

Vat photopolymerization (VP) 3D printing is an attractive strategy to manufacture customized polymer parts. The properties of printed materials are limited by the need to employ a low viscosity liquid resin and achieve rapid polymerization kinetics. To circumvent this limitation, dual‐cure methods have been developed using reagents embedded in the liquid resin formulation; however, the reagent‐based approach requires the discovery and optimization of new chemistry for each desired material. Here, in this work, we demonstrate a catalytic, dual‐cure platform that enables access to both Nylon‐6 and polyester interpenetrating networks through VP 3D printing under a universal approach. Structure–reactivity relationships of the latent NHC catalysts led to the identification of a magnesium chloride–NHC adduct as a latent catalyst that is orthogonal to radical polymerization and can be unmasked at elevated temperatures post‐printing to initiate ring‐opening polymerization of lactones and lactams. This strategy results in access to semicrystalline materials, which are a challenging morphology to access via VP 3D printing, that have attractive mechanical properties and can be printed at high resolution. This work represents the first photochemical‐based 3D printing of Nylon‐based materials and demonstrates the value of catalytic approaches to access new material properties in VP 3D printing.

Colliver, Cali N. [University of North Carolina, C

Production and Evaluation of Fluorophore-Doped Polymer Substrates to Screen for Plastic-Degrading Enzymes

Fast and sensitive analytical methods are the key to efficient screening of plastic-degrading enzymes. Here, we present a streamlined and affordable approach to assess the enzymatic deconstruction of insoluble synthetic polymers by blending them with a fluorescent dye, rhodamine 6G, and we evaluate this screening method using poly(ethylene terephthalate) (PET) as a model material. Our results indicate that enzymatic depolymerization of the rhodamine-doped PET can be observed in a high-throughput fashion by following release of the fluorophore. The fluorescence data obtained during the hydrolysis of rhodamine-doped PET by 14 PET hydrolases, produced with a robotic platform, correlated with the quantitative chromatographic analysis of PET degradation products. Remarkably, the use of the rhodamine-loaded PET substrate resulted in negligibly low background signals even when detecting PETase activity in crude cell lysates, suggesting suitability for screening of a wide variety of samples. Encouraged by these results, we next produced a selection of polyethylene- and nylon-based materials loaded with rhodamine 6G. While rapid leaching of fluorophore observed with nylon substrates limits the utility of the method for detecting nylonase activity, the rhodamine-loaded polyethylene showed promising performance in passive diffusion tests, indicating that this latter substrate may be used to screen for polyolefin-degrading enzymes.

09 BIOMASS FUELS

Circularity in Sequence-Controlled Copolyamides Enabled by Regioselective Enzymatic Hydrolysis

Sequence-controlled polymers enable precise control over macromolecular structures and function, but both their synthesis and end-of-life management remain fundamental challenges. Achieving high sequence fidelity is synthetically demanding, and conventional depolymerization methods lack regioselectivity, leading to irreversible loss of encoded molecular information and limiting polymer circularity. Enzymatic catalysis offers a potential solution by combining substrate specificity with selective bond cleavage. Here, we report the synthesis, characterization, and regioselective enzymatic depolymerization of poly- (X,AMA), a sequence-controlled copolyamide composed of alternating hexamethylenediamine−adipic acid (MA) and pxylylenediamine− adipic acid (XA) repeat units. Poly(X,AMA) was synthesized via solid-state polycondensation (SSP) of sequence-defined oligomers, enabling precise control over repeat-unit order. Polymer microstructure and sequence fidelity were confirmed by 13 C NMR spectroscopy and MALDI−TOF mass spectrometry. Comparison with a statistical copolymer analogue and Nylon-66 demonstrated pronounced differences in crystallinity, morphology, and thermal behavior arising from sequence control. Screening of 96 Nylon hydrolase homologues against poly(X,AMA) revealed strongly enzyme-dependent depolymerization profiles. While tetrad formation was generally favored, enzymes displayed pronounced sequence selectivity, preferentially releasing distinct sequence-defined tetrads XAMA or MAXA. SSP of sequence-defined tetrad MAXA produced a copolyamide with near identical monomer ordering as poly(X,AMA). Computational modeling of enzyme−substrate complexes identified structural features consistent with the observed regioselectivity. Together, these results establish selective enzymatic depolymerization as a viable strategy for the circular recycling of sequence-controlled polymers and provide a foundation for the rational engineering of enzymes for programmable polymer deconstruction.

Amides

Epoxy-based vitrimeric semi-interpenetrating network/MXene nanocomposites for hydrogen gas barrier applications

Herein, we report MXene-filled epoxy-based vitrimeric nanocomposites featuring a semi-interpenetrating network (S-IPN) to develop a hydrogen gas (H 2 ) barrier coating with self-healing characteristics for compressed H 2 storage applications. The reversible epoxy network was formed by synthesizing linear epoxy chains with pendent bis-hydroxyl groups using amino diol, which were then crosslinked with 1,4-benzenediboronic acid to generate dynamic boronic ester linkages. To achieve the S-IPN-type molecular arrangement, the epoxy chains were in situ crosslinked in the presence of poly(ethylene-co-vinyl alcohol) (EVOH), giving rise to a self-healing network (EEP) with a healing efficiency of 87%. Into the S-IPN vitrimer (EEP), a 2D platelet-type nanofiller MXene was incorporated to introduce a tortuous path for H 2 gas diffusion along with improved mechanical properties. The nanocomposite coating was applied to nylon 6 liner material, which is conventionally used in all-composite H 2 storage vessels. Further, the application of a 2 wt% MXene/EEP nanocomposite coating showed a permeability coefficient of 0.062 cm 3 mm m -2 d -1 atm -1 exhibiting ~96% reduction in gas permeability compared to uncoated nylon 6. The same nanocomposite exhibited a healing efficiency of 79%. Increasing the MXene loading to 10 wt% further reduced the permeability coefficient to 0.002 cm 3 mm m -2 d -1 atm -1 ; however, the healing efficiency decreased due to restricted chain mobility. In essence, the current work highlights the potential of vitrimeric S-IPN nanocomposite coatings for H 2 gas-barrier applications, enhancing safety and performance.

42 ENGINEERING

DAISY Benchmark Performance Data

This repository contains the underlying data from benchmark experiments for Drifting Acoustic Instrumentation SYstems (DAISYs) in waves and currents described in "Performance of a Drifting Acoustic Instrumentation SYstem (DAISY) for Characterizing Radiated Noise from Marine Energy Converters" (https://link.springer.com/article/10.1007/s40722-024-00358-6). DAISYs consist of a surface expression connected to a hydrophone recording package by a tether. Both elements are instrumented to provide metadata (e.g., position, orientation, and depth). Information about how to build DAISYs is available at https://www.pmec.us/research-projects/daisy. The repository's primary content is three compressed archives (.zip format), each containing multiple MATLAB binary data files (.mat format). A table relating individual data files to figures in the paper, as well as the structure of each file, is included in the repository as a Word document (Data Description MHK-DR.docx). Most of the files contain time series information for a single DAISY deployment (file naming convention: [site]_DAISY_[Drift #].mat) consisting of processed hydrophone data and associated metadata. For a limited number of DAISY deployments, the hydrophone package was replaced with an acoustic Doppler velocimeter (file naming convention: [site]_DAISY_[Drift #]_ADV.mat). Data were collected over several years at three locations: (1) Sequim Bay at Pacific Northwest National Laboratory's Marine & Coastal Research Laboratory (MCRL) in Sequim, WA, the energetic tidal channel in Admiralty Inlet, WA (Admiralty Inlet), and the U.S. Navy's Wave Energy Test Site (WETS) in Kaneohe, HI. Brief descriptions of data files at each location follow. - MCRL - (1) Drift #4 and #16 contrast the performance of a DAISY and a reference hydrophone (icListen HF Reson), respectively, in the quiescent interior of Sequim Bay (September 2020). (2) Drift #152 and #153 are velocity measurements for a drifting acoustic Doppler velocimeter in in the tidally-energetic entrance channel inside a flow shield and exposed to the flow, respectively (January 2018). (3) Two non-standard files are also included: DAISY_data.mat corresponds to a subset of a DAISY drift over an Adaptable Monitoring Package (AMP) and AMP_data.mat corresponds to approximately co-temporal data for a stationary hydrophone on the AMP (February 2019). - Admiralty Inlet - (1) Drift #1-12 correspond to tests with flow shielded DAISYs, unshielded DAISYs, a reference hydrophone, and drifting acoustic Doppler velocimeter with 5, 10, and 15 m tether lengths between surface expression and hydrophone recording package (July 2022). (2) Drift #13-20 correspond to tests of flow shielded DAISYs with three different tether materials (rubber cord, nylon line, and faired nylon line) in lengths of 5, 10, and 15 m (July 2022). - WETS - (1) Drift #30-32 correspond to tests with a heave plate incorporated into the tether (standard configuration for wave sites), rubber cord only, and rubber cord, but with a flow shielded hydrophone (November 2022). (2) Drift #49-58 and Drift #65-68 correspond to measurements around mooring infrastructure at the 60 m berth where time-delay-of-arrival localization was demonstrated for different DAISY arrangements and hydrophone depths (November 2022).

16 TIDAL AND WAVE POWER

The effect of stretching on polyamide – 6: assessment of crystallinity, mechanical properties, and surface roughness

Polyamide-6 (PA6), or nylon-6, is a widely used low-cost polymer material for various applications. Manufacturing PA6 into fibers involves a spinning process such as melt extrusion, which orients the polymer chains into a semicrystalline structure. When stretching the produced fibers to high strains, the PA6 fibers transition the metastable gamma phase back into the stable gamma phase. The effects of these large stretches on mechanical properties have not been explored after the stretch has been released. In this study, the effects on mechanical properties were studied by stretching the PA6 fibers from 10% to 50% tensile strain and subsequently releasing the fibers. The stretched fibers were characterized by X-ray diffraction and atomic force microscopy to determine the changes to the crystal structure and surface roughness. The stretched fibers were then tensile tested to failure and the tensile properties were examined. The stress-strain curves on the post-stretched PA6 fibers showed clear softening in the fibers with lower initial moduli after 30% stretching. Furthermore, these results may hold a clue to softening of fibers in applications with repeated loading and have implications for mechanical stability and fatigue of this polymeric material.

36 MATERIALS SCIENCE

Upcycling waste polystyrene to adipic acid through a hybrid chemical and biological process

Oxidative catalytic depolymerization of polystyrene (PS) can produce benzoic acid, but the annual consumption of benzoic acid is ~40 times lower than PS. For this catalytic oxidation method to be a viable means to manage PS waste, benzoic acid should be converted to higher-volume chemicals. We demonstrate a hybrid chemical and biological process that uses PS as feedstock for production of adipic acid, a high-volume co-monomer for nylon 6,6 via benzoic acid. Mn/Br co-catalyzed autoxidation of PS to benzoic acid proceeds with a yield of up to 94% in a solvent mixture of benzoic acid and water. The PS-derived benzoic acid undergoes bioconversion at near-quantitative yield to muconic acid, which is readily converted to adipic acid through catalytic hydrogenation. Process modeling, techno-economic analysis, and life cycle assessment estimate an adipic acid minimum selling price of $3.18/kg, with a 61% decrease in greenhouse gas emissions relative to production from fossil fuels.

09 BIOMASS FUELS

Lignin to adipic acid in a high-yield chemical and biological redox process

Viable manufacturing pathways to produce bio-based chemicals from renewable feedstocks, such as lignin derived from plant biomass, are needed to decarbonize the chemicals manufacturing sector. Converting the recalcitrant lignin polymer to valuable bioproducts remains a longstanding challenge in biorefining, with the highest reported single-product yield from lignin currently around 20 wt%. Most existing lignin depolymerization strategies target aryl–ether bond cleavage, which can produce aromatic monomers in yields of only about 30 wt%, and still as complex mixtures with C–C-linked dimers and oligomers. The recalcitrance of these C–C linkages between aromatic moieties fundamentally limits single-product yields from lignin, prompting the development of strategies to efficiently cleave these C–C bonds. Here, in this study, we show how reductive processing of lignin from poplar accesses a hydrocarbon mixture of alkyl-aromatic monomers and oligomers that is privileged for oxidative conversion to monomeric aromatic carboxylic acids, comprising mostly benzoic acid and phthalic acid isomers in up to 73 wt% monomer yields, using a Co/Mn/Br catalyst. The soil bacterium Pseudomonas putida KT2440 was engineered to convert this mixture of aromatic carboxylic acids to muconolactone, a precursor to bio-based nylons, enabling final adipic acid yields up to 26 wt% (gram adipic acid per gram lignin) with a maximum theoretical yield of 57 wt%. This pairing of reductive and oxidative steps with lignin resembles processes in petrochemical refining and shows how lignin may be converted into a single, valuable bioproduct in high yields.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH

Retrobiosynthesis of unnatural lactams via reprogrammed polyketide synthase

Engineered polyketide synthases (PKSs) have great potential as biocatalysts. These unnatural enzymes are capable of synthesizing molecules that are either not amenable to biosynthesis or are extremely challenging to access chemically. PKSs can thus be a powerful platform to expand the chemical landscape beyond the limits of conventional metabolic engineering. Here we employ a retrobiosynthesis approach to design and construct PKSs to produce δ-valerolactam (VL) and three enantiopure α-substituted VL analogues that have no known biosynthetic route. We introduce the engineered PKSs and pathways for various malonyl-CoA derivatives into Pseudomonas putida and use proteomics, metabolomics and culture condition optimization to improve the production of our target compounds. These α-substituted VLs are polymerized into polyamides (nylon-5) or converted into their N-acryloyl derivatives. RAFT polymerization produces bio-derived polymers with potential biomedical applications. Overall, this interdisciplinary effort highlights the versatility and effectiveness of a PKS-based retrobiosynthesis approach in exploring and developing innovative biomaterials.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH

Self‐Standing Carbon Nanofibers@Carbon Felt Electrodes to Boost Electrolyzer Productivity: Application to the Electro‐Manufacturing of trans ‐3‐Hexenedioic Acid and Adipic Acid

The industrial implementation of electrosynthesis for chemical manufacturing remains constrained by the limited surface area of conventional electrodes. Herein, this challenge is addressed by designing a carbon nanofiber@carbon felt (CNF@CF) electrode platform that combines the high conductivity, flexibility, and ease of handling of commercial carbon felts (CF) with the large surface area and tunable surface chemistry of carbon nanofibers (CNFs). CNFs are deliberately grown onto the CF scaffold to form a sword-in-sheath structure, where entangled nanofibers wrap the felt macrofibers to provide excellent mechanical stability and electrical conductivity without binders. CNF@CF is evaluated both as an electrode and as a catalyst support for the electrochemical hydrogenation of cis,cis-muconic acid (ccMA), a biobased platform molecule key to the production of performance polyamides and renewable Nylon 6,6. As a noncatalytic electrode for the partial hydrogenation to trans-3-hexenedioic acid, CNF@CF achieves a threefold increase in both cumulative productivity and Faradaic efficiency (FE) compared to bare CF. A similar boost in catalytic activity and energy efficiency is observed using Pd/CNF@CF for the hydrogenation of ccMA to adipic acid. These results highlight the opportunities of the CNF@CF platform for electro-organic synthesis and sustainable chemical manufacturing.

electrochemical hydrogenation

High compressive energy absorption and shape recovery behavior of additively manufactured textile-inspired cylindrical braided metamaterials

Mechanical metamaterials (MMs) are engineered structures with unique mechanical properties that arise from their unique spatial arrangement or lattice-like structure. The most commonly designed MMs such as honeycomb and re-entrant auxetics are prone to failure at the sharp corners and weak joints due to the increased stress concentration under deformation. To mitigate this challenge, braided MM structures involving intertwining threads of nylon—forming curved unit cells—have been studied. These textile-inspired cylindrical braided metamaterials (CBMMs) with contrasting unit cells, namely diamond and regular CBMMs, were fabricated by 3D printing. The layer-by-layer deposited structure built by fused filament fabrication delivered an assembly of overlapped threads that are fused at the contact point. To understand deformation behavior of these MMs, finite element models were developed for various load scenarios including quasi-static compression, cyclic and creep loads at room temperature. Stress distribution, deformation mechanisms, and failure modes were analyzed and validated by experiments to analyze the geometries and associated performance. The diamond CBMMs showed stress softening at 30 % compressive strain, withstanding a load of ∼440 N, whereas the regular CBMMs at 50 % strain experienced ∼250 N. The diamond CBMMs delivered higher creep resistance under sustained load and better energy absorption under cyclic loading than the regular CBMMs. The latter, however, exhibited 94 % shape recovery in contrast to 88 % recovery in former prototype during their first cyclic load. In conclusion, this study helps design mechanical lightweight devices that endure significant sustained load and exhibit enhanced energy absorption and shape recovery characteristics in cyclic loading.

Creep

Rational design of semi-interpenetrating network based on hyperbranched polyglycerol grafted MXene/polyurethane–epoxy for compressed hydrogen storage

Here, hydrogen (H 2 ) energy has emerged as a promising alternative in the automotive sector to replace fossil fuel; however, its storage with volumetric efficiency remains a challenge. The latest type IV storage vessel featuring a polymeric liner with composite overwrap incurs hydrogen saturation, which eventually causes failure. To prevent the H 2 dissolution in the liner, we have developed a barrier coating comprised of polyurethane/epoxy semi-interpenetrating network (S-IPN) combined with hyperbranched polyglycerol grafted MXene (h-MXene). The hyperbranched structure facilitated the dispersion of MXene in the coating solution by enhancing the exfoliation and improved the polymer filler interaction by forming covalent and H-bonding through end-terminal hydroxyl groups. Leveraging the dense network of S-IPN combined with the dispersed layer structured h-MXene significantly increased the tortuosity of the spray-coated barrier film applied to the nylon 6 liner. The coating exhibited a 90 % reduction in the H 2 gas permeability at only 2 wt% h-MXene concentration, which further improved to above 98 % at 10 wt% loading. Additionally, the h-MXene considerably improved the adhesion with the liner even in a highly stretched condition, signifying the durability of the coating under cyclic pressurization and depressurization of the storage vessel.

08 HYDROGEN

Development of fiber orientation in injection molding: Comparison of glass fiber, carbon fiber and their hybrid composites

Fiber orientation distribution (FOD) in injection-molded panels with respect to distance from the gate was analyzed using X-ray computed tomography (X-CT) for glass fiber (GF), carbon fiber (CF), and hybrid CF/GF (CGF) reinforced nylon 66. To understand the reason behind the FOD with different fiber types, computational fluid dynamics (CFD) and rheology were performed. Samples were extracted at three locations: near the gate, center, and opposite end. Thickness of the layers of typical skin-shell-core type FOD varied with fiber type and location. GF achieved flow direction alignment (in shell) earlier than viscous CF and CGF near the gate, whereas CF showed the highest flow-direction alignment at the center due to shear induced orientation. At the opposite end, GF experienced more backflow than others indicating faster mold filling owing to its lower viscosity. Hybrid CGF exhibited GF-dominated center and CF-dominated end region. The numerical model used to obtain FOD and rheological predictions for the CF and GF composites served to corroborate the trends observed in the experimental trials. The FOD responses across fiber types and location were reflected in their longitudinal and transverse properties. Only GF showed higher longitudinal modulus over transverse modulus near the gate attributed to rapid alignment, whereas CF and CGF exhibited opposite trend. However, fountain flow enhanced the longitudinal modulus over transverse modulus with the distance for all, particularly for CF. This study offers insights into mold filling behavior of different fibers which are critical in optimizing injection molding conditions for tailored final properties.

36 MATERIALS SCIENCE

Recycling of additively printed anisotropic Nd-Fe-B bonded magnets

A high potential cost-effective and environmentally friendly method has been applied for recycling anisotropic Nd-Fe-B bonded magnets. Waste additively printed Hydrogenation-Disproportionation-Desorption-Recombination (HDDR) Nd-Fe-B anisotropic bonded magnet was pulverized into composite powder containing Nd-Fe-B particles and nylon binder through cryomilling at a liquid nitrogen temperature (~77 K) under Ar inert atmosphere. Then, the cryomilled composite powder was warm compacted into a bonded magnet. Further, the magnetic particles were aligned during post-compaction annealing under a magnetic field of 30 kOe. The recycled bonded magnets have a higher density (3% enhancement), but slightly inferior magnetic properties compared to the original magnets, i.e., the magnetic remanence, coercivity and maximum energy product are reduced by 2%, 3% and 8%, respectively. The scanning electron microscopy revealed that some HDDR Nd-Fe-B powder crumbled into fine particles during cryomilling. Powder X-ray diffraction showed a small amount of Nd-oxide impurity in the cryomilled powder. The slightly deteriorated magnetic properties are ascribed to the oxidation of Nd-Fe-B particles due to formation of fresh fracture surface during cryomilling. The approach enables the direct reuse of end-of-life bonded magnets in an economical and environmentally friendly way.

36 MATERIALS SCIENCE

In situ oxidation of reduced graphene oxide membranes by peracetic acid for dye desalination

Graphene oxide (GO) membranes with tunable interlayer spacings are of interest for dye removal from salty textile wastewater, and the membranes are often reduced to improve their stability, which inevitably lowers water permeance. Herein, we demonstrate that reduced GO (rGO) membranes can be facilely modified using peracetic acid (PAA) in situ to dramatically enhance water permeance while retaining dye rejection. Specifically, PAA-modified membranes (PrGO) are synthesized by vacuum-filtering hydrazine-reduced rGO nanosheets onto Nylon substrate and then exposing them to PAA solutions. The effects of the rGO layer thickness, PAA content, and PAA exposure time on the membrane chemistry, nanostructures, and salt/dye separation properties are thoroughly examined. For example, the PAA oxidation of a 100 nm-thick rGO membrane for 10 min increases water permeance by 180 %, from 35 to 93 Liter m −2 h −1 bar −1 , and decreases Na 2 SO 4 rejection from 10 % to 3.3 % while retaining the rejection of Congo red at ≈99.7 %. The PrGO membranes exhibit stable water permeance and >99 % dye rejection in multi-cycle tests in a crossflow system, surpassing state-of-the-art GO membranes and showcasing their potential for practical applications.

Dye desalination

N 2 O deconstruction of polycyclooctene to generate carbonyl-functionalized macromonomers

Deconstruction of polyolefins into functionalized macromonomers presents a compelling strategy for polyolefin upcycling by creating macromonomers through dehydrogenation/depolymerization. We show that nitrous oxide (N 2 O), a greenhouse gas waste product from the production of nylon, mediates the deconstruction of polycyclooctene (PCOE) and generates carbonyl-functionalized macromonomers. Carbonyl incorporation and macromonomer molar mass were well controlled by reaction time, and subsequent hydrogenation readily removed residual carbon-carbon double bonds. Here, we also demonstrated that the reaction could progress efficiently with substrates of moderate levels of unsaturation, closely mimicking partially dehydrogenated polyethylene. Such carbonyl-functionalized macromonomers could serve as feedstock for preparing vitrimers and other functional polymers.

36 MATERIALS SCIENCE

Delamination recycling of multilayer plastic films: Solvent-assisted separation pathways and recovery of solid polyolefins

Multilayer plastic films are excellent packaging materials due to the bound layers of multiple polymers, with each different polymer contributing to the film properties. Desirable properties lead to continuously growing demand for multilayer films. Multilayer plastic films are typically single-use and, as such, their increased production and disposal have led to waste management problems. Multilayer films are not currently recyclable primarily due to the multiple bound polymers. This work advances delamination as a recycling process to separate and sequester valuable polymers from multilayer films, facilitating the incorporation of these polymers into the circular economy. We effect delamination in a physical process that preserves targeted polymers as solid film, hence retaining their embodied energy. This work documents three different pathways of inducing delamination of multilayer films, with appropriate solvents disrupting adhesion between adjacent layers or dissolving a minor component of the film in less than an hour and at temperatures below 90°C, and where all initial polyethylene is maintained in its solid form throughout the process and is recovered at high purity. Solvent-based delamination is exemplified on commercial multilayer films with majority polyethylene (PE), and polyethylene terephthalate (PET) or ethylene vinyl alcohol copolymer (EVOH) or nylon also present. Solvent-based delamination is an energy-efficient and environmentally friendly recycling process that improves upon dissolution-precipitation recycling, since delamination involves very little dissolution and no precipitation, and is superior to pyrolysis which breaks down the polymers, while delamination keeps polymer chains intact. Furthermore, delamination recycling can contribute to the sustainable use of multilayer films as they continue to protect our food and medicine.

Chemical Recycling