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At least 145 records · Page 8
All sourcesNASA NTRSDOE OSTI
DOE OSTI2023

Proteomes reveal metabolic capabilities of Yarrowia lipolytica for biological upcycling of polyethylene into high-value chemicals

ABSTRACT Polyolefins derived from plastic wastes are recalcitrant for biological upcycling. However, chemical depolymerization of polyolefins can generate depolymerized plastic (DP) oil, comprising of a complex mixture of saturated, unsaturated, even, and odd hydrocarbons suitable for biological conversion. While DP oil contains a rich carbon and energy source, it is inhibitory to cells. Understanding and harnessing robust metabolic capabilities of microorganisms to upcycle the hydrocarbons in DP oil, both naturally and unnaturally occurring, into high-value chemicals are limited. Here, we discovered that an oleaginous yeast, Yarrowia lipolytica, undergoing short-term adaptation to DP oil robustly utilized a wide range of hydrocarbons for cell growth and production of citric acid and neutral lipids. When growing on hydrocarbons, Y. lipolytica partitioned into planktonic and oil-bound cells with each exhibiting distinct proteomes and amino acid distributions invested in establishing these proteomes. Significant proteome reallocation toward energy and lipid metabolism, belonging to 2 of the 23 Eukaryotic Orthologous Groups classes C and I, enabled robust growth of Y. lipolytica on hydrocarbons, with n-hexadecane as the preferential substrate. This investment was even higher for growth on DP oil where classes C and I were ranked one and two, respectively, and many associated proteins and pathways were expressed and upregulated including the hydrocarbon degradation pathway, Krebs cycle, glyoxylate shunt and, unexpectedly, propionate metabolism. However, a reduction in proteome allocation for protein biosynthesis, at the expense of the observed increase toward energy and lipid metabolisms, might have caused the inhibitory effect of DP oil on cell growth. IMPORTANCE Sustainable processes for biological upcycling of plastic wastes in a circular bioeconomy are needed to promote decarbonization and reduce environmental pollution due to increased plastic consumption, incineration, and landfill storage. Strain characterization and proteomic analysis revealed the robust metabolic capabilities of Yarrowia lipolytica to upcycle polyethylene into high-value chemicals. Significant proteome reallocation toward energy and lipid metabolisms was required for robust growth on hydrocarbons with n-hexadecane as the preferential substrate. However, an apparent over-investment in these same categories to utilize complex depolymerized plastic (DP) oil came at the expense of protein biosynthesis, limiting cell growth. Taken together, this study elucidates how Y. lipolytica activates its metabolism to utilize DP oil and establishes Y. lipolytica as a promising host for the upcycling of plastic wastes.

1-alkenes↗
DOE OSTI2021

High Dose and Dose Rate 60 Co γ-Irradiation of High-Density Polyethylene

We have irradiated high-density polyethylene ribbons and cylinders to ~200 kGy at a dose rate of ~5 kGy day -1 , using a 60 Co source. The radiolytically-generated gas consists almost entirely of H 2 . Based on the time- and dose-dependence of the outgassing, we have determined the radiation- chemical yield for the evolved H 2 , as well as the diffusion coefficient of H 2 in HDPE. We find that the evolved gas yield G evolved depends on the interplay of sample geometry, experimental timescale, and the diffusion coefficient of H 2 in HDPE. When these factors facilitate completion of diffusion prior to gas quantification, such as for sub-mm-thickness ribbons, we measure a time- and dose-invariant value of G evolved = 0.0076 cm 3 std. H 2 J -1 that is in agreement with literature reports. When sample geometry and experiment timescale do not permit completion of diffusion, we measure a time- and dose-dependent value of G evolved . We have developed a model for the transient outgassing behavior of the cylinders, and fitted it to the experimental data. Based on these fits, we estimate a room-temperature diffusivity of D H 2 /HDPE ≈ 1.67 ± 0.12 x 10 -6 cm 2 s -1 for H 2 in HDPE, in good agreement with literature values. At present, the effects of dose rate and γ-photon energy on HDPE gas yield are not known and require further investigation.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Pulsed Sphere Time of Flight Neutron Spectrum Measurements: Blank Run and 1.8 Mean-Free-Path thick Polyethylene Moderating Sphere

From the late 1960s to 1985, Lawrence Livermore National Laboratory (LLNL) undertook a series of ‘pulsed sphere’ experiments for 32 materials involving 148 different experiments using 75 different spheres to measure the neutron leakage spectra for different materials from 14-MeV neutrons generated by 3 H(d, n) 4 He reactions induced by an incident D+ beam from the Insulated Core Transformer (ICT) accelerator at LLNL. This deuteron beam was focused to impinge on tritium loaded onto a titanium substrate within a low mass target assembly placed within the center of a spherical shell constructed from the material of interest. The neutron time of flight was measured at a detector outside a collimator. The program was intended to be comprehensive with numerous targets of various thicknesses spanning the periodic table from H to 239 Pu. Five different neutron detectors were utilized to avoid possible systematic errors due to differences in detector responses. Further, these measurements were designed with the aim that the simple geometry of the measurements could be easily simulated to validate Monte Carlo transport codes and nuclear data libraries. As a result, these benchmarks have been extensively used in the validation of ENDL, ENDF and other libraries. Two experiments selected as benchmark cases in this evaluation are: 1) target assembly without material sphere (blank run), and 2) target assembly with a hollow polyethylene sphere, 1.8 mean free path (mfp) or 16.56 cm thick.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2020

TEX-HEU: Integral Experiments with Highly Enriched Uranium and Polyethylene [Slides]

This presentation discusses Thermal/Epithermal eXperiments (TEX) in relation to integral experiments spanning a wide range of fission energy spectra utilizing existing NCSP fissile material assets, TEX-Pu for plutonium, and TEX-HEU highly enriched uranium (HEU) for highly enriched uranium. It also discusses the TEX-HEU design, the use of HEU fuel, and polyethylene parts. The experiment, executed in the Nuclear Criticality Experiment Research Center of the Nevada National Security Site is discussed, specifically how it was assembled on the Comet Universal Critical Assembly Machine. Measured quantities and various critical configurations are listed. In conclusion, the presentation states that they successfully assembled and documented the baseline TEX-HEU experiments, that six critical configurations and one reproducibility measurement were produced, and that they are compiling results to submit to the International Criticality Safety Benchmark Evaluation Project. A future experiment campaign is planned in 2021 with Hafnium as a diluent.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2025

A Semi-Detailed Pyrolytic Gas-Phase Kinetic Model for the Volatiles of Polyethylene Thermal Degradation

This work presents a semi-detailed kinetic model to address the pyrolytic gas-phase reactivity of volatiles formed during thermal degradation of polyethylene (PE). The model builds on a validated multi-step condensed-phase model and employs validated lumping approaches. Short-chain compounds are modelled with high detail, while long-chain ones are described by surrogate species representative of diesel-cuts (NC16H32) and waxes (NC30H60). The reactivity of short chains is described through the comprehensive CRECK kinetic model, updated to align C5-C7 olefins based on recent literature experimental data. Due to the lack of experimental data for longer olefins, their reactivity is modeled by analogy to the shorter ones, ensuring an asymptotic behavior with increasing carbon numbers. The semi-detailed model is validated through experimental data on PE pyrolysis, assuming an instantaneous mixing of the inert inlet flow with released volatiles, followed by a segregated plug-flow behavior. Validation across different reactor setups confirms the model’s capability to predict detailed product distributions. Despite minor discrepancies, the proposed model effectively captures experimental trends. Further work will address modelling the reactivity in oxygen-containing environments.

kinetics↗
DOE OSTI2024

High-Density Polyethylene Custom Focusing Lenses for High-Resolution Transient Terahertz Biomedical Imaging Sensors

Transient terahertz time-domain spectroscopy (THz-TDS) imaging has emerged as a novel non-ionizing and noninvasive biomedical imaging modality, designed for the detection and characterization of a variety of tissue malignancies due to their high signal-to-noise ratio and submillimeter resolution. We report our design of a pair of aspheric focusing lenses using a commercially available lens-design software that resulted in about 200 × 200-μm2 focal spot size corresponding to the 1-THz frequency. The lenses are made of high-density polyethylene (HDPE) obtained using a lathe fabrication and are integrated into a THz-TDS system that includes low-temperature GaAs photoconductive antennae as both a THz emitter and detector. The system is used to generate high-resolution, two-dimensional (2D) images of formalin-fixed, paraffin-embedded murine pancreas tissue blocks. The performance of these focusing lenses is compared to the older system based on a pair of short-focal-length, hemispherical polytetrafluoroethylene (TeflonTM) lenses and is characterized using THz-domain measurements, resulting in 2D maps of the tissue refractive index and absorption coefficient as imaging markers. For a quantitative evaluation of the lens effect on the image resolution, we formulated a lateral resolution parameter, R2080, defined as the distance required for a 20–80% transition of the imaging marker from the bare paraffin region to the tissue region in the same image frame. The R2080 parameter clearly demonstrates the advantage of the HDPE lenses over TeflonTM lenses. The lens-design approach presented here can be successfully implemented in other THz-TDS setups with known THz emitter and detector specifications.

47 OTHER INSTRUMENTATION↗
DOE OSTI2021

The Reactivity of Polyethylene Microplastics in Water under Low Oxygen Conditions Using Radiation Chemistry

Polyethylene (PE) is an intensely utilized polymer, which has consequently led to it becoming a common environmental contaminant. PE and other plastic waste are known to be highly persistent in surface waters; however, chemical and physical changes do take place over time, dependent mostly on highly variable natural conditions, such as oxygen (O2) availability. Gamma radiation was used to generate reactive oxygen species, namely hydroxyl radicals, in initially aerated aqueous solutions to simulate the natural weathering of microplastics in waters where there are fluctuations and often depletions in dissolved O2. The headspace of the irradiated PE-containing solutions was probed for the formation of degradation products using solid-phase microextraction (SPME) fibers in combination with gas chromatography mass spectrometry (GCMS). The major species detected were n-dodecane, with trace levels of tridecane, 2-dodecanone, and hexadecane, which were believed to be predominately adsorbed in the PE microplastics in excess of their aqueous solubility limits. Surface characterization by Raman spectroscopy and light and dark field microscopy indicated no change in the chemical composition of the irradiated PE microplastics under low O2 to anaerobic conditions. However, morphological changes were observed, indicating radical combination reactions.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2025

A Semi-Detailed Pyrolytic Gas-Phase Kinetic Model for the Volatiles of Polyethylene Thermal Degradation

This work presents a semi-detailed kinetic model to address the pyrolytic gas-phase reactivity of volatiles formed during thermal degradation of polyethylene (PE). The model builds on a validated multi-step condensed-phase model and employs validated lumping approaches. Short-chain compounds are modelled with high detail, while long-chain ones are described by surrogate species representative of diesel-cuts (NC16H32) and waxes (NC30H60). The reactivity of short chains is described through the comprehensive CRECK kinetic model, updated to align C5-C7 olefins based on recent literature experimental data. Due to the lack of experimental data for longer olefins, their reactivity is modeled by analogy to the shorter ones, ensuring an asymptotic behavior with increasing carbon numbers. The semi-detailed model is validated through experimental data on PE pyrolysis, assuming an instantaneous mixing of the inert inlet flow with released volatiles, followed by a segregated plug-flow behavior. Validation across different reactor setups confirms the model’s capability to predict detailed product distributions. Despite minor discrepancies, the proposed model effectively captures experimental trends. Further work will address modelling the reactivity in oxygen-containing environments.

kinetics↗
DOE OSTI2024

Environmental and economic analyses of chemical recycling via dissolution of waste polyethylene terephthalate

Globally, more than 1000 organizations and 175 nations are facing the plastic waste problem and have realized the need to transition from “linear-to-circular” economy of plastics. While the current mechanical recycling technologies for plastics are struggling to increase the U.S. plastic recycling rates beyond 9%, chemical recycling technologies become important complementary technologies to the predominant mechanical recycling that are needed to realize the circular economy in plastics supply chains. Dissolution is one such chemical recycling technology that can recycle waste plastic back into high-quality virgin grade plastic. However, the environmental and economic impacts of chemical recycling of waste polyethylene terephthalate (PET) via dissolution technology using a green solvent are unknown. Our study evaluated environmental metrics such as greenhouse gas (GHG) emissions and cumulative energy demand, and economic metrics such as net present value (NPV), minimum selling price, payback period, return on investment, and discounted internal rate of return for three dissolution processes with polymer recovery via anti-solvent, evaporation, and cooling precipitation techniques. The dissolution process with evaporation technique was the most economically favorable, whereas that with cooling technique was the most environmentally favorable. The anti-solvent approach had low economic performance and the highest environmental impacts. The NPV for all of these technologies ranged from $2.67 MM to $10.93 MM for a capacity of 8,400 MT/year and was found to be the highest for dissolution with evaporation approach and the least for anti-solvent approach. The cradle-to-gate GHG emissions and energy demand for PET dissolution processes ranged from 1.33-3.77 kg CO2-eq/kg of chemically recycled (CR) PET and18.9-56.1 MJ/kg of CR-PET, respectively. These economic and environmental metrics will be helpful in evaluating the sustainability of circular PET supply chains in the U.S.

09 BIOMASS FUELS↗
DOE OSTI2020

Stabilizing Zinc Anode Reactions by Polyethylene Oxide Polymer in Mild Aqueous Electrolytes

Abstract Zn dendrites growth and poor cycling stability are significant challenges for rechargeable aqueous Zn batteries. Zn metal deposition‐dissolution in aqueous electrolytes is typically determined by Zn anode–electrolyte interfaces. In this work, the role of a long‐chain polyethylene oxide (PEO) polymer as a multifunctional electrolyte additive in stabilizing Zn metal anodes is reported. PEO molecules suppress Zn 2+ ion transfer kinetics and regulate Zn 2+ ion concentration in the vicinity of Zn anodes through interactions between ether groups of PEO and Zn 2+ ions. The suppressed Zn 2+ ion transfer kinetics and homogeneous Zn 2+ ion distribution at the interface promotes dendrite‐free homogeneous Zn deposition. In addition, electrochemically inert PEO molecules adsorbed onto Zn anodes can protect the anode surfaces from H 2 generation and, thereby, enhance their electrochemical stability. Stable cycling over 3000 h and high reversibility (Coulombic efficiency > 99.5%) of Zn anodes is demonstrated in 1 m ZnSO 4 electrolyte with 0.5 wt% PEO. This finding provides helpful insights into the mechanism of Zn metal anodes stabilization by low‐cost multifunctional polymer electrolyte additives that stabilize interfacial reactions.

Jin, Yan↗
DOE OSTI2020

Polyethylene Terephthalate Deconstruction Catalyzed by a Carbon‐Supported Single‐Site Molybdenum‐Dioxo Complex

Abstract Polyethylene terephthalate (PET) is selectively depolymerized by a carbon‐supported single‐site molybdenum‐dioxo catalyst to terephthalic acid (PTA) and ethylene. The solventless reactions are most efficient under 1 atmosphere of H 2 . The catalyst exhibits high stability and can be recycled multiple times without loss of activity. Waste beverage bottle PET or a PET + polypropylene (PP) mixture (simulating the bottle + cap) proceeds at 260 °C with complete PET deconstruction and quantitative PTA isolation. Mechanistic studies with a model diester, 1,2‐ethanediol dibenzoate, suggest the reaction proceeds by initial retro‐hydroalkoxylation/β‐C−O scission and subsequent hydrogenolysis of the vinyl benzoate intermediate.

Kratish, Yosi↗
DOE OSTI2022

Catalytic Degradation of Polyethylene Terephthalate Using a Phase‐Transitional Zirconium‐Based Metal–Organic Framework

Abstract Polyethylene terephthalate (PET) is utilized as one of the most popular consumer plastics worldwide, but difficulties associated with recycling PET have generated a severe environmental crisis with most PET ending its lifecycle in landfills. We report that zirconium‐based metal–organic framework (Zr‐MOF) UiO‐66 deconstructs waste PET into the building blocks terephthalic acid (TA) and mono‐methyl terephthalate (MMT) within 24 hours at 260 °C (total yield of 98 % under 1 atm H 2 and 81 % under 1 atm Ar). Extensive structural characterization studies reveal that during the degradation process, UiO‐66 undergoes an intriguing transformation into MIL‐140A, which is another Zr‐MOF that shows good catalytic activity toward PET degradation under similar reaction conditions. These results illustrate the diversity of applications for Zr‐MOFs and establish MOFs as a new class of polymer degradation catalysts with the potential to address long‐standing challenges associated with plastic waste.

Wu, Yufang↗
DOE OSTI2023

Polyethylene Incorporating Diels–Alder Comonomers: A “Trojan Horse” Strategy for Chemically Recyclable Polyolefins

Abstract Polyolefins with periodic unsaturation in the backbone chain are sought after for synthesizing chemically recyclable polymers or telechelic polyolefin macromonomers. Here we introduce a bottom‐up synthesis of unsaturated high‐density polyethylene (HDPE) via copolymerization of ethylene with dimethyl 7‐oxabicyclo[2.2.1]hepta‐2,5‐diene‐3,5‐dicarboxylate followed by post‐polymerization retro‐Diels–Alder to unveil hidden double bonds in the polymer backbone. The incorporation of this “Trojan Horse” comonomer was varied and a series of unsaturated HDPE polymers with block lengths of 1.2, 1.9, and 3.5 kDa between double bonds was synthesized. Cross metathesis of unsaturated HDPE samples with 2‐hydroxyethyl acrylate yielded telechelic ester terminated PE macromonomers suitable for the preparation of ester‐linked PE. These materials were depolymerized and repolymerized, making them suitable candidates for chemical recycling. The ester‐linked PE displayed thermal and mechanical properties comparable to commercial HDPE.

Parke, Sarah M.↗
DOE OSTI2024

A Vitrimer Acts as a Compatibilizer for Polyethylene and Polypropylene Blends

Abstract Polymer compatibilization plays a critical role in achieving polymer blends with favorable mechanical properties and enabling efficient recycling of mixed plastic wastes. Nonetheless, traditional compatibilization methods often require tailored designs based on the specific chemical compositions of the blends. In this study, we propose a new approach for compatibilizing polymer blends using a dynamically crosslinked polymer network, known as vitrimers. By adding a relatively small amount (1–5 w/w%) of a vitrimer made of siloxane‐crosslinked high‐density polyethylene (HDPE), we successfully compatibilized unmodified HDPE and isotactic polypropylene (iPP). The vitrimer‐compatibilized blend exhibited enhanced elongation at break (120 %) and smaller iPP domain sizes (0.4 μm) compared to the control blend (22 % elongation at break, 0.9 μm iPP droplet size). Moreover, the vitrimer‐compatibilized blend showed significantly improved microphase stability during annealing at 180 °C. This straightforward method shows promise for applications across various polymer blend systems.

Yokoyama, Kosuke↗
DOE OSTI2022

Catalytic Degradation of Polyethylene Terephthalate Using a Phase-Transitional Zirconium-Based Metal–Organic Framework

Polyethylene terephthalate (PET) is utilized as one of the most popular consumer plastics worldwide, but difficulties associated with recycling PET have generated a severe environmental crisis with most PET ending its lifecycle in landfills. We report that zirconium-based metal–organic framework (Zr-MOF) UiO-66 deconstructs waste PET into the building blocks terephthalic acid (TA) and mono-methyl terephthalate (MMT) within 24 hours at 260 °C (total yield of 98 % under 1 atm H 2 and 81 % under 1 atm Ar). Extensive structural characterization studies reveal that during the degradation process, UiO-66 undergoes an intriguing transformation into MIL-140A, which is another Zr-MOF that shows good catalytic activity toward PET degradation under similar reaction conditions. Here these results illustrate the diversity of applications for Zr-MOFs and establish MOFs as a new class of polymer degradation catalysts with the potential to address long-standing challenges associated with plastic waste.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Polyethylene Incorporating Diels–Alder Comonomers: A “Trojan Horse” Strategy for Chemically Recyclable Polyolefins

Polyolefins with periodic unsaturation in the backbone chain are sought after for synthesizing chemically recyclable polymers or telechelic polyolefin macromonomers. Here we introduce a bottom-up synthesis of unsaturated high-density polyethylene (HDPE) via copolymerization of ethylene with dimethyl 7-oxabicyclo[2.2.1]hepta-2,5-diene-3,5-dicarboxylate followed by post-polymerization retro-Diels–Alder to unveil hidden double bonds in the polymer backbone. The incorporation of this “Trojan Horse” comonomer was varied and a series of unsaturated HDPE polymers with block lengths of 1.2, 1.9, and 3.5 kDa between double bonds was synthesized. Cross metathesis of unsaturated HDPE samples with 2-hydroxyethyl acrylate yielded telechelic ester terminated PE macromonomers suitable for the preparation of ester-linked PE. These materials were depolymerized and repolymerized, making them suitable candidates for chemical recycling. Here, the ester-linked PE displayed thermal and mechanical properties comparable to commercial HDPE.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗