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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 73 records · Page 4
All sourcesNASA NTRSDOE OSTI
DOE OSTI2025

Influence of functional additives, fillers, and pigments on thermal and catalytic pyrolysis of polyethylene for waste plastic upcycling

Pyrolysis offers a relatively green and economical method to convert waste plastics into valuable chemicals and fuels without the need for harmful solvents, toxic chemicals, or costly high-pressure reactors. Despite its popularity among chemical upcycling technologies, industrial adoption suffers from feedstock heterogeneity, low-quality products, and catalyst deactivation. Most plastics in our daily lives are formulated with functional additives, fillers, and colorants. These additives remaining in end-of-life waste streams increase feedstock heterogeneity, creating a challenging issue in recycling plastics. Still, the potential impacts of additives on the chemical upcycling of plastics have been poorly understood. In this study, polyethylene compounded with a range of widely used additives (antioxidants, stabilizers, pigments, fillers, slip agents, and flame retardants) was subjected to both thermal pyrolysis and catalytic pyrolysis in different catalyst-to-feedstock contact modes. It showed that many inorganic additives, such as talc, kaolin, CaCO 3 , TiO 2 , carbon black, and zinc stearate, facilitated polymer decomposition during pyrolysis, increasing light hydrocarbons while also promoting aromatic and carbon residue formation. Conversely, antioxidants and stabilizers inhibited depolymerization, favoring heavier hydrocarbons. During catalytic pyrolysis with HZSM-5 zeolite, additives strongly enhanced aromatic and catalytic coke formation, especially when there was direct contact between plastics and catalysts. Although certain additives seem beneficial in the short term by promoting polymer cracking and improving the selectivity of aromatics, the transport of the additives and their degradation products and increased carbon coking can contaminate products, deactivate or modify catalysts, and foul reactors. These findings address a critical knowledge gap in effectively converting waste plastics via a greener route.

42 ENGINEERING↗
DOE OSTI2026

Recent advances in chemical recycling and upcycling of plastic waste into valuable materials, chemicals, and energy: a comprehensive review

The global plastic waste crisis has increased in severity in recent years: annual plastic production is projected to reach 500 million metric tons by 2025, and plastic waste accumulation is expected to surpass 12 billion metric tons. Despite these growing volumes, only ∼9% of plastic waste is currently recycled; the majority is either landfilled, incinerated, or mismanaged, contributing to escalating greenhouse gas emissions—from 1.7 Gt carbon dioxide equivalent (CO 2 -eq.) in 2015 to an estimated 6.5 Gt CO 2 -eq. by 2050—and physical environmental pollution. This review provides a comprehensive overview of advanced plastic upcycling strategies to address this issue and recover value from diverse plastic waste streams. Recent developments in solvent-based dissolution, chemical depolymerization, and thermochemical conversions are examined for major plastic types, including polyolefins, polycondensation polymers, and PVC. Underlying reaction pathways, catalyst designs, and processing parameters that govern product selectivity, efficiency, and conversion yields are discussed in depth. Emerging techniques such as microwave-assisted depolymerization, tandem catalysis, and co-processing approaches are highlighted for their potential to enhance efficiency under milder conditions. Emphasis is also placed on the production of high-value products such as monomers, naphtha-range hydrocarbons, and syngas, and discussion is provided on catalyst stability, contaminant removal, scalability, life cycle effects on the environment, and technoeconomic viability. Finally, the review outlines future research directions focused on catalyst innovation, integrated process design, supportive policy frameworks, and interdisciplinary collaboration. All recommendations are aimed at accelerating large-scale implementation of plastic upcycling technologies and advancing the global circular plastics economy.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

A New Approach to Fundamental Mechanism Discovery in Polymer Upcycling

We present a new experimental methodology for detailed experimental investigations of depolymerization reactions over solid catalysts. This project aims to address a critical need in fundamental research on chemical upcycling of polymers – the lack of rapid, sensitive, isomerselective probing techniques for the detection of reaction intermediates and products. Our method combines a heterogeneous catalysis reactor for the study of multiphase (gas/polymer melt/solid) systems, coupled to a vacuum UV photoionization time-of-flight mass spectrometer. This apparatus draws on our expertise in probing complex gas-phase chemistry and enables highthroughput, detailed chemical speciation measurements of the gas phase above the catalyst, providing valuable information on the heterogeneous catalytic reactions. Using this approach, we investigated the depolymerization of high-density polyethylene (HDPE) over Ir-doped zeolite catalysts. We showed that the product distribution was dominated by low-molecular weight alkenes with terminal C=C double bonds and revealed the presence of many methyl-substituted alkenes and alkanes, suggesting extensive methyl radical chemistry. In addition, we investigated the fundamental reactivity of model oligomer molecules n-butane and isobutane over ZSM-5 zeolites. We demonstrated the first direct detection of methyl radical intermediates, confirming the key role of methyl in zeolite-catalyzed activation of alkanes. Our results show the potential of this experimental method to achieve deep insight into the complex depolymerization reactions and pave the way for detailed mechanistic studies, leading to increased fundamental understanding of key processes in chemical upcycling of polymers.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

Upcycling Polyethylene Waste to Advanced Carbon Materials for Energy Storage Applications

Polyethylene is notoriously difficult to upcycle because it decomposes into light gases at approximately 350-400 °C which prevents processing it at higher temperatures to convert it into high-value carbon materials, such as graphene or graphite. We address this challenge by using an air-based, thermo-oxidation process, which heats polyethylene (PE) just below the decomposition point to initiate oxidation and cross-linking of PE alkyl chains. These molecular transformations allow PE to be further graphenized or graphitized at higher temperatures without decomposing. The PE-derived graphene has a specific surface area up to 1,800 m 2/g and Raman ID/IG ratio of 0.85, which enables it to be used as an electrode material for a symmetric supercapacitor with the 1 M H2SO4 electrolyte. The PE-derived graphene material has a comparable electrochemical capacitive performance, such as power density, specific capacitance, and long cycle stability, to the commercial state of art porous carbon electrode. The stabilized PE could also be converted into highly crystalline flake graphite via low-temperature catalytic graphitization. The PE-derived graphite is used for the lithium-ion battery anode, which showed comparable electrochemical battery performance, such as reversible rate performance and long-term cyclic stability, to the current use battery-grade graphite, thus providing a scalable method to upcycle PE plastic waste into high-value carbon material.

Gao, Yuan↗
DOE OSTI2024

Upcycling Low Linear Density Polyethylene Waste into Turbostratic Graphene for High Mass Loading Supercapacitors

In this work, LLDPE was upcycled into a high quality turbostratic graphene using a pre-treatment step to oxidatively crosslink the polymer with the assistance of solid additives (KCl and K2CO3) that improve crosslinking by increasing the effective surface area of the polymer melt during processing. After this pretreatment step, the crosslinked polymer could then be carbonized and catalytically graphenized between 400-950 °C without complete decomposition of the material. The LLDPE derived graphene (LLDPE-G) obtained from this process has a Brunauer–Emmett–Teller (BET) specific surface area, up to 1800 m2g-1 and average Raman ID/IG and I2D/IG ratios of 0.85 and 0.57, respectively, indicating high quality graphene. When used as an electrode material in symmetric supercapacitors, LLDPE-G possesses an outstanding specific capacitance up to 175 Fg-1 at a mass loading of 20 mgcm-2, which is two times the commercial requirement, yielding an excellent areal capacitance of 3.5 Fcm-2. Moreover, LLDPE-G exhibits exceptional cycling stability with a capacitance retention of 95.8% after 100,000 cycles at a current density of 4.0 Ag-1. Additionally, the KCl and K2CO3 were recycled and reused over 3 complete cycles to make new LLDPE-G with the material quality and electrocapacitive performance retained and verified after each cycle. Our approach creates new opportunities for upcycling not only waste LLDPE but also other varieties of PE to high value graphene materials.

Gao, Yuan [NETL Site Support Contractor, National ↗
DOE OSTI2020

Today’s Energy Challenges, Tomorrow’s Solutions: Circular Economy: Designing to Reduce, Reuse, and Upcycle

Transitioning to a Circular Economy the days of creating, using, and disposing of materials are rapidly coming to a close. This linear economy is not only inefficient and unsustainable, but the scarcity of resources we ultimately will face will make it impossible to maintain. That's why NREL is dedicating resources to research that will underpin a circular economy - designing materials with reducing, reusing, and upcycling in mind for energy-relevant and energy-intensive materials, processes, and technologies. This effort will help mitigate supply issues, promote upcycling, reduce waste, and add value to end-of-life products.

circular economy↗
DOE OSTI2025

Cathode Upcycling for Direct Recycling of Lithium‐Ion Batteries Using a Precipitation Approach

With the increased production of electric vehicles to reduce carbon emissions, the lithium-ion battery market to supply those vehicles has grown dramatically. To enhance battery sustainability and circularity, direct recycling methods aim to recover intact cathode materials. However, end-of-life cathode materials are typically 15–20 years old and often have lower energy density compared to current cathode materials. To address this challenge, a rapid precipitation process is developed to boost energy density by converting low Ni-compositions, LiNi 0.33 Co 0.33 Mn 0.33 O 2 (NMC111), into higher Ni-compositions (NMC622). This process forms a Ni-rich coating on cathode particles that diffuses into the core upon high-temperature relithiation, increasing compositional homogeneity. The upcycling process leverages existing infrastructure, offering low capital cost and minimal additional chemical input. Through ex situ tomographic transmission X-ray microscopy (TXM), 3D Ni:Co elemental mixing is quantified, confirming that elemental content evens at the secondary particle level with a mean NMC622 composition upon relithiation. However, elemental gradients remain in the single crystalline primary particles. Ex situ high-resolution and in situ wide-angle X-ray diffraction reveals concurrent structural changes during the relithiation process. These findings provide key insights into the structural and chemical mechanisms of elemental diffusion to obtain further improvements of increased capacity and retention through compositional conversion of cathode materials.

Cathode Upcycling↗
DOE OSTI2025

Bio‐Inspired Cascade Photocatalysis on Fe Single‐Atom Carbon Nitride Upcycles Plastic Wastes for Effective Acetic Acid Production

Plastic imposes a critical threat to the environment, ecosystems, and human health because of the low utilization efficiency of plastics. Here, we demonstrate a sustainable, highly efficient cascade photocatalysis for upcycle plastics to value-added acetic acid using Fe single-atom catalysts (Fe@C 3 N 4 SAC) at ambient conditions. Inspired by Phanerochaete chrysosporium microbial, the defective Fe@C 3 N 4 SAC acts as a bifunctional cascade photocatalyst for both Fenton-like and CO 2 reduction reactions. During the reaction, hydroxyl radicals (*OH) form and subsequently oxidize plastics into CO 2 intermediates. These CO 2 intermediates are then photo-reduced to CH 3 COOH on the same catalyst via cascade photocatalysis. The mechanism is confirmed by in situ multimodal microscopy and spectroscopies, with density functional theory calculations. A state-of-art CH 3 COOH yield of 63.8 mg h −1 gcat −1 from PVC, 12.7 mg h −1 gcat −1 from PE, 5.4 mg h −1 gcat −1 from PET, and 5.3 mg h −1 gcat −1 from PP are directly obtained under AM1.5G solar irradiation and further validated under real sunlight (≈0.6 sun), achieving 5.6 mg h −1 gcat −1 from PET, using low-cost Fe@C 3 N 4 SAC in a sealed reactor by enhancing the photon transport and utilization efficiency. The techno-economic analysis shows it is promising to practically mitigate plastic based on broader social welfare assessments.

cascade photocatalysis↗
DOE OSTI2024

Chloride and Hydride Transfer as Keys to Catalytic Upcycling of Polyethylene into Liquid Alkanes

Abstract Transforming polyolefin waste into liquid alkanes through tandem cracking‐alkylation reactions catalyzed by Lewis‐acid chlorides offers an efficient route for single‐step plastic upcycling. Lewis acids in dichloromethane establish a polar environment that stabilizes carbenium ion intermediates and catalyzes hydride transfer, enabling breaking of polyethylene C−C bonds and forming C−C bonds in alkylation. Here, we show that efficient and selective deconstruction of low‐density polyethylene (LDPE) to liquid alkanes is achieved with anhydrous aluminum chloride (AlCl 3 ) and gallium chloride (GaCl 3 ). Already at 60 °C, complete LDPE conversion was achieved, while maintaining the selectivity for gasoline‐range liquid alkanes over 70 %. AlCl 3 showed an exceptional conversion rate of 5000 , surpassing other Lewis acid catalysts by two orders of magnitude. Through kinetic and mechanistic studies, we show that the rates of LDPE conversion do not correlate directly with the intrinsic strength of the Lewis acids or steric constraints that may limit the polymer to access the Lewis acid sites. Instead, the rates for the tandem processes of cracking and alkylation are primarily governed by the rates of initiation of carbenium ions and the subsequent intermolecular hydride transfer. Both jointly control the relative rates of cracking and alkylation, thereby determining the overall conversion and selectivity.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2025

Advances and Challenges in Low‐Temperature Upcycling of Waste Polyolefins via Tandem Catalysis

Abstract Polyolefin waste is the largest polymer waste stream that could potentially serve as an advantageous hydrocarbon feedstock. Upcycling polyolefins poses significant challenges due to their inherent kinetic and thermodynamic stability. Traditional methods, such as thermal and catalytic cracking, are straightforward but require temperatures exceeding 400 °C for complete conversion because of thermodynamic constraints. We summarize and critically compare recent advances in upgrading spent polyolefins and model reactants via kinetic (and thermodynamic) coupling of the endothermic C─C bond cleavage of polyolefins with exothermic reactions including hydrogenation, hydrogenolysis, metathesis, cyclization, oxidation, and alkylation. These approaches enable complete conversion to desired products at low temperatures (<300 °C). The goal is to identify challenges and possible pathways for catalytic conversions that minimize energy and carbon footprints.

C-C cleavage↗
DOE OSTI2025

Reciprocal Ternary Molten Salts Enable the Direct Upcycling of Spent Lithium‐Nickel‐Manganese‐Cobalt Oxide (NMC) Mixtures to Make NMC 622

Cathode active material is the most valuable component of spent lithium‐ion batteries, accounting for ≈30% of their overall value. Direct recycling of cathode materials involves recovering, regenerating, and reusing them without breaking down their chemical structure. This approach maximizes the added value of the cathode compound and reduces manufacturing costs by avoiding the need for virgin material production. However, one key challenge in scaling direct recycling from lab to industry is the requirement for highly purified cathode materials, contrasting with the low purity of black mass generated from battery shredding. No efficient separation process currently exists to isolate different lithium‐nickel‐manganese‐cobalt oxides (NMCs) from each other. Thus, direct recycling technologies that can operate with mixtures of multiple NMC stoichiometries will be best‐suited for industrial adoption. This study explores the direct recycling of NMC mixtures into NMC 622 using a “reciprocal ternary molten salts (RTMS)” system. Ionothermal relithiation and upcycling within the RTMS system successfully restore the layered structure, lithium content, and electrochemical performance of degraded NMCs, yielding results comparable to pristine NMC 622 (P‐NMC 622).

25 ENERGY STORAGE↗
DOE OSTI2023

Bona fide upcycling strategy of anhydride cured epoxy and reutilization of decomposed dual monomers into multipurpose applications

Waste epoxy materials become an enormous problem to society and the environment. The advantages of epoxy resins derive from their rigid and chemically stable networks, but these qualities also make them difficult to dispose of or recycle. In this work, we demonstrated an efficient degradation of anhydride cured epoxy resin by aminolysis in aminoethanol without using any catalysts. The epoxy resin was fully decomposed at 160 °C in 4 h, resulting in two distinct high purity monomers (HHPA-OH and BPA-OH). To fully realize this upcycling approach, The BPA-OH was used to synthesize a polyurethane coating with an excellent glass transition temperature (88.9 °C), scratch hardness (8H), gouge hardness (6H), adhesive strength (5B), and strong solvent resistance. The HHPA-OH with two hydroxyl groups was reacted with methacrylic anhydride to form a dimethacrylate monomer which was then used as a viable crosslinker for photo-curable 3D printing thermosetting polymer with tensile strength as high as 64 MPa and impact strength of 4.86 kJ/m 2 . This work demonstrates a feasible pathway to convert anhydride cured epoxy waste to new monomeric recyclates for superior polymer products.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2026

Elucidation of odd-chain dicarboxylate metabolism in Acinetobacter baylyi and application to polyethylene upcycling

Polyethylene (PE) is a versatile polymer, but its end-of-life management is challenging due to its recalcitrant structure. We present a promising approach combining chemical degradation and bio-upcycling to convert postconsumer PE waste into a value-added bioproduct. Specifically, PE was degraded into acetic acid and C 4 –C 7 dicarboxylic acids by nitric acid. We then elucidated the catabolic pathways for glutarate (C 5 ) and pimelate (C 7 ) in the nonmodel bacterium Acinetobacter baylyi ADP1 through RNA sequencing, phenotyping, and enzymatic assays. Whole-genome sequencing of evolved isolates also identified a crucial IclR family transcriptional regulator, DcaS, which acts as a repressor of dicarboxylate metabolism. The reverse-engineered strain exhibited enhanced substrate utilization compared to the wild-type strain. Using rational metabolic engineering, the PE deconstruction products were bioconverted into the valuable chemical lycopene, highlighting the potential of this microbial chassis to produce value-added bioproducts from postconsumer PE waste, thus promoting a circular economy for plastics.

metabolic engineering↗
DOE OSTI2022

Value-creating upcycling of retired electric vehicle battery cathodes

The electrification revolution in the automobile and other industries demands annual production capacity of batteries of at least 10 2 GWh, which presents a twofold challenge: supply of key materials such as cobalt and nickel and recycling when batteries are retired from use. Pyrometallurgical and hydrometallurgical recycling are currently used in industry but suffer from complexity, high costs, and secondary pollution. Here we report a molten-salt-based method for direct recycling (MSDR) that is environmentally benign and creates value on the basis of a techno-economic analysis using real-world data and price information. We also experimentally demonstrate the feasibility of MSDR by upcycling a low-nickel polycrystalline LiNi 0.5 Mn 0.3 Co 0.2 O 2 (NMC) cathode material into Ni-rich (Ni > 65%) single-crystal NMCs with increased energy density (>10% increase) and outstanding electrochemical performance (>94% capacity retention after 500 cycles). This work may open opportunities for closed-loop recycling of electric vehicle batteries and manufacturing of next-generation NMC cathode materials.

25 ENERGY STORAGE↗
DOE OSTI2025

Tailored glycolysis of Nylon 6 to enable upcycling into high-strength adhesives

Nylon is a high-strength polyamide widely used in automotive, textiles, packaging, etc. However, its durability makes nylon waste difficult to manage, with recycling limited to mechanical grinding to make fillers. Here, we report a catalytic glycolysis approach to deconstruct Nylon 6 into controlled-length oligomers, enabling upcycling into value-added materials. A low-molecular-weight oligomer (M n = 1.8 kg/mol) was repolymerized with diepoxy-terminated poly(bisphenol A-co-epichlorohydrin) via mechanochemistry to create a high-performance adhesive. This copolymer achieves lap shear strengths over 22 MPa on steel and bonds steel to carbon fiber composites, nearly tripling the performance of commercial adhesives even at 90°C. Thermomechanical analyses show that the adhesive retains thermal stability similar to nylon 6 but melts at lower temperatures, allowing easier processing. The material can be reprocessed and reused without significant performance loss. This study demonstrates a strategy to convert nylon 6 waste into valuable materials, offering a sustainable path for difficult-to-recycle plastics.

Nylon waste↗
DOE OSTI2026

Techno-Economic and Life Cycle Assessment of Chemical Recycling and Upcycling of Mixed Plastics Waste Containing Poly-vinyl-chloride

Developing technologies that completely remove chlorine from plastic waste can allow its chemical recycling and upcycling with catalytic methods. Here, this study compares eight processes involving different dechlorination methods (absorption columns, adsorption in beds of zeolites, catalytic dechlorination, and dissolution in ionic liquids) and chemical conversion technologies (incineration, pyrolysis, hydrogenolysis) to upgrade mixed plastics waste to various products (e.g., electricity, fuels, virgin polymers, and lubricant oil). The analysis determines that the absorption of chlorine in columns with basic aqueous solutions is limited to plastics waste with PVC concentrations below 0.1%. Dissolution in ionic liquids is not cost-competitive. On the contrary, two-step processes with catalytic dechlorination followed by thermochemical catalytic depolymerization, either pyrolysis or hydrogenolysis, significantly improve process economics and emissions. The most economically viable alternative is hydrogenolysis for producing lubricants, while the technology with the lowest global warming potential is chemical recycling via catalytic pyrolysis.

circular economy↗
DOE OSTI2025

Engineering microbial consortia for mixed plastic upcycling

Recent studies in developing processes using ‘single’ plastic waste for microbial conversion have demonstrated great promise in advancing a circular economy. However, chemical complexity and compositional variability of post-consumer ‘mixed’ plastic waste pose huge challenges to using it as a feedstock for biomanufacturing. Here, we present a process leveraging a synthetic microbial consortium, comprising Rhodococcus jostii strain PET and Acinetobacter baylyi ADP1, enabled by engineering the division of labor. The robust consortium synergistically and stably consumes diverse mixtures of oxygenated compounds, derived from the depolymerization of post-consumer, mixed plastic waste, regardless of the fluctuating plastic waste compositions. We evaluate the upcycling potential of the stable consortium by applying rational metabolic engineering to both specialists, enabling the funneling of these oxygenates into lycopene and lipids. This work highlights the potential of stable microbial consortia to valorize untapped, mixed plastic waste for sustainable biomanufacturing, offering a promising solution to global plastic pollution.

60 APPLIED LIFE SCIENCES↗