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All sources NASA NTRS DOE OSTI

DOE OSTI2024

Unraveling the Pyrolytic Behavior and Kinetics of Single Polymers and Plastic-Rich Municipal Solid Waste Using Thermal Analysis

Pyrolysis is a highly promising thermochemical recycling technology for converting heterogenous plastic waste into sustainable fuels in a single step. Therefore, understanding the pyrolysis mechanism is essential for enabling rational reactor design and enhancing efficient recycling techniques. In this study, the thermal degradation behaviors and corresponding kinetics of pure polymers (PE, PP, and PET) and plastic-rich MSW were examined using simultaneous thermogravimetric analysis (TGA) and differential scanning calorimetry (DSC). Experiments were carried out in the temperature range of 30-800°C with variable heating rates from 5°C/min to 20°C/min in an ultra-high purity Argon atmosphere. Our results indicated that the plastic pyrolysis was an endothermic process, with varying decomposition temperature ranges depending on their structure and composition. Various iso-conversional model-free methods (Friedman, Flynn-Wall-Ozawa, Starink, and Kissinger-Akahira-Sunose) were utilized to determine the apparent activation energy of the plastic degradation, which increased in the following order: PET (214 kJ/mol), PP (218 kJ/mol), PE (245 kJ/mol), and MSW (249 kJ/mol). Finally, Criado’s master plots were employed to identify the best-fitting reaction model and the pre-exponential factor was subsequently determined.

Bashir, Muhammad Aamir↗

DOE OSTI2021

Pycheron: A Python-Based Seismic Waveform Data Quality Control Software Package

Supplementing an existing high-quality seismic monitoring network with openly available station data could improve coverage and decrease magnitudes of completeness; however, this can present challenges when varying levels of data quality exist. Without discerning the quality of openly available data, using it poses significant data management, analysis, and interpretation issues. Incorporating additional stations without properly identifying and mitigating data quality problems can degrade overall monitoring capability. If openly available stations are to be used routinely, a robust, automated data quality assessment for a wide range of quality control (QC) issues is essential. To meet this need, we developed Pycheron, a Python-based library for QC of seismic waveform data. Pycheron was initially based on the Incorporated Research Institutions for Seismology’s Modular Utility for STAtistical kNowledge Gathering but has been expanded to include more functionality. Pycheron can be implemented at the beginning of a data processing pipeline or can process stand-alone data sets. Its objectives are to (1) identify specific QC issues; (2) automatically assess data quality and instrumentation health; (3) serve as a basic service that all data processing builds on by alerting downstream processing algorithms to any quality degradation; and (4) improve our ability to process orders of magnitudes more data through performance optimizations. This article provides an overview of Pycheron, its features, basic workflow, and an example application using a synthetic QC data set.

58 GEOSCIENCES↗

DOE OSTI2023

Increased range and contrast in fog with circularly polarized imaging

Fogs, low lying clouds, and other highly scattering environments pose a challenge for many commercial and national security sensing systems. Current autonomous systems rely on optical sensors for navigation whose performance is degraded by highly scattering environments. In our previous simulation work, we have shown that polarized light can penetrate through a scattering environment such as fog. We have demonstrated that circularly polarized light maintains its initial polarization state better than linearly polarized light, even through large numbers of scattering events and thus ranges. This has recently been experimentally verified by other researchers. In this work, we present the design, construction, and testing of active polarization imagers at short-wave infrared and visible wavelengths. We explore multiple polarimetric configurations for the imagers, focusing on linear and circular polarization states. The polarized imagers were tested at the Sandia National Laboratories Fog Chamber under realistic fog conditions. Here, we show that active circular polarization imagers can increase range and contrast in fog better than linear polarization imagers. We show that when imaging typical road sign and safety retro-reflective films, circularly polarized imaging has enhanced contrast throughout most fog densities/ranges compared to linearly polarized imaging and can penetrate over 15 to 25 m into the fog beyond the range limit of linearly polarized imaging, with a strong dependence on the interaction of the polarization state with the target materials.

47 OTHER INSTRUMENTATION↗

DOE OSTI2024

Properties and Autoignition Reactivity of Diesel Boiling Range Ethers Produced from Guerbet Alcohols

We examine the properties of diesel boiling range ethers made from coupling of alcohols produced by oligomerization of ethanol (Guerbet alcohols) for their utility as low-carbon liquid fuel blendstocks. Basic properties of boiling point, flash point, freezing point, density and viscosity are well suited for blending into diesel fuels. For the mixture of ethers the lightest component, di-n-butyl ether, can be present at up to 20 vol% while still having adequately high flashpoint for safe handling. Soot formation tendency (as yield sooting index) is well below that of conventional diesel. The ethers have similar compatibility with elastomers as conventional diesel, based on Hansen solubility parameter analysis. Oxidation stability was assessed for 30 vol% blends of individual ethers in a conventional diesel fuel using a long-term storage test. Over 6 weeks we observed no formation of peroxides or degradation. n-alkyl ethers with carbon number of 8 or higher have cetane number over 100, which is outside the defined range of cetane number, while branched ethers are over 70. The ethers also blend antagonistically into conventional diesel for cetane number, meaning that the blend cetane value is lower than predicted based on a linear by volume, mass, or mole model. We show that aromatics and naphthenes likely act as radical scavengers to slow or shut down autoignition of the highly reactive ethers at low to medium blend levels. Overall, diesel boiling range ethers show significant promise as high quality low-net carbon diesel blendstocks.

09 BIOMASS FUELS↗

DOE OSTI2026

Machine Learning Calibration of Groundwater Table Depth in ELM: Impact on Land Surface Hydrology and Land‐Atmosphere Fluxes

Accurate representation of groundwater table depth (GWTD) is crucial for simulating hydrological cycling in Earth system models (ESM). Nevertheless, there is a notable gap in the literature regarding the validation of GWTD simulations in ESMs and their subsequent impact on downstream hydrological components. This study explores the calibration of parameterization of global GWTD using machine learning within the Energy Exascale Earth System Model (E3SM) Land Model (ELM). Despite achieving significant gains in simulating GWTD through calibration, offline ELM simulations unexpectedly show that these improvements do not translate to substantial enhancements in model performance for other key hydrological variables, including soil moisture (SM), runoff, groundwater contribution to runoff or base flow index (BFI), and evapotranspiration and its partitioning. The performance in SM and runoff was even degraded in some regions, while BFI was mostly overestimated. Although there is significant improvement in GWTD within the critical range of 1–5 m, where groundwater traditionally influences land surface energy fluxes, these improvements occurred mostly in humid areas where the impact of GWTD on surface processes is minimal. Although the impacts of model calibration are generally small in offline ELM simulations, coupled land-atmosphere simulations exhibit much stronger responses to GWTD calibration, highlighting the role of land-atmosphere feedbacks in Earth system modeling. These findings underscore the need for integrated calibration strategies that simultaneously optimize multiple hydrological variables. However, if a single-variable approach is necessary, it is crucial to establish clear priorities for calibration, identifying the most critical variables that have the greatest impact on overall model performance.

Fang, Yilin [Pacific Northwest National Laboratory↗

DOE OSTI2019

Thermoplastic moulding of regenerated silk

Early insights into the unique structure and properties of native silk suggested that β-sheet nanocrystallites in silk would degrade prior to melting when subjected to thermal processing. Since then, canonical approaches for fabricating silk-based materials typically involve solution-derived processing methods, which have inherent limitations with respect to silk protein solubility and stability in solution, and time and cost efficiency. In this study, we report a thermal processing method for the direct solid-state moulding of regenerated silk into bulk ‘parts’ or devices with tunable mechanical properties. At elevated temperature and pressure, regenerated amorphous silk nanomaterials with ultralow β-sheet content undergo thermal fusion via molecular rearrangement and self-assembly assisted by bound water to form a robust bulk material that retains biocompatibility, degradability and machinability. This technique reverses presumptions about the limitations of direct thermal processing of silk into a wide range of new material formats and composite materials with tailored properties and functionalities.

36 MATERIALS SCIENCE↗

DOE OSTI2024

Light-inducible protein degradation in E. coli with the LOVdeg tag

Molecular tools for optogenetic control allow for spatial and temporal regulation of cell behavior. In particular, light-controlled protein degradation is a valuable mechanism of regulation because it can be highly modular, used in tandem with other control mechanisms, and maintain functionality throughout growth phases. Here, we engineered LOVdeg, a tag that can be appended to a protein of interest for inducible degradation in Escherichia coli using blue light. We demonstrate the modularity of LOVdeg by using it to tag a range of proteins, including the LacI repressor, CRISPRa activator, and the AcrB efflux pump. Additionally, we demonstrate the utility of pairing the LOVdeg tag with existing optogenetic tools to enhance performance by developing a combined EL222 and LOVdeg system. Finally, we use the LOVdeg tag in a metabolic engineering application to demonstrate post-translational control of metabolism. Together, our results highlight the modularity and functionality of the LOVdeg tag system and introduce a powerful new tool for bacterial optogenetics.

59 BASIC BIOLOGICAL SCIENCES↗

DOE OSTI2024

Light-inducible protein degradation in E. coli with the LOVdeg tag

Tague, Nathan (ORCID:0000000281146700)↗

DOE OSTI2021

Outlier classification using autoencoders: application for fluctuation driven flows in fusion plasmas

Understanding the statistics of fluctuation driven flows in the boundary layer of magnetically confined plasmas is desired to accurately model the lifetime of the vacuum vessel components. Mirror Langmuir probes (MLPs) are a novel diagnostic that uniquely allow us to sample the plasma parameters on a time scale shorter than the characteristic time scale of their fluctuations. Sudden large-amplitude fluctuations in the plasma degrade the precision and accuracy of the plasma parameters reported by MLPs for cases in which the probe bias range is of insufficient amplitude. While some data samples can readily be classified as valid and invalid, we find that such a classification may be ambiguous for up to 40% of data sampled for the plasma parameters and bias voltages considered in this study. In this contribution, we employ an autoencoder (AE) to learn a low-dimensional representation of valid data samples. By definition, the coordinates in this space are the features that mostly characterize valid data. Ambiguous data samples are classified in this space using standard classifiers for vectorial data. In this way, we avoid defining complicated threshold rules to identify outliers, which require strong assumptions and introduce biases in the analysis. By removing the outliers that are identified in the latent low-dimensional space of the AE, we find that the average conductive and convective radial heat fluxes are between approximately 5% and 15% lower as when removing outliers identified by threshold values. For contributions to the radial heat flux due to triple correlations, the difference is up to 40%.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2022

The Bacteroidetes Aequorivita sp. and Kaistella jeonii Produce Promiscuous Esterases With PET-Hydrolyzing Activity

Certain members of the Actinobacteria and Proteobacteria are known to degrade polyethylene terephthalate (PET). Here, we describe the first functional PET-active enzymes from the Bacteroidetes phylum. Using a PETase-specific Hidden-Markov-Model- (HMM-) based search algorithm, we identified several PETase candidates from Flavobacteriaceae and Porphyromonadaceae. Among them, two promiscuous and cold-active esterases derived from Aequorivita sp. (PET27) and Kaistella jeonii (PET30) showed depolymerizing activity on polycaprolactone (PCL), amorphous PET foil and on the polyester polyurethane Impranil ® DLN. PET27 is a 37.8 kDa enzyme that released an average of 174.4 nmol terephthalic acid (TPA) after 120 h at 30°C from a 7 mg PET foil platelet in a 200 μl reaction volume, 38-times more than PET30 (37.4 kDa) released under the same conditions. The crystal structure of PET30 without its C-terminal Por-domain (PET30ΔPorC) was solved at 2.1 Å and displays high structural similarity to the Is PETase. PET30 shows a Phe-Met-Tyr substrate binding motif, which seems to be a unique feature, as Is PETase, LCC and PET2 all contain Tyr-Met-Trp binding residues, while PET27 possesses a Phe-Met-Trp motif that is identical to Cut190. Microscopic analyses showed that K. jeonii cells are indeed able to bind on and colonize PET surfaces after a few days of incubation. Homologs of PET27 and PET30 were detected in metagenomes, predominantly aquatic habitats, encompassing a wide range of different global climate zones and suggesting a hitherto unknown influence of this bacterial phylum on man-made polymer degradation.

59 BASIC BIOLOGICAL SCIENCES↗

DOE OSTI2024

Piezocatalytic ZnS:Mn 2+ Nanocrystals for Enhanced Organic Dye Degradation

Piezocatalysis, an emerging approach that harnesses mechanical energy to drive chemical reactions, has garnered significant attention due to its potential applications in diverse fields, particularly in environmental remediation. Its broader application, however, is often hindered by the low efficiency of existing piezocatalytic materials. Here, we report the synthesis of Mn 2+ -doped ZnS nanocrystals with improved piezoelectric properties using an emulsion-based colloidal assembly technique. Through well-controlled Mn 2+ doping, these nanocrystals demonstrate high piezocatalytic activity for degrading organic dyes under ultrasonic vibration. The optimal performance is achieved with 3% Mn 2+ doping, outperforming many existing piezocatalysts. Mechanistic studies reveal the generation of reactive oxygen species as the primary driving force for degradation. Notably, pre-excitation with UV light further boosts the piezocatalytic efficiency of these metal ion-doped ZnS nanocrystals by filling electron trap states, leading to improved overall performance. This research paves the way for developing high-performance piezocatalysts, expanding the potential of piezocatalysis for a wide range of applications.

36 MATERIALS SCIENCE↗

DOE OSTI2023

Characterization of Cycle-Aged Commercial NMC and NCA Lithium-ion Cells: I. Temperature-Dependent Degradation

Lithium-ion batteries are widely used in applications from consumer electronic devices to stationary energy storage. Appropriate management of batteries is challenging due to limited data on their performance and materials degradation. Previous studies have focused on characterization of single cells under specific operating conditions. In the present work, commercial 18650 lithium-ion cells with LiNi x Mn y Co 1-x-y O 2 (NMC) and LiNi x Co y Al 1-x-y O 2 (NCA) positive electrodes were characterized by a wide range of electrochemical and materials techniques after cycling at 15, 25, or 35 °C to ∼80% capacity. The NCA cells exhibit weak temperature dependence in their cycle aging and materials degradation. The NMC cells exhibited increased capacity fade and materials degradation as ambient temperature decreased. All cells exhibited loss of lithium inventory as their primary degradation mode. However, the NCA cells only showed evidence of solid electrolyte interphase (SEI) growth whereas the NMC cells showed signs of Li plating at 15 °C, transitioning to SEI growth at 35 °C. The NMC cells displayed signs of loss of active material at the positive electrode at lower temperatures, suggesting that Li plating is correlated to additional processes that increase the rate of degradation. These results highlight the importance of avoiding broad generalizations about Li-ion battery temperature dependence.

25 ENERGY STORAGE↗

DOE OSTI2025

Synthetic active liquid crystals powered by acoustic waves.

Active nematic materials combine orientational order with activity at the microscopic level. Current experimental realizations of active nematics include vibrating elongated particles, cell layers, suspensions of elongated bacteria, and a mixture of bio-filaments with molecular motors. The majority of active nematics are of biological origin. The realization of a fully synthetic active liquid crystal comprised of a lyotropic chromonic liquid crystal energized by ultrasonic waves, is reported. This synthetic active liquid crystal is free from biological degradation and variability, exhibits phenomenology associated with active nematics, and enables precise and rapid activity control over a significantly extended range. It is demonstrated that the energy of the acoustic field is converted into microscopic extensile stresses disrupting long-range nematic order and giving rise to an undulation instability and proliferation of topological defects. The emergence of unconventional free-standing persistent vortices in the nematic director field at high activity levels is revealed. The results provide a foundation for the design of externally energized active liquid crystals with stable material properties and tunable topological defect dynamics crucial for the realization of reconfigurable microfluidic systems.

active matter↗

DOE OSTI2025

A critical review of electrochemical heat pump technologies: Status, challenges, and perspectives

The development of advanced heat pump technologies is critical for reducing global energy consumption in the building sector, where space heating and cooling account for nearly 50% of energy use. Electrochemical heat pumps (EHPs) offer a promising alternative to vapor compression systems by enabling direct electrochemical-to-thermal energy conversion, often with environmentally benign working fluids that exhibit low or zero global warming potential (GWP). Prior literature has predominantly focused on chemically reactive heat pumps, while comprehensive assessments of electrochemical mechanisms remain limited. Here, this review addresses this gap by systematically evaluating the underlying principles, architectures, and performance metrics of EHP systems. Compared to conventional vapor compression systems, EHPs can achieve 10%-30% higher energy efficiency, with reported cooling coefficients of performance (COP c ) ranging from 3.5 to 14.3 under standard operating conditions. Despite these advantages, widespread adoption is hindered by challenges including membrane degradation, electrode fouling, sluggish redox kinetics, and elevated system-level capital costs. To address these limitations, the review outlines three research priorities: (i) the development of advanced membranes, catalysts, and electrode materials with enhanced chemical and mechanical stability; (ii) the application of molecular-level simulations for the rational design of high-performance redox-active working fluids; and (iii) the integration of advanced diagnostic techniques for real-time monitoring and sustained operation of EHPs. By consolidating recent advances and explicitly identifying technological and scientific gaps, this work uniquely contributes a comprehensive framework for guiding future electrochemical heat pump research and facilitating the transition to sustainable thermal management technologies.

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗

DOE OSTI2023

Estimate long-term impact on battery degradation by considering electric vehicle real-world end-use factors

Many estimates of battery capacity degradation are based on accelerated lab tests that involve charge-discharge cycles or rely on data or electrochemical modeling. These methods are reasonable for technology benchmarking but rarely consider real-world end-use factors. To address this issue, this study develops the Battery Run-down under Electric Vehicle Operation (BREVO) model. It links the driver's travel pattern to physics-based battery degradation and powertrain energy consumption models. The model simulates the impacts of charging behavior, charging rate, driving patterns, and multiple energy management modules on battery capacity degradation. It finds that, over a 10-year timespan, firstly, for a random driver situated in the New England area, daily direct-current fast charging (60 kW) could lead to up to 22% less battery capacity when compared to daily Level-1 charging (1.8 kW). Second, the battery thermal management system can delay battery degradation by approximately 0.5% in the New England area. Third, warmer ambient temperatures enhance BEV battery usage. The model indicates that the battery capacity in the Los Angeles area is 6% higher than that in the New England area. The BREVO model provides crucial information for consumers and BEV manufacturers on range anxiety, BEV battery design, and decision support of battery warranty.

25 ENERGY STORAGE↗

DOE OSTI2025

A genome-scale metabolic model for the denitrifying bacterium Thauera sp. MZ1T accurately predicts degradation of pollutants and production of polymers

The denitrifying bacterium Thauera sp . MZ1T, a common member of microbial communities in wastewater treatment facilities, can produce different compounds from a range of carbon (C) and nitrogen (N) sources under aerobic and anaerobic conditions. In these different conditions, Thauera modifies its metabolism to produce different compounds that influence the microbial community. In particular, Thauera sp . MZ1T produces different exopolysaccharides with floc-forming properties, impacting the physical disposition of wastewater consortia and the efficiency of nutrient assimilation by the microbial community. Under N-limiting conditions, Thauera sp . MZ1T decreases its growth rate and accelerates the accumulation of polyhydroxyalkanoate-related (PHA) compounds including polyhydroxybutyrate (PHB), which plays a fundamental role as C and energy storage in this β-proteobacterium. However, the metabolic mechanisms employed by Thauera sp . MZ1T to assimilate and catabolize many of the different C and N sources under aerobic and anaerobic conditions remain unknown. Systems biology approaches such as genome-scale metabolic modeling have been successfully used to unveil complex metabolic mechanisms for various microorganisms. Here, we developed a comprehensive metabolic model (M-model) for Thauera sp . MZ1T ( i Thauera861), consisting of 1,744 metabolites, 2,384 reactions, and 861 genes. We validated the model experimentally using over 70 different C and N sources under both aerobic and anaerobic conditions. i Thauera861 achieved a prediction accuracy of 95% for growth on various C and N sources and close to 85% for assimilation of aromatic compounds under denitrifying conditions. The M-model was subsequently deployed to determine the effects of substrates, oxygen presence, and the C:N ratio on the production of PHB and exopolysaccharides (EPS), showing the highest polymer yields are achieved with nucleotides and amino acids under aerobic conditions. This comprehensive M-model will help reveal the metabolic processes by which this ubiquitous species influences communities in wastewater treatment systems and natural environments.

Tec-Campos, Diego (ORCID:0000000188194150)↗

DOE OSTI2021

Experimental Investigation on the Performance Loss of Cross-Linked Polymers During Photo-Oxidative Aging

Abstract Polymeric substances have seen an unprecedented integration in countless applications and fields of life, subjecting them to a broad range of environmental conditions, which can cause a form of damage to the structural and mechanical properties of these components known as aging. In this study we investigate the effects of the degradation of polymeric materials due to the extended exposure to sunlight, which can be simulated through controlled photo-oxidative aging using ultraviolet (UV) radiation as the main catalyst of this phenomenon. The effects on mechanical behavior and chemical properties of four polymeric materials with different mechanical characteristics was accordingly monitored throughout the study. The materials range in hardness with the polyurethane adhesive being the hardest and acting plastically, followed by an acrylic which exhibits greater hardening with time, a polyurethane sealant, which behaves in an elastomeric manner, and a silicon sealant, which is the softest of the set. Samples were prepared and subjected to UV radiation at three different temperatures namely 45, 60 and 80°C, for different aging periods ranging from 1 day for higher temperatures to 150 days for lower ones. The samples were then subjected to the Fourier transform Infrared spectroscopy (FTIR) test to monitor the change in the chemical composition of the materials along the aging durations and conditions. The materials were then subjected to mechanical testing along two modes of mechanical loading, which are a simple tension until failure and a double-cyclic test with progressively increasing strain limits after every two successful cycles until the sample reaches failure. The samples are loaded at constant strain rates throughout both tests. These tests revealed the change of behavior of our materials along the aging periods and conditions. The changes in mechanical behavior vary across each individual material depending on the aging temperature and period, with the changes ranging from hardening to softening, embrittlement or an increase in the maximum strain the material can endure before failure. A general trend would be that most materials become harder after photo-oxidation, however due to the range of temperatures in the aging conditions, thermo-oxidation, which causes softening in some of the polymers, has an increasingly notable effect at higher temperatures. A visible correlation can be noted between the change in mechanical behavior and a change in absorbance of Infrared Radiation (IR) in the FTIR spectrum, as the greater the crosslinking throughout the polymer matrix, the lower the absorbance of IR radiation due to the increased stiffness of the overall macro-molecular structure.

Korayem, Abd-Elrahman↗

DOE OSTI2024

Pool Boiling Reliability Tests and Degradation Mechanisms of Microporous Copper Inverse Opal (CuIOs) Structures: Preprint

The rising power density in electronic systems requires thermal management solutions that are both high-performing and reliable. Porous materials such as Copper Inverse Opals (CuIOs) have unique structural features, including high permeability and high thermal conductivity, to enhance pool boiling performance. However, there is little understanding of the degradation mechanism of such porous materials under pool boiling conditions. In this study, samples of 10-micrometer-thick CuIOs with 4.8-micrometer diameter, covering silicon substrate of area 11-mm by 11-mm, with various heated areas ranging from 2.5-mm by 2.5-mm to 10-mm by 10-mm, were tested in 100 degrees C deionized water at a constant heat flux of 110 watts per square cm for 3-7 days. The combined effect of erosion and corrosion caused structural degradation of the CuIOs. The directly heated area had the most severe degradation while the edge of the heater and the unheated area showed progressively less degradation, maintaining some CuIOs structure even after the 7-day reliability test. Among all the tested samples with various heater sizes, the 2.5-mm by 2.5-mm heater sample - in which the heater size was designed to be comparable to the water bubble characteristic length - had the largest critical heat flux (CHF) up to 300 watts per square cm with a superheat of approximately 13 degrees C. Additionally, CuIOs with a smaller heated area performed better in terms of reliability. This study offers preliminary insights into CuIOs degradation mechanisms, contributing to the development of more robust thermal management solutions. We expect that electroless plating of CuIOs with gold (Au), nickel (Ni), and atomic layer deposition of aluminum oxide in combination with appropriate application-specific coolants will further improve the reliability and lifetime of the CuIOs.

boiling-induced degradation↗