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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 19 records
All sourcesNASA NTRSDOE OSTI
DOE OSTI2020

A Physically-Based Model for Thermo-Oxidative and Hydrolytic Aging of Elastomers

A computationally efficient model is proposed to capture the loss of mechanical performance due to chemical aging that are formed as the competition of chain scission and cross-link formation/dissolution, such as thermo-oxidative aging or hydrolytic aging. The model should be considered an extension of our recent models [1, 2, 3] which further simplifies the matrix behavior based on the assumption of independence of environmental and mechanical damage. The model uses this assumption to reduce the necessary material parameters needed to model constitutive and inelastic behavior of elastomers during aging. To this end, the model can provide accurate predictions of the material performance with the significantly fewer number of fitting parameters. The model is relevant for all decay mechanisms formed by the occurrence of two simultaneous micro-mechanisms; (i) formation/reduction of the cross-links, and (ii) chain scission, both of which are present in thermo-oxidation and hydrolytic aging. Assuming the alteration of the chain density along the aging trajectory is identical to the peroxide cross-link density for thermo-oxidation, and the change of the average molecular weight for hydrolysis, the strain energy of polymer matrix can be rewritten as a function of deformation, deformation history, storage time and aging temperature. Next, the modified network alteration model is formulated for implementation into Finite Element (FE) simulations. The model is built on the presumption of homogeneous and consistent oxygen/water absorption and thus is mainly relevant for relatively thin samples exposed to environmental loads for a long time. The proposed model includes only six physically inspired material parameters. Therefore, while it is computationally efficient, it shows good agreement with own experimental data, which performed on various range of accelerated aging temperatures and times. With respect to its computational efficiency, simplicity, accuracy, and interpret-ability, the model is the right choice for advanced implementations in FE programs.

42 ENGINEERING↗
DOE OSTI2020

Hydrolytic Aging in Rubber-Like Materials: A Micro-Mechanical Approach to Modeling

Abstract The effect of hydrolytic aging on mechanical responses of Rubber likes materials, in particular, Mullins effect and the permanent set has been modeled. Hydrolytic aging is considered as the result of the competition between two phenomena (1) chain scission and (2) cross-link scission/reformation. Both phenomena were modeled and thus, the strain energy of the polymer matrix is written with respect to three independent mechanisms; i) the shrinking original matrix which has not been attacked by water, ii) conversion of the first network to a new network due to the reduction of the crosslinks, and iii) energy loss from network degradation due to water attacks to ester groups. The model is validated with respect to a set of experimental data. Besides accuracy, the simplicity and few numbers of fitting parameters make the model a good choice for further implementations.

Bahrololoumi, Amir↗
DOE OSTI2021

A Modified Network Alteration Model to Predict Quasi-Static Behavior of the Cross-Linked Polymers During Hydrolytic Aging

Abstract The network alteration theory is utilized to capture the effects of hydrolytic aging on the mechanical integrity of the polymer matrix. Hydrolytic degradation generally considered as a result of two simultaneous chemical phenomena; (i) reduction of the cross-links, and (ii) active chain loss. Assuming the alteration of the chain density is identical to the change of the number average molecular weight along the aging trajectory, the strain energy of polymer matrix can be rewritten as a function of deformation, deformation history, storage time, and aging temperature. The proposed model includes only five physically inspired material parameters. Thus, while it is computationally efficient, it shows good agreement with own experimental data, which performed on various range of accelerated aging temperatures and times. With respect to its computational efficiency, simplicity, accuracy, and interpret-ability, the model is a good choice for advanced implementations in FE programs.

Bahrololoumi, Amir↗
DOE OSTI2020

A multi-physics constitutive model to predict hydrolytic aging in quasi-static behaviour of thin cross-linked polymers

The effect of hydrolytic aging on mechanical quasi-static responses of rubber-like materials, in particular, the idealized Mullins effect and permanent set have been modeled. The effect of hydrolytic damage on the mechanical integrity of the polymer matrix is modeled as the direct competition of two micro-structural phenomena (i) chain scission and (ii) reduction of cross-links. Both phenomena and their correlation were modeled and thus, the strain energy of the polymer matrix is written with respect to three independent mechanisms; i) the shrinking original matrix that has not been attacked by water, ii) conversion of the first network to a new network due to the reduction of the cross-links, and iii) energy loss from network degradation due to water attacks to polymer active agents. The proposed model satisfies the Clausius-Duhem inequality and is thus physically feasible. The model is validated with respect to sets of our experimental data and other sets available in the literature. The proposed model is based on the assumption of homogeneous diffusion and mainly relevant for thin samples. In view of its accuracy, interpret-ability, and deep insight it provides into the nature of damage accumulation, the model is a good choice for further implementation in FE applications.

42 ENGINEERING↗
DOE OSTI2022

A Micro-Mechanical Constitutive Model to Predict Hygrothermal Aging of Cross-Linked Polymers

Abstract A multi-physics material model is presented to describe the effects of temperature, oxygen, and humidity on the constitutive response of cross-linked polymers. The effect of hygrothermal damage on the mechanical integrity of the polymer matrix can be considered as the result of damage accumulation of two independent aging mechanism namely, i) thermo-oxidative, and ii) hydrolytic aging. In order to capture the mutual effects of thermo-oxidative and hydrolytic aging, an assumption has been made that each of the aging phenomenon can be superposed to each other. In fact, each of them works independently and as a result, they can compete with each other. Utilizing the theory of network decomposition, all phenomena and their correlation were modeled and thus, the strain energy function of the polymer matrix is written with respect to four independent mechanisms, i) the shrinking original matrix that has neither been attacked by water nor oxygen, ii) conversion of the first network to two new network due to the reduction and formation of cross-links, and iii) energy loss from network degradation due to attack of the water molecules to polymer active agents. Moreover, the proposed model is micro-mechanically based and is mainly relevant on thin samples due to our underlying assumption of homogeneous diffusion of oxygen and water throughout the matrix. The model has been validated against extensive data-sets obtained from experiments we specifically designed for concept validation.

Bahrololoumi, Amir↗
DOE OSTI2022

A physics-informed multi-agents model to predict thermo-oxidative/hydrolytic aging of elastomers

This paper introduces a novel physics-informed multi-agents constitutive model to propose prediction in quasi-static constitutive behavior of cross-linked elastomer and the loss of mechanical performance during environmental aging. The presented model is used to simulate the effect of single-mechanism chemical aging (i.e. thermal-inducedor hydrolytic aging) on the behavior of the material in this hybrid framework. Those environmental single-mechanism damages change the polymer matrix over time due to massive chain scission, chain formations, and changing the arrangement of molecules in the polymer matrix. Here we propose a data-driven super-constrained machine-learned engine to represent damage in the polymer matrix and capture the changes in material behavior, including its inelastic features such as Mullins effect and permanent set in the course of aging. We have simplified the 3D stress–strain tensor mapping problem into a small number of super-constrained 1D mapping problems by means of a sequential order reduction. An assembly of multiple replicated conditional neural-network learning-agents (L-agents) is trained to systematically simplify the high-dimensional mapping problem into multiple 1D problems, each represented by a different type of agent. Our hybrid framework is designed to capture the effect of deformation history, aging time, and aging temperature. The model is validated with respect to a comprehensive set of experiments specifically designed to benchmark model capabilities and also against available data in the literature. Thermodynamic consistency and frame independency have been verified. Besides acceptable predictive abilities, a significant reduction of computational cost to predict behavior at multiple states of deformation is the most significant feature of this model.

42 ENGINEERING↗
DOE OSTI2023

A Physics-Based Data-Driven Approach for Modeling of Environmental Degradation in Elastomers

Abstract Elastomers are now commonly used in a number of industries, including aerospace, structure, transportation, shipbuilding, and automotive, due to their excellent workability, formability, and flexibility. During their activity, elastomers are subjected to harsh environmental conditions, which decreases their resilience. False predictions made early in their lives can have major financial and environmental implications. Elastomers’ performance and properties, such as strength, durability, and density, are influenced by chemical changes in these materials, known as degradation, which occurs over time. This process can alter the morphology of a polymer matrix as well as cause chain scission and cross-linking, resulting in different behaviors than that of the unaged material. To demonstrate the effect of thermaloxidative aging on the mechanical behavior of elastomers, several experimental and theoretical models have been proposed. In view of the large volume of experimental data available on micro-structural evolution in the course of aging, we propose a physics-based data-driven approach to overcome the shortcomings of both phenomenological and micro-mechanical models. This work presents a novel thermodynamically consistent, multiagent machine-learned model for predicting the constitutive behavior of cross-linked elastomers during environmental aging, such as thermo-oxidative and hydrolytic aging for various states of deformation. Single mechanism degradation changes the polymer matrix over time where it is causing chain scission, reduction of cross-links, and morphology change. To capture the idealized Mullins effect and permanent set due to the effect of single aging mechanisms on nonlinear mechanical responses of elastomers, we propose a data-driven model for simulating inelastic elements in a polymer matrix. By using a sequential order reduction, we were able to reduce the 3D stress-strain tensor mapping problem to a small number of super-constrained 1D mapping problems. To systematically classify such mapping problems into a few categories, an assembly of multiple replicated conditional neural network learning agents (L-agents) is used based on our recent work. Each category is represented by a different type of agent. The effect of deformation history, aging time, and aging temperature is captured by this model. The model is validated using a broad collection of data, ranging from our experimental results to data from the literature. In addition, thermodynamic consistency and frame independence are investigated. The most significant achievements of this model are its precision, simplicity, and prediction of inelasticity under various states of deformation. The model’s accuracy and simplicity make it a good option for commercial and industrial applications. Conveniently, due to the model modular nature, it can be expanded in the future to include viscoelasticity and non-isotropic formation for better precision.

Ghaderi, Aref↗
DOE OSTI2022

Experimental Characterization of Hygrothermal Aging: Competition Between Thermo-Oxidation and Hydrolysis Phenomena

Abstract In this work, we have presented a comparison between effects of accelerated thermo-oxidative, hydrolytic and hygrothermal aging on the mechanical and chemical properties of a polyurethane based (PUB) adhesive. The adhesive is a flexible adhesive which is extensively used in automobile industry as a glass sealant. During service life it gets exposed to the hygrothermal environment and the integrity of matrix interface is most vulnerable. This study focuses on weighing and comparing effects of different aging environments on material behavior; and it shows that hygrothermal aging environment results as a competition between two sub-aging phenomena i.e., thermo-oxidation and hydrolytic aging. Samples were exposed to 0%RH, 80%RH and submerged condition in distilled water. Uni-axial tensile tests, and cross-link density analysis by swelling test were carried out on as-received and aged samples. The aging process was conducted at three different temperatures (60°C, 80°C and 95°C) and for four different exposure durations of 1, 10, 30, and 90 days. This work confirms that the effect of hygrothermal aging is a result of competition between thermo-oxidation and hydrolytic aging environments. The total mechanical and environmental damage incurred by specimens is a collaborative effect of all exposure environments involved i.e., aging time, temperature, oxygen, water and humidity. The results are in agreement with the chemical test outcomes as well.

Shaafaey, Mamoon↗
DOE OSTI2023

Effect of Dual Environment Aging on Flexible Polyurethane Based Adhesive

Abstract Environmental degradation of adhesives naturally increases with the intensity of the ambient weathering agents involved. During service life, these materials are never subjected to a constant environmental loading. Real-time applications expose the material to multiple weather conditions, ranging from dry to humid or fully wet conditions. While some understanding exists about aging environments in isolation, we intend to investigate the effect of multiple environments on the constitutive behavior of the materials in question. The extent of damage can be accessed by analyzing the changes in constitutive behavior and toughness of aged material. Therefore, this aging experiment was designed around two-way aging regimes involving combinations of thermo-oxidation, hydrolytic and hygrothermal aging environments. We selected a polyurethane based flexible adhesive which is commonly used in the automotive industry as a glass sealant. The aged specimens were subjected to uniaxial tensile tests, and variation in material toughness and constitutive behavior was analyzed to ascertain the mechanics involved in the case of each environmental exposure. We outlined how different environments affect the material in isolation and how they interact with other weathering conditions. This study will help better understand and model the damage mechanics involved in exposure to multiple environmental conditions.

Shaafaey, Mamoon↗
DOE OSTI2024

Investigating the Crosslinking, Degradation, and Adhesion Behavior of Photovoltaic Encapsulants Under Thermal Accelerated Aging

Degradation of photovoltaic (PV) module encapsulant characteristics that lead to mechanical embrittlement and delamination remains a cause of failure in solar installations. A multiscale reliability model connecting the encapsulant mechanical and fracture properties to the degraded molecular structure and interfacial bonding to adjacent solar cell and glass substrates was previously published. The model, developed primarily for poly(ethylene-co-vinyl acetate) acetate (EVA) encapsulants, remains to be experimentally validated. Determining the degradation and crosslinking kinetics of alternative encapsulants, such as polyolefin elastomer (POE) and EVA/POE/EVA composites (EPE), can generalize the model. In this work, we subject fully cured EVA, POE, and EPE encapsulants to accelerated thermal aging to determine how high temperatures impact reaction kinetics. An increase in gel content (crosslinking) and decrease in crystallinity of the encapsulants under hot-aerobic (90 degrees C, 22% RH) and hot-anaerobic (90 degrees C, sealed in N 2 air) aging were observed, even in the absence of UV and crosslinking initiators. Fourier transform infrared spectroscopy (FTIR)-attenuated total reflectance analysis showed insignificant encapsulant degradation, demonstrating the critical role of UV and moisture in accelerating degradation. Adhesion testing performed on coupon-level specimens (cell/encapsulant/glass laminates) showed decreases in adhesion energy, Gc , from 5000 h of hot-dry (90 degrees C, ~1% RH) and hot-humid (90 degrees C, 60% RH) aging. POE coupons demonstrated the best stability, followed by EPE then EVA. For EVA and POE, hot-humid aged coupons experienced a larger decrease in Gc due to enhanced hydrolytic degradation. Hot-dry aging condition demonstrated that thermal degradation of the interface could be significant even if the encapsulant experiences negligible degradation in the absence of UV and elevated humidity.

accelerated aging↗
DOE OSTI2020

Build Orientation Dependent Microstructure in Polymer Laser Sintering: Relationship to Part Performance and Evolution with Aging

Laser sintering (LS) is widely used to produce functional polymeric parts; however, the resulting parts are often limited by their porous structure, and performance of the part may be strongly anisotropic. Relating the structural features of parts to build process conditions or powder feedstock has been explored previously. In contrast, little is known regarding how the unique internal structures of LS parts evolve and relate to their performance later in their life cycle, for example, after use in a real-world operating environment. In this study, a tightly controlled LS build process and measurement campaign by standard X-ray computed tomography (XCT), supported by high-resolution synchrotron XCT, was used to benchmark the internal microstructure (e.g. porosity) as a function of four different build orientations in printed polyamide-12 (PA-12) parts. The initial performance of the parts after printing was characterized by tensile testing and dynamic mechanical analysis (DMA). Arrays of PA-12 parts in different build orientations were exposed to steam (under pressure) and air across multiple temperature and time points for the purposes of accelerated aging through oxidative and hydrolytic breakdown. Exposing parts to steam dramatically altered the internal microstructure and functional properties such as the glass transition temperature, tensile properties, and damping behavior. Notably, post-aging XCT revealed large microstructural changes after only 40 h of steam treatment relative to the as-printed specimens. Furthermore, pore reorganization and changes in crystallinity occurred regardless of whether the steam temperature was aggressive enough to induce a significant loss in mechanical properties. The build orientation dependence on the aging rate was minimal with the relative trend in performance persisting across most metrics among the different orientations even after aging.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Role of n-phenyl-β-naphthylamine in the Acid-Nitroplasticizer Thermal Aging (ANTA) Experiment

A short-term aging study, which was named as Acid-Nitroplasticizer Thermal Aging (ANTA), was conducted to explore the complex chemistry between n-phenyl-β-naphthylamine (PBNA), HNO x , and nitroplasticizer (NP). Aging of NP with PBNA and acid treatments have demonstrated that PBNA is an effective antioxidant and an anti-hydrolytic agent (e.g., inhibits HNO 3 ) and have allowed the identification of nitroso-PBNA (PBNA-NO). The direct conversion of PBNA to PBNA-NO via scavenging of HONO, known as nitrosation, is a preceding event of PBNA nitration, which provides evidence to the HONO elimination as the key mechanism in the early stage of NP aging. Through the kinetics of both nitrosation and nitration, the accuracy of a prediction on PBNA consumption in NP degradation is further improved.

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

Water Sorption Study of Various Polymers and Polymeric Composites

In the formulations of many composite materials, polymeric materials are often used as binder materials to enhance processability, functionality, and safety during manufacturing. For instance, poly(ester urethane), such as Estane® 5703, is used in the formulation of PBX 9501, and vinyl copolymer elastomer (VCE) is used in the formulation of VCE/filler compos ites. The stability of these binders directly impacts the overall stability and performance of their composites. Estane and VCE are prone to hydrolytic degradation, with water sorption behavior playing a significant role in their long-term stability and aging behavior. Hence, it is critical to study their water sorption behavior under various humidity and tempera ture conditions. To improve the accuracy and reduce labor-intensive work involved in water sorption experiments, an automated Dynamic Vapor Sorption (DVS) system was employed, which can generate large datasets. To efficiently process and analyze these datasets, Python scripts were developed. These scripts not only streamlined data processing, but also accu rately derived the Arrhenius parameters related to water diffusion and sorption properties for the tested materials. This approach offers a robust framework for evaluating water trans port and sorption processes in polymeric materials and adds valuable capabilities to future water sorption testing efforts.

36 MATERIALS SCIENCE↗
DOE OSTI2026

Collaborative Approach to Identify Degradation Mechanisms and Validate Aging Protocols for a Diverse Set of DAC Materials (TCF Base Technology-Specific Final Report)

This work supports the mission of the U.S. Department of Energy to promote American energy leadership, technological innovation, and economic growth through the development of technologies for cost effective carbon capture. While capture technologies can provide carbon dioxide for enhanced oil recovery, many capture materials suffer from oxidative, hydrolytic and/or thermal degradation which leads to capacity loss and unwanted emissions such as ammonia. Short lifetimes increase operational costs and cost studies suffer from uncertainty because the true lifetimes of many capture materials are unknown. In this study, a suite of capture materials were studied to quantify their degradation, provide insight into the mechanisms that lead to their uptake loss and provide validated accelerated aging protocols for industry.

36 MATERIALS SCIENCE↗
DOE OSTI2022

The Natural and Accelerated Evolution of EVA Adhesion Through Intermediate Exposures

Ethylene vinyl acetate (EVA) encapsulants comprise the majority of the encapsulants currently in use; much work has been done to understand and model the adhesive characteristics of EVA-encapsulated modules, but limited work has provided reliable insight into adhesion during the intermediate stages of exposure, limiting the ability to validate model predictions in this range. We provide the adhesion energy measurements for EVA adhesion after nearly six years of field aging and 10 000 h of accelerated aging. Both field and accelerated aging reveal a distinct plateau that emerges during the intermediate exposure periods (after one year in the field and after 1000 h in a chamber). At 10 000 h, adhesion within accelerated aged minimodules falls to a level generally seen after long-term field exposures (>15 years). Previous modeling predicted that adhesion would steadily decrease over the lifetime of a module, but these current results uncover an intermediate plateauing trend that is important to accurately modeling the evolution of adhesion and predicting adhesive failure. Based on these findings, three key model refinements concerning the rate of UV-radical formation and subsequent β-scission, the rate and acceleration of hydrolytic depolymerization, and the profile of the plasticity contribution over time are implemented and discussed.

14 SOLAR ENERGY↗
DOE OSTI2020

Poly(lactic acid)-Based Ink for Biodegradable Printed Electronics With Conductivity Enhanced through Solvent Aging

Biodegradable electronics is a rapidly growing field, and the development of controllably biodegradable, high-conductivity materials suitable for additive manufacturing under ambient conditions remains a challenge. Here, printable conductive pastes that employ poly(lactic acid) (PLA) as a binder and tungsten as a conductor are demonstrated. These composite conductors can provide enhanced stability in applications where moisture may be present, such as environmental monitoring or agriculture. Post-processing the printed traces using a solvent-aging technique increases their conductivity by up to 2 orders of magnitude, with final conductivities approaching 5000 S/m. Such techniques could prove useful when thermal processes including heating or laser sintering are limited by the temperature constraints of typical biodegradable substrates. Finally, both accelerated oxidative and hydrolytic degradation of the printed composite conductors are examined, and a fully biodegradable capacitive soil moisture sensor is fabricated and tested.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Decomposition of Irganox 1010 in plastic bonded explosives

Abstract Degradation pathways of Irganox 1010 in aged plastic bonded explosive (PBX) 9501 were investigated using ultrahigh performance liquid chromatography coupled to quadrupole time of flight mass spectrometry (UHPLC‐QTOF). Using a targeted approach, a total of 44 Irganox 1010 decomposition products were discovered. These decomposition products were formed through hydrolysis, scission, and/or oxidation of Irganox 1010. The hydrolytic decomposition of Irganox is a straightforward process resulting in the cleavage of the ester group(s) while oxidation and scission are more complicated and can happen at multiple locations on the Irganox 1010 molecule. Moreover, due to the symmetric nature of Irganox 1010, multiple decomposition reactions can occur. Indeed some decomposition products exhibited hydrolysis, oxidation, and scission. In order to probe any trends in the aged PBX 9501 samples, principal component analysis (PCA) was implemented. The greatest chemical differences between the aged PBX samples was hydrolysis of the ester functional groups on Irganox 1010. Despite the negative connotations of hydrolysis, the Irganox 1010 decomposition products are still able to function as a radical scavenger in PBX 9501 as intended.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗