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At least 505 records · Page 28
All sourcesNASA NTRSDOE OSTI
DOE OSTI2025

Polysulfamates as “Macroisosteres” of Polyurethanes with Improved Degradability

Abstract Addressing the environmental persistence of plastics requires the development of next‐generation polymers that combine high performance with enhanced degradability. Progress toward this grand challenge has been impeded, in part, by the absence of a general blueprint for the macromolecular design of such materials. Herein, we introduce a “macroisostere” design strategy, where the carbonyl group (–CO–) in polyurethanes (PUs) is replaced with a sulfonyl group (–SO 2 –), resulting in a virtually unknown family of polymers called polysulfamates. This approach, inspired by the use of bioisosteres in drug discovery, aims to preserve key interchain interactions that contribute to thermomechanical performance while enhancing the hydrolytic lability of the polymer backbone. The optimization of a Sulfur(VI) Fluoride Exchange (SuFEx) polymerization allowed the synthesis of ten polysulfamates structurally analogous to common PUs. Comparative analysis of one PU and its polysulfamate analog showed that this isosteric substitution increases thermal stability, slightly lowers the glass transition temperature, and retains similar hardness and reduced Young's modulus. Notably, the S(VI)‐based polysulfamate demonstrated significantly enhanced hydrolytic degradability. These results highlight the potential of the “macroisostere” approach as a generalizable strategy for designing high‐performance, degradable alternatives to traditional plastics.

Chemistry↗
DOE OSTI2022

Gamma Radiation-Induced Degradation of Acetohydroxamic Acid (AHA) in Aqueous Nitrate and Nitric Acid Solutions Evaluated by Multiscale Modelling

Acetohydroxamic acid (AHA) has been proposed for inclusion in advanced, single-cycle, used nuclear fuel reprocessing solvent systems for the reduction and complexation of plutonium and neptunium ions. For this application, a detailed description of the degradation of AHA in dilute aqueous nitric acid is required. To this end, we present a comprehensive, multiscale computer model for the coupled radiolytic and hydrolytic degradation of AHA in aqueous sodium nitrate and nitric acid solutions. Rate coefficients for the reactions of AHA and HA with the oxidizing nitrate radical were measured for the first time using pulsed electron radiolysis and used as inputs in the kinetic model. The computer model results are validated by comparison to experimental data from steady state gamma irradiations, for which the agreement is excellent. Here, the presented model accurately predicts the yields of the major degradation products of AHA: acetic acid, hydroxylamine, nitrous oxide, and molecular hydrogen.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2023

Analysis of degradation products in thermally treated TATB

Delineating the chemical composition of TATB (1,3,5-triamino-2,4,6-trinitrobenzene) residues produced from the exposure to abnormal thermal environments should lead to a better understanding of the decomposition paths. Identifying and quantifying each compound in thermally produced residues, monitors which compounds are degrading or forming along the decomposition route, as well as providing input for the kinetic models of those pathways. Here, in this paper, we report the methodology of isolating, identifying, and where possible, quantifying soluble compounds present in solid residues of thermally treated TATB (330 °C for tens of minutes). Samples were extracted with DMSO, separated using chromatography, and quantified using their absorption at 354 nm. Identification of unknown compounds was accomplished using high resolution mass spectrometry. TATB, F1 (diamino-dinitro-benzofurazan), HO-TATB (2,4,6-triamino-1-hydroxyl-3,5-dinitrobenzene), and T4A (1-chloro-3,5-dinitro-2,4,6-triaminobenzene) were trace compounds detected in the unreacted TATB. Ten more compounds that formed in the residues were structurally identified including F2 (amino-nitro-difurazan). Several more compounds were observed but not completely identified. We propose possible structures for the unknowns. Of the compounds formed, F1 was the most abundant compound reaching 4.5 % by weight of the degraded solid sample. Other degradation compounds were estimated to sum to trace levels, well below 1 %. Most compounds were new, having not been detected and identified in previous studies of production grade and thermally aged TATB. Many compounds only reached detectable concentrations after several min of thermal exposure.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Strong degradation of polycarbonate and polystyrene by the CO 2 capture solvent diethyl sebacate

Here, we report on observations of strong degradation of a polycarbonate vessel by a solvent being considered for a CO 2 capture process, diethyl sebacate. This degradation led to failure of a polymeric hollow fiber membrane unit. Additional tests showed rapid degradation of polycarbonate safety glasses and polystyrene-based petri dishes by exposure to diethyl sebacate at ambient conditions. We also report on safe operations with diethyl sebacate in extensive experiments studying the corrosion of steel in CO 2 -pressurized reactors lined with PTFE and using PTFE gaskets. Used diethyl sebacate was also stored for long time periods in bottles made from low-density polyethylene bottles without physical deterioration. These observations indicate that care must be taken in development of new contactors and processes for CO 2 capture with diethyl sebacate and related solvents and in the choice of material for storage.

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

Iron-activated persulfate oxidation degrades aqueous Perfluorooctanoic acid (PFOA) at ambient temperature

Perfluorooctanoic acid (PFOA, C 8 HF 15 O 2 ) is an industrial surfactant that is highly resistant to natural breakdown processes such as those mediated by heat, hydrolysis, photolysis, and biodegradation. Many efforts have been developed to breakdown PFOA to less harmful species due to its widespread human exposure and potential toxicity. However, these methods require high temperature or specialized equipment with serious disadvantages of high energy cost for long-term use. For this paper, we investigated the effectiveness of PFOA degradation by ferrous iron-activated persulfate oxidation (IAPO) under various aqueous geochemical conditions. Approximately 64% of PFOA (initial concentration = 1.64 μmol L –1 ) was degraded after 4 h under illuminated anoxic conditions at ambient temperature. This degradation rate and magnitude support the potential use of IAPO as a novel inexpensive and environmentally friendly method to remediate PFOA in soil and groundwater.

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

A review of emerging photoinduced degradation methods for per- and polyfluoroalkyl substances in water

The remediation of per- and polyfluoroalkyl substances (PFAS) in water continues to garner significant attention due to their environmental persistence and adverse health effects. Among the various PFAS remediation methods, photoinduced approaches have recently emerged as promising techniques for the degradation of these persistent contaminants. However, many questions remain unanswered regarding the detailed mechanisms in these photoinduced methods as well as the best ways to leverage these approaches for PFAS degradation. In this review, we provide an update on recent experimental and theoretical developments in photoinduced PFAS degradation techniques over the past 2–5 years. We conclude with a perspective of promising research directions in this vibrant area and give recommendations on future experimental and computational approaches needed to further advance these photoinduced remediation capabilities.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Engineering of holocellulase in biomass-degrading fungi for sustainable biofuel production

Biofuels, such as bioethanol, are a clean and sustainable form of energy and have emerged as a viable alternative to fossil fuels. Plant biomass is an important raw material for the production of clean and renewable energy. The holocellulose contained in the composition of plants may be broken down into simple sugars, such as glucose, which are fermented by yeast to produce bioethanol. The conversion of glucose polymers into fermentable sugars is accomplished by enzymes known as holocellulases, which are produced by lignocellulolytic fungi. These enzymes act synergistically for the efficient degradation of cellulose polymers, and the fine and coordinated regulation of this process is performed by transcription factors (TFs). TFs are regulatory proteins that bind to the promoter region of their target genes (CAZymes, sugar transporters, signaling proteins, other TFs, etc.) to induce or repress their transcription. This review aims to understand the main regulatory mechanisms involved in plant biomass degradation by the most studied lignocellulolytic fungi Trichoderma sp., Aspergillus sp., Penicillium sp., and Neurospora crassa. In this context, the most studied TFs related to holocellulose degradation and genetic modification of TFs or promoters as a valuable tool to improve enzyme production for biotechnological purposes have been discussed. Furthermore, this review enables the expansion of knowledge on the regulation of the cellulolytic system of filamentous fungi and the application of this knowledge to the improvement of numerous bioproducts. Engineering TFs and promoters may yield more efficient strains that may be active in plant biomass hydrolysis. In this way, the technological processes for obtaining ethanol from lignocellulose may become more commercially viable.

09 BIOMASS FUELS↗
DOE OSTI2020

Degradation of impact toughness in cast stainless steels during long-term thermal aging

Cast austenitic stainless steels (CASSs) have been extensively used for the large components of nuclear reactor primary coolant systems. Since the cast steels inevitably contain degradable metastable phases and replacement of the large coolant system components is impractical, the thermal embrittlement of CASS components has been a serious concern in the extended-term operation of nuclear power plants. This study aimed to systematically measure and analyze the effect of long-term thermal aging on the Charpy impact toughness to provide a comprehensive understanding of thermal degradation behavior and a practical aging model to predict the degree of thermal degradation in the cast stainless steels. Additionally, the materials tested in the research include eight CASS alloys (two CF3s, one CF3M, three CF8s, and two CF8Ms) and two reference wrought materials (304L and 316L), in which the nominal δ-ferrite content ranges from ~2% to 33%. These stainless steels have been thermally aged at two light water reactor (LWR) temperatures (290 and 330 °C) and at two accelerated-aging temperatures (360 and 400 °C) for up to 30,000 h; these include both under-aged and over-aged conditions relative to the extended service lifetime (80 years). Charpy impact testing was performed for aged and non-aged specimens, and the impact (absorbed) energy parameters were correlated with a new aging parameter (A). Both the reduction of impact fracture toughness and the shift of ductile-brittle transition temperature were strongly dependent on the δ-ferrite content and degree of thermal aging. A linear relationship was found between the increasing rate of the index transition temperature T 41J and aging parameter A; base on which an empirical model was proposed for prediction of the transition temperature as a simple function of the aging parameter (A) and δ-ferrite content (F). Finally, the critical aging parameter for embrittlement (AC) was evaluated and compared with the existing δ-ferrite content criteria.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Coupling of multiscale imaging analysis and computational modeling for understanding thick cathode degradation mechanisms

Here, using a thick NMC811 (LiNi 0.8 Mn 0.1 Co 0.1 O 2 ) electrode as an example, we present a macro- to nanoscale 2D and 3D imaging analysis approach coupled with 4D (space + time) computational modeling to probe its degradation mechanism in a lithium-ion battery cell. Particle cracking increases and contact loss between particles and carbon-binder domain are observed to correlate with the cell degradation. This study unravels that the reaction heterogeneity within the thick cathode caused by the unbalanced electron conduction is the main cause of the battery degradation over cycling. The increased heterogeneity in the system will entail more cathode regions where the degree of active material utilization is uneven, leading to higher probabilities of particle cracking. These findings shed light on the crucial role of the electronic and ionic transportation networks in the performance deterioration of the thick cathode. They also provide guidance for cathode architecture optimization and performance improvement.

25 ENERGY STORAGE↗
DOE OSTI2024

From phase decomposition to evaporation: A multi-modal evaluation of thermally degraded model lightweight high-entropy alloy

Lightweight high-entropy alloys (LHEAs) have the potential to replace conventional lightweight materials due to their superior mechanical properties and thermal stability. However, the thermal degradation pattern of LHEAs from phase decomposition to evaporation is not clear. We develop a new Al-based dual phase (FCC + HCP) LHEA—AlTi 0.45 CuZn, and further investigate its thermal degradation behavior for potential high-temperature structural applications. Using multimodal advanced characterization techniques such as differential scanning calorimetry/thermogravimetric analysis, scanning/transmission electron microscopy, and synchrotron X-ray diffraction/pair distribution function (XRD/PDF), a sequence of thermal degradation events beyond the thermal phase stability limit—between 250 and 360 °C—is observed. These include phase decomposition at ~360 °C, Zn evaporation at ~750 °C, and LHEA melting at 880 °C which results in ~25% cumulative weight loss. The formation of Al-Ti phase off the AlTi 0.45 CuZn matrix is due to the largest negative mixing enthalpy for Al-Ti than other binary pairs. Similarly, Zn evaporation from AlTi 0.45 CuZn LHEA is due to its faster evaporation rate than other constituent elements. The high-resolution synchrotron XRD and PDF results support the aforementioned observations; in addition, they reveal local atomic arrangements, local strain, and sluggish grain growth in the LHEA. Among other LHEAs of close density range (5.55 ≤ ρ ≤ 5.85 g/cc), the investigated LHEA exhibits outstanding nano-indentation hardness values due to the coupled grain size effect and HCP phase strengthening of the FCC matrix. As the search for LHEAs for lightweight applications grows, this study shows the potential use of AlTi 0.45 CuZn LHEA for structural applications even at elevated temperatures.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2022

The Acyl-Proteome of Syntrophus aciditrophicus Reveals Metabolic Relationships in Benzoate Degradation

Syntrophus aciditrophicus is a syntrophic bacterium degrading fatty and aromatic acids into acetate, CO 2 , formate, and H 2 , consumed by methanogenic archaea. The syntroph’s acyllysine modifications were analyzed with a workflow avoiding antibody enrichment, enabling unbiased global acylation profiling. Seven acyl modification types were identified, six corresponding to reactive acyl-CoA species intermediates in benzoate degradation. Benzoatedegrading enzymes were also prominent among the 60 acylated proteins. The abundant acylations and active deacylases suggest that post-translational modifications directly regulate syntrophic benzoate degradation

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2024

Effect of supplementary cementitious materials on the degradation of cement-based barriers in radioactive waste repository: A case study in Korea

This study focuses on investigating the chemical degradation characteristics of cementitious barriers used in low- and intermediate-level radioactive waste repository by reactive transport modeling. The impact of the blending with supplementary cementitious materials (SCMs) in the barriers on the chemical degradation was evaluated to find the optimum barrier design. A number of different barrier designs were examined by replacing ordinary Portland cement (OPC) by SCMs (i.e., fly ash, silica fume, and blast-furnace slag). The simulation results showed that silica fume blended barrier has better durability against chemical degradation by rainwater compared to fly ash or blast-furnace slag blended barriers. In addition, the chemical durability of silica fume-based barrier increased with increasing replacement level up to about 20 %. It seems that the amount of formed calcium silicate hydrate (CSH) in the initial cement-based barrier highly affects the overall chemical durability. The newly developed reactive transport model demonstrated its capability for understanding the barrier performance and investigating the optimal design of the barrier system.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2025

A survey on degradation modeling, prognosis, and prognostics-driven maintenance in wind energy systems

Wind energy generation proliferated over the past decades, introducing unique challenges and opportunities for failure prediction, operation and maintenance. Decision-makers are continuously looking into new methods to infer failure mechanisms and behaviors of wind turbine components to detect and intervene in the failures before they happen. Evidently, degradation modeling and prognosis become engaging topics for researchers and practitioners to prevent catastrophic failures. Prognostics-driven approaches predict the time of failure for the components (e.g., predicting remaining useful life), which provides significant insights for scheduling of operations and maintenance activities. Integrating these prognostics-driven insights into wind farm operations and maintenance presents a substantial challenge, demanding careful consideration of numerous factors such as accessibility, crew routing, and spare part logistics. This study provides state-of-the-art review for degradation modeling, prognosis, and prognostics-driven maintenance techniques for wind energy systems. The discussed techniques align with the United Nations' sustainable development goals, in particular Goal 7 (Affordable and Clean Energy), by enhancing effectiveness and sustainability of wind energy operations. This work also showcases open research questions related to degradation modeling, prognosis, and prognostics-driven maintenance.

Altinpulluk, Nur Banu↗
DOE OSTI2026

Shrub and sedge rhizosphere communities display distinct affinities toward exudates and soil organic matter degradation: a quantitative stable isotope probing analysis

Warming temperatures are accelerating permafrost thaw and changing tundra vegetation, where woody shrubs are displacing sedges. Shrubs, such as Betula nana, and sedges, such as Eriophorum vaginatum, exhibit distinct life strategies including unique root-associated, or rhizosphere microbial communities. As permafrost thaws it unlocks previously unavailable carbon and nutrient sources resulting in deeper roots and a translocation of rhizosphere communities. Because permafrost microbial communities contain lower diversity and biomass than rhizosphere communities, the coalescence of rhizosphere and permafrost microbial communities could alter soil organic matter (SOM) degradation rates and increase greenhouse gas emissions. To identify metabolic strategies across distinct rhizosphere and permafrost microbial communities we conducted an isotope tracing incubation experiment. We inoculated thawed permafrost with shrub and sedge rhizosphere communities while adding exudates or water daily and compared this to an uninoculated control. After 46 days, we spiked samples with 18O enriched water or 13C enriched exudates and measured isotope incorporation into microbial DNA with quantitative stable isotope probing (qSIP). Our results indicate that exudate additions had little effect on uninoculated permafrost communities but the addition of exudates and rhizosphere inoculants had a compounding effect on respiration rates. We found that soils inoculated with shrub rhizosphere communities contained a mixture of exudate and SOM degraders while soils inoculated with sedge rhizosphere communities contained mainly SOM degraders. Finally, we found that individual microbial taxa exhibited maximum growth rates under specific combinations of microbial inoculant communities and exudate addition treatments. Our results reveal that microbial niches are strongly influenced by substrate preferences and community context, and suggest that a reduction in sedges and an expansion of shrubs may provide a mechanism by which permafrost carbon losses are mitigated through corresponding shifts in microbial communities and their substrate preferences.

Schaefer, Sean R [Natural Resources and Earth Syst↗
DOE OSTI2020

Impact of environmental variables on the degradation of photovoltaic components and perspectives for the reliability assessment methodology

Backsheet cracking has been a major issue observed in the field; however, standardized qualification tests, such as IEC61215, are inadequate to reliably identify such failures of PV modules due to the lack of the critical weathering factors applied sequentially or in combination, such as those found in the service environments. To address this problem, in this work we investigated the effects of various environmental variables on the degradation and failure behaviors of the polyamide-based backsheet in PV modules retrieved from five different locations, encompassing a variety of climates, including humid subtropical, hot-summer Mediterranean, tropical savanna climate and hot arid. The correlations between the degradation indicators and the weathering variables were further demonstrated by principle components analysis (PCA). We found strong relationships between: carbonyl formation and reflected solar radiation; hydroxyl formation and module temperature; yellowness and NO2 concentration, while no simple correlation could be found between a specific weathering factor and cracking. By introducing additional stress factors to the aged polyamide-based backsheet films with the novel 'fragmentation test', we successfully reproduced the field cracking behaviour. This study has demonstrated that different degradation modes of PV components respond differently to the environmental stresses encountered in service. Thereby, any accelerated laboratory test based on a single set condition or lacking key environmental variables would be inadequate to assess the long-term performance of PV modules and components. A new reliability-based methodology is proposed to quantitatively link laboratory testing with field results for the service life prediction of PV materials.

14 SOLAR ENERGY↗
DOE OSTI2022

Simultaneous neutron and X-ray tomography for visualization of graphite electrode degradation in fast-charged lithium-ion batteries

Advanced battery characterization using neutron and X-ray-based imaging modalities is crucial to reveal fundamental degradation modes of lithium-ion batteries (LIBs). Taking advantage of the sensitivity of neutrons to some low-Z (Li) and X-rays to high-Z materials (Cu), here we demonstrate the viability of simultaneous neutron and X-ray tomography (NeXT) as a non-destructive imaging platform for ex-situ 3D visualization of graphite electrode degradation following extreme fast charging (XFC). In addition, we underscore the benefits of the simultaneous of NeXT by combining the neutron and X-ray tomography data from the same sample location for material identification and segmentation of one pristine and two XFC-cycled graphite electrodes (9C charge for 450 cycles). Our ex-situ results and methodology development pave the way for the design of NeXT-friendly LIB geometries that will allow operando and/or in-situ 3D visualization of electrode degradation during XFC.

25 ENERGY STORAGE↗
DOE OSTI2022

Hydrobiological Mechanism Controlling the Synergistic Effects of Unsaturated Flow and Soil Organic Matter on the Degradation of Emerging Organic Contaminants in Soils

We report hydrology is a key factor influencing microbial degradation of emerging organic contaminants (EOCs) in soils, but the underlying mechanisms are not clear. In this study, biotic and abiotic column experiments were performed to investigate the removal and degradation of five EOCs in soils with different soil organic matter (SOM) contents under saturated and unsaturated flow conditions. In biotic experiments, 54–90% of bisphenol A (BPA) and 9–22% of ibuprofen (IBU) were removed from the aqueous phase of saturated columns due to adsorption and biodegradation. The biodegradation removed 26–65% of BPA and 1–22% of IBU. Decreasing soil pore water saturation from 100 to 80% increased BPA removal to 97–100% and IBU removal to 42–43% due to increased biodegradation (67–81% for BPA and 36–39% for IBU). No significant removal of BPA and IBU was observed in SOM-removed soils under saturated and unsaturated flow conditions. The desaturation did not influence sorptive losses of BPA (< 27%) and IBU (< 7%), suggesting their negligible adsorption at air–water interfaces but increased biodegradation of BPA and IBU sorbed at SOM–water interfaces. The study shows that soil drying and SOM can synergistically degrade BPA and IBU but have no effect on recalcitrant carbamazepine, tetracycline, and ciprofloxacin.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2023

Degradation in Ni-Rich LiNi 1– x – y Mn x Co y O 2 /Graphite Batteries: Impact of Charge Voltage and Ni Content

Ni-rich LiNi 1– x–y Mn x CoyO 2 (NMC) materials are attractive as cathodes for Li-ion batteries due to their high energy density and low Co content. However, these materials may display poor electrochemical reversibility relating to structural and interfacial instabilities. The influence of Ni content and level of delithiation during charge on degradation mechanisms and relevance to electrochemical cycling behavior are probed for LiNi 0.6 Mn 0.2 Co 0.2 O 2 (NMC622) and LiNi 0.8 Mn 0.1 Co 0.1 O 2 (NMC811) cathode materials in a full cell configuration under two upper voltage limits (4.1 and 4.3 V). The combined use of dQ/dV analysis of electrochemical voltage profiles, operando XRD, and postcycling scanning electron microscopy (SEM) measurements indicates that a major contributor to capacity fade is the large anisotropic volume change from an H2 $\leftrightarrows$ H3 phase transition and associated mechanical degradation particularly for NMC811. Notably, transition metal dissolution and deposition on the negative electrode are found to correlate with the structural changes occurring in the cathode under high voltage charge. X-ray photoelectron spectroscopy (XPS) analyses of the cycled cathodes reveal a more organic-rich cathode–electrolyte interphase (CEI) when cycling to 4.3 V with lower relative amounts of LiF. Surface reconstruction is not a significant factor under these cycling conditions as determined by soft X-ray absorption spectroscopy (sXAS) analysis. The results emphasize the opportunity to match the electrochemical test parameters with the specific NMC active material to mitigate degradation and extend cycle life.

36 MATERIALS SCIENCE↗