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At least 1,441 records · Page 80
All sourcesNASA NTRSDOE OSTI
DOE OSTI2024

Analytical Tools to Assess Polymer Biodegradation: A Critical Review and Recommendations

Many petroleum-derived plastic materials are highly recalcitrant and persistent in the environment, posing significant threats to human and ecological receptors due to their accumulation in ecosystems. In recent years, research efforts have focused on advancing biological methods for polymer degradation. Enzymatic depolymerization has emerged as particularly relevant for biobased plastic recycling, potentially scalable for industrial use. Biodegradation involves adsorption to the plastic solid surface, followed by an interfacial reaction, resulting in cleavage of bonds of polymer chains exposed on the surface. Here, widely varying substrate-specific kinetics are observed, with the polymer’s properties possessing a significant impact on the rate of this interfacial catalysis. Thus, there is a critical need for sensitive and accurate characterization of the material surface during and after interfacial depolymerization to fully understand the reaction mechanisms. Here, we provide a critical review of a range of techniques used in the analysis of material surfaces to characterize the chemical, topological, and morphological features relevant to the study of enzymatic biocatalysis, including microscopy techniques, spectroscopic techniques (e.g., X-ray diffraction analysis, Fourier transform infrared attenuated total reflectance spectroscopy, and mass spectrometry detection of analytes associated with degradation). Techniques for evaluation of surface energy and topology in their relevancy for sensitive detection of biological surface modifications are also discussed. In addition, this paper provides an overview of the strengths of these techniques and compares their performance in both sensitivity and throughput, including emerging techniques, which can be useful, particularly for the rapid analysis of the surface properties of polymeric materials in high-throughput screening of candidate biocatalysts. This research serves as a starting point in selecting and applying appropriate methodologies that provide direct evidence to the ongoing biotic degradation of polymeric materials.

Colachis, Matthew↗
DOE OSTI2024

Sustainability and affordability of building electrification: A state-by-state holistic approach for multifamily buildings

This paper explores the evolving narrative of building electrification, considering its potential to solve climate change. Previous research has predominantly focused on hybrid renewable energy portfolios and increasing home pricing premiums, overlooking the perspectives of renters burdened by housing costs. Moreover, existing studies have primarily examined the effects of electrification on single-family homes and case studies, neglecting multifamily buildings and their relationship with the grid. This comprehensive study leverages calibrated building energy models to address these gaps and evaluates sustainability through carbon dioxide emissions and affordability through economic performance. The findings demonstrate significant progress in electrification since 2017, with nearly all states showing decreased energy usage in the electrified models. Environmentally, twenty-two states perform better or comparably with the electrified models in the most recent study. Economically, challenges persist, but a sensitivity analysis demonstrates how results could improve soon. Furthermore, the study discusses the outlook of electrified multifamily buildings, considering ongoing decarbonization plans for the electric grid. In three case studies, electrification demonstrates improvements in over half of the states by 2026. Overall, the research highlights the importance of expanding analysis to include multifamily buildings and emphasizes the positive impact of electrification as a viable energy, environmental, and economic solution.

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗
DOE OSTI2025

Challenges in spatial metabolomics and proteomics for functional tissue unit and single-cell resolution

While transcriptomics is the most broadly applied technology for global spatial and single cell measurements in healthy and diseased tissues. Transcripts are often used as a proxy for protein and even metabolite measurements, but it has become commonly accepted that extrapolating this kind of information is a poor proxy and not a substitute for direct measurement. Within the last decade advanced developments of mass spectrometry-based assays have made these direct measurements not only possible, but routine. Where mass spectrometry has become an enabling technology, and various methods can now detect hundreds of metabolites and thousands of proteins from samples. Not only can this be performed within bulk measurements, but much effort has been directed into translating these measurements to single cells and tissues at cellular resolution. The information obtained from mass spectrometry is now able to trace metabolic events and decipher feedback loops across anatomical regions, connecting genetic and metabolic networks that define phenotypes. Herein, we will broadly overview developments in the field over the past decade, leading into several case studies which highlight the direct measurement of metabolites, proteins, and proteoforms from thinly sliced tissues. Much of this work is feasible due to multidisciplinary team science, and we offer brief perspective on paths forward and the challenges that persist with adoption and application of spatial omics.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2020

Hydroxypyridinone-based stabilization of Np(IV) enabling efficient U/Np/Pu separations in the Adapted PUREX process

The classical process to recover uranium (U) and plutonium (Pu) from used nuclear fuel using tributyl phosphate (TBP), namely the Plutonium Uranium Redox EXtraction (PUREX) process, is complicated by the persistent presence of neptunium (Np) and thus requires extra purification steps. The concept of Adapted PUREX seeks to achieve Np recovery by adjusting the valence of the metal more effectively, thereby controlling its behavior more precisely. This study introduces the use of an aqueous hydroxypyridinone chelator, 3,4,3-LI(1,2-HOPO) (abbreviated as HOPO), to dictate the behavior of Np for recovery and meanwhile simplify cumbersome reprocessing steps. The interactions between Np and HOPO were probed mechanistically by way of absorption spectrophotometry, in conjunction with cyclic voltammetry. UV–Vis-NIR spectra illustrated the reduction of NpO 2 2+ to Np 4+ , with a fast reaction rate. Cyclic voltammetry revealed quasi-reversible processes between the oxidized and reduced forms of the ligand and its Np complexes. The corresponding heterogeneous rate constants (k 0 ) were estimated from the peak-to-peak separation potentials (ΔE p ), at ~ 4 – 35 μm/s for both HOPO and NpHOPO, with scan rates of 0.01 – 0.4 V/s. Meanwhile, the electromotive force (E MF ) as well as the change of Gibbs free energy (ΔG) were assessed from the half-wave potential (E 1/2 ), demonstrating the completeness of NpO 2 2+ reduction to Np 4+ by HOPO. The cumulative formation constant of the resulting NpHOPO complex (logβ 101 ) was determined by metal competition titration to be 42.0 ± 0.6, corroborating the extraordinarily high affinity of HOPO to tetravalent metal ions. Here, the prowess of valence control by HOPO and the high stability of the formed complex resulted in enhanced separations of Np from U and of Pu from U, with a maximum separation factor of ~7000 for both, nearly 90- and 10300-fold higher, respectively, than the values obtained using conventional PUREX formulae.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2020

Microbial extracellular polysaccharide production and aggregate stability controlled by switchgrass ( Panicum virgatum ) root biomass and soil water potential

Deep-rooting perennial grasses are promising feedstocks for biofuel production, especially in marginal soils lacking organic material, nutrients, and/or that experience significant water stress. Perennial grass roots influence surrounding soil conditions and microbial activities, and produce extracellular polymeric substances (EPS) composed primarily of extracellular polysaccharides (EPSac). These polymers can alleviate microbial moisture and nutrient stress, and enhance soil characteristics through improved water retention and aggregate stability—which may in turn enhance carbon persistence. Here, we used a 13 CO 2 greenhouse tracer experiment to examine the effect of switchgrass cultivation on EPSac production and origin in a marginal soil with five fertilization/water treatments (control, +N, +NP, +P, low water), and compared these results with measurements of field soils collected after long-term switchgrass cultivation. Soils with added nitrogen and phosphorus (+NP) had the highest root biomass, EPSac and percentage of water-stable soil aggregates. Multiple linear regression analyses revealed that root biomass and soil water potential were important determinants of soil EPSac production, potentially by controlling carbon supply and diurnal changes in moisture stress. Path analysis showed that soil aggregation was positively correlated with bulk soil EPSac content and also regulated by soil water potential. High mannose content indicated the majority of EPSac was of microbial origin and 13 CO 2 labeling indicated that 0.18% of newly fixed plant carbon was incorporated into EPSac. Analysis of field soils suggests that EPSac is significantly enhanced after long-term switchgrass cultivation. Taken as a whole, our greenhouse and field results demonstrate that switchgrass cultivation can promote microbial production of EPSac, providing a mechanism to enhance aggregation in marginal soils.

13c labeling↗
DOE OSTI2021

Belowground allocation and dynamics of recently fixed plant carbon in a California annual grassland

Plant roots and the organisms that surround them are a primary source for stabilized soil organic carbon (SOC). While grassland soils have a large capacity to store organic carbon (C), few field-based studies have quantified the amount of plant-fixed C that moves into soil and persists belowground over multiple years. Yet this characteristic of the soil C cycle is critical to C storage, soil water holding capacity, nutrient provisions, and the management of soil health. Here, we tracked the fate of plant-fixed C following a five-day 13 CO 2 labeling of a Northern California annual grassland, measuring C pools starting at the end of the labeling period, at three days, four weeks, six months, one year, and two years. Soil organic carbon was fractionated using a density-based approach to separate the free-light fraction (FLF), occluded-light fraction (OLF), and heavy fraction (HF). Using isotope ratio mass spectrometry, we measured 13 C enrichment and total C content for plant shoots, roots, soil, soil dissolved organic carbon (DOC), and the FLF, OLF, and HF. The chemical nature of C in the HF was further analyzed by solid state 13 C nuclear magnetic resonance (NMR) spectroscopy.

13C-NMR↗
DOE OSTI2022

Susceptibility of new soil organic carbon to mineralization during dry-wet cycling in soils from contrasting ends of a precipitation gradient

The persistence of soil organic carbon (SOC) is influenced by soil physicochemical properties, organic matter quality, and climatic conditions that govern its vulnerability to microbial activity. We compared the susceptibility of newly formed SOC to mineralization in two soils (Andosols) that developed under contrasting precipitation regimes. Soil from the high rainfall region (‘high rain ’) had higher SOC and lower iron concentrations than soils exposed to less rainfall (‘low rain ’). We amended soils with 13 C-labeled carbohydrates and measured the amount of substrate-derived SO 13 C mineralized when exposed to dry-wet cycling following months-long incubations. We hypothesized that susceptibility would differ due to iron content and mineralogy, initial SOC, substrate solubility (cellulose versus glucose amendment), and microbial substrate use efficiency (SUE). We found that SO 13 C was less susceptible to dry-wet cycling when more 13 C was assimilated into microbial biomass and co-localized with mineral surfaces than when co-localized with existing organo-mineral surfaces, according to microscale NanoSIMS imaging. Considerably less SO 13 C was susceptible to mineralization in the ferrihydrite-rich (low SOC) low rain soil than the leached (high SOC) high rain soil when C was added as either glucose (7.3-fold less C mineralized) or cellulose (15.2-fold less). Additionally, the SUE of glucose was comparable to cellulose in low rain soil where SO 13 C was less water soluble and coprecipitated with ferrihydrite, and used half as efficiently as cellulose in high rain soil. Our results show that the susceptibility of newly formed SOC to mineralization is modified by the effects of bioavailability on microbial metabolism and the availability of mineral surfaces for forming new organo-mineral complexes.

21 NanoSIMS↗
DOE OSTI2022

Microbe-iron interactions control lignin decomposition in soil

Lignin decomposition is critically linked to terrestrial carbon (C) cycle due to the enormous C mass of lignin and its importance in controlling overall rates of litter decomposition. Interactions between lignin and iron (Fe) minerals have been increasingly recognized as key mediators of lignin decomposition in experimental studies. However, we still lack a quantitative understanding of how Fe minerals interact with microbes to control lignin decomposition. Here, we leveraged experimental results from an incubation of Fe-rich soil, in which lignin decomposition rates were measured at aerobic conditions after four levels of pre-treated O2 availability, to examine microbe-Fe (MiFe) interactions in lignin decomposition with a MiFe model. We quantified how Fe redox cycling interacted with microbial activities to control lignin decomposition via data-model integration. Our results showed that the MiFe model with time-dependent growth and mortality functions better represented CO2 release from lignin decomposition (R2 ranging from 0.96 to 0.97) than models assuming either first-order or Michaelis-Menten kinetics. Reduction of Fe(III) to Fe(II) after pre-treatments with lower O2 availability stimu-lated the Fenton reaction to break down macro-molecular lignin into small molecules available to microbes. The small molecules of lignin and necromass bounded with oxidized Fe and were protected from decomposition. After 1-year incubation, the model implied that most of C stabilized with Fe minerals was derived from small molecular lignin C. Our quantitative analysis of microbe-Fe interactions sheds new light on lignin decomposition and preservation and helps improve model prediction of soil C persistence under global change.

Liao, Cuijuan↗
DOE OSTI2024

Getting to the root of the problem: Soil carbon and microbial responses to root inputs within a buried paleosol along an eroding hillslope in southwestern Nebraska, USA

Large quantities of soil carbon (C) can persist within paleosols for millennia due to burial and subsequent isolation from plant-derived inputs, atmospheric conditions, and microbial activity at the modern surface. Erosion exposes buried soils to modern root-derived C influx via root exudation and root turnover, thus stimulating microbial activity leading to SOC decomposition and accumulation through organo-mineral stabilization of modern C. With this study we aim to quantify how modern root-derived C inputs impact paleosol C decomposition and stabilization across varying degrees of isolation from modern surface conditions in southwestern Nebraska, USA, where hillslope erosion is bringing a buried Late-Pleistocene-early Holocene paleosol (the “Brady Soil”) closer to the modern surface. We collected Brady Soil samples from 0.2m, 0.4m, and 1.2m below the modern surface and conducted two lab-based incubations. Soils were amended with either (1) a lab-synthesized mixture of low molecular weight compounds (12 atom% 13 C), or (2) 13 C enriched root residues (92 atom% 13 C), in 30-day and 240-day incubation experiments, respectively. Here we determined microbial responses to synthetic root exudates and residues by partitioning the 13 C label from Brady Soil C, including measurements of total, root, and primed C respiration, microbial biomass C (MBC), microbial C use efficiency (CUE). To assess the capacity of isolated paleosols to accrue modern plant C, we used Nano-scale Secondary Ion Mass Spectrometry imaging. We found that: (1) adding root-derived C inputs primed Brady Soil C across all depths, and was mediated by depth and composition of root additions; (2) root-derived C inputs stimulated microbial biomass C (MBC) growth similarly across depths, but the magnitude of CUE and MBC varied by chemistry of root-derived additions; (3) new particulate organic matter was incorporated into mineral-associated pools over time; (4) material from the added root residues was found in association with bacterial cells and fungal hyphae as well as with soil aggregate and mineral surfaces. Our study shows that paleosols defy expectations of C content and reactivity with depth, and changes in land cover and climate will expose buried paleosols to modern surface conditions, increasing respired C. This work highlights the importance of evaluating the role resurfacing buried soils through landscape change plays in C cycle feedbacks to the climate system.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2024

Moisture-mineral interactions drive bacterial and organic matter turnover in glacier-sourced riparian sediments undergoing pedogenesis

Glacial recession is occurring at unprecedented rates resulting in increased sediment accumula-tions in some riverine ecosystems. Increased sediment deposition has implications for ecosystem stability (e.g., floods and river paths) and environmental services (e.g., carbon sequestration). Soils and sediments have an enormous potential to retain carbon (C), predominantly due to sorp-tion to mineral surfaces. However, C persistence may be sensitive to climate-change induced temperature and moisture variations. We coupled ultrahigh resolution organic matter composition classification with bacterial characterization and respiration measurements to test the combined effects of temperature (4 vs 20°C) and moisture (50 vs 100% water-filled pore space) on C turn-over in sediments maintained under different mineralogical conditions (illite-amended vs non-amended). Here we show that the inhibition of CO 2 emissions from the combined effect of in-creased moisture content and illite was reflected in the turnover of key molecular signatures, such as the nominal oxidation state of C, often irrespective of temperature. However, shifts in bacteri-al communities from a coupled moisture-mineral interaction, were temperature-dependent. Our results highlight the importance of moisture in driving mineral-organic interactions and suggest that C in clay-rich, water-saturated sediments is both thermodynamically unfavorable and miner-al-protected from microbial consumption.

58 GEOSCIENCES↗
DOE OSTI2025

Phosphate amendment drives bloom of RNA viruses after soil wet-up

Soil rewetting after a dry period results in a surge of activity and succession in both microbial and DNA virus communities. Less is known about the response of RNA viruses to soil rewetting—while they are highly diverse and widely distributed in soil, they remain understudied. We hypothesized that RNA viruses would show temporal succession following rewetting and that phosphate amendment would influence their trajectory, as viral proliferation may cause phosphorus limitation. Using 39 time-resolved metatranscriptomes and amplicon data, 2190 RNA viral populations were identified across five phyla, with 26 % of these predicted to infect bacteria, and 11 % fungi. Only 1.2 % of viral populations had annotated capsid genes, suggesting most persist via intracellular replication without a free virion phase. Phosphate amendment altered RNA viral community composition within the first week and amended vs. unamended communities remained distinguishable for up to three weeks. While the overall host community remained stable, certain bacterial populations showed reduced abundance in phosphate-amended soils, likely due to increased viral lysis, as RNA bacteriophages proliferated significantly. Notably, 60 % of the viruses with increased abundance under phosphate amendment belonged to basal Lenarviricota clades rather than well-known groups like Leviviricetes. We estimate RNA bacteriophage infections may affect 10 7 –10 9 bacteria per gram of soil, aligning with the total bacterial population (10 7 –10 10 g -1 soil), suggesting that RNA phages significantly influence bacterial communities post-wet-up, with phosphorus availability modulating this effect.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2019

A copula-based Bayesian method for probabilistic solar power forecasting

With increased penetration of solar energy sources, solar power forecasting has become more crucial and challenging. This paper proposes a copula-based Bayesian approach to improve probabilistic solar power forecasting by capturing the joint distribution between solar power and ambient temperature. A prior forecast distribution is first obtained using different underlying point forecasting models. Parametric and empirical copulas of solar power and temperature are then developed to update the prior distribution to the posterior forecast distribution. A public solar power database is used to demonstrate effectiveness of the proposed method. Numerical results show that the copula-based Bayesian method outperforms the forecasting method that directly uses temperature as a feature. The Bayesian method is also compared with persistent models and show improved performance. Furthermore, this article includes supplementary material (data and code) for reproducibility.

24 POWER TRANSMISSION AND DISTRIBUTION↗
DOE OSTI2024

Use of physics to improve solar forecast: Part III, impacts of different cloud types

Cloud-type impacts present a great challenge to solar forecasting due to diverse and complex cloud-radiation interactions. This third part of our paper sequence seeks to address this challenge by quantifying the forecast accuracies under eight cloud types: cumulus (Cu), stratified clouds (St), altocumulus (Ac), altostratus (As), cirrostratus/anvil (Cr), cirrus (Ci), congestus (Co), deep convective clouds (Dc) across four physics-informed persistence models reported in Part I. To generalize the cloud impacts, the eight cloud types are further grouped into three cloud categories based on their common features: weak convective clouds, stratiform clouds, and strong convective clouds. Here, the decade-long (2001 ~ 2014) collocated measurements of irradiances and cloud types at the U.S. Department of Energy (DOE) Atmospheric Radiation Measurement (ARM) Program South Great Plain (SGP) Central Facility site are used for model evaluation. Results reveal a clear performance hierarchy for global horizontal irradiance (GHI) and direct normal irradiance (DNI): best for weak convective clouds and cirrus, intermediate for stratiform clouds, and worst for strong convective clouds. Performance for diffuse horizontal irradiance (DHI) is less influenced by cloud types. Cloud albedo dominates all three irradiances for Dc, while both cloud albedo and cloud fraction are influential for other cloud types. A 12 %~33 % improvement in accuracy at 6-hour lead time compared to the benchmark smart model confirms the effectiveness of incorporating physics into the models for various cloud types; further improvements are expected by directly integrating cloud type information into forecasting models by modifying the physical formulation of cloud-radiation interaction, and/or using more advanced machine learning models.

14 SOLAR ENERGY↗
DOE OSTI2023

In-situ determination of moisture- and temperature-driven deflection of an encapsulated Si photovoltaic cell

Module reliability and service lifetime are critical factors in improving photovoltaic system performance and reducing the levelized cost of electricity (LCOE). Soldering and lamination of the cell impart residual stresses that persist over time and superimpose additional loads during operation. This paper demonstrates the use of X-ray Topography (XRT) to image in-situ the dynamic response of a glass/backsheet mini-module upon drying at elevated temperature after saturation at humidity levels compatible with accelerated testing. The local water content in the encapsulant is also determined in-situ over time via Water Reflectometric Detection (WaRD), with diffusion of water in the front (glass side) and rear (backsheet side) resolved. As water diffuses out from the back of the glass/backsheet module, the cell curves towards the backsheet concomitantly. Here we find that the cell edges deflect 40μm out-of-plane with respect to its center while the encapsulant dries, compared to ~100 μm deflection when heating from 25°C to 85°C. The local cell deflections (changes in cell orientation) are correlated with the dynamic loss of water in the backside encapsulant. We conclude that the observed cell deflections are the result of hygroscopic stress induced by the encapsulant upon moisture outdiffusion. Therefore, the cell experiences a continually changing stress state and curvature dependent on local humidity and temperature. Depending on cell architecture and interconnection, this “breathing” mode of the cell may induce wear out and fatigue of the interconnects, affect the electrical connection of cracked pieces or cause failure near the interconnected edges of two cells.

14 SOLAR ENERGY↗
DOE OSTI2023

Topological band gap in intercalated epitaxial graphene

The study of functional manipulation of graphene is a critical subject, both for fundamental research and practical applications. In this study, we present that the intercalation of 5d transition metals into epitaxial graphene on SiC is a promising strategy for the realization of topologically nontrivial phases with a finite band gap in graphene. Employing first-principles calculations, grounded in density functional theory, we demonstrate that Re- and Ta-intercalated graphene evolve into two-dimensional topological insulators. These exhibit linear Dirac cones and quadratic bands with topological band gaps, respectively. The emergence of these topological states is attributed to the strong spin–orbit coupling strength of the intercalants. We show that the corresponding topological edge states persist within the finite bulk band gap, aligning with the bulk-boundary correspondence. Furthermore, we explore the spin splitting of the band structure, brought about by the inversion symmetry breaking and the spin–orbit coupling. Finally, our study underscores that the intercalation of graphene is an effective and a feasible approach for manipulating the band gap and the topological nature of graphene. Such intercalated graphene systems hold potential utility for spintronics and low-dimensional quantum device applications.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Depth-specific distribution of bacterial MAGs in permafrost active layer in Ny Ålesund, Svalbard (79°N)

Arctic soil microbial communities may shift with increasing temperatures and water availability from climate change. We examined temperature and volumetric liquid water content (VWC) in the upper 80 cm of permafrost-affected soil over 2 years (2018–2019) at the Bayelva monitoring station, Ny Ålesund, Svalbard. We show VWC increases with depth, whereas in situ temperature is more stable vertically, ranging from -5°C to 5°C seasonally. Prokaryotic metagenome-assembled genomes (MAGs) were obtained at 2–4 cm vertical resolution collected while frozen in April 2018 and at 10 cm vertical resolution collected while thawed in September 2019. The most abundant MAGs were Acidobacteriota, Actinomycetota, and Chloroflexota. Actinomycetota and Chloroflexota increase with depth, while Acidobacteriota classes Thermoanaerobaculia Gp7-AA8, Blastocatellia UBA7656, and Vicinamibacteria Vicinamibacterales are found above 6 cm, below 6 cm, and below 20cm, respectively. All MAGs have diverse carbon-degrading genes, and Actinomycetota and Chloroflexota have autotrophic genes. Further, genes encoding β -glucosidase, N-acetyl-β-D-glucosaminidase, and xylosidase increase with depth, indicating a greater potential for organic matter degradation with higher VWC. Acidobacteriota dominate the top 6 cm with their classes segregating by depth, whereas Actinomycetota and Chloroflexota dominate below ~6 cm. This suggests that Acidobacteriota classes adapt to lower VWC at the surface, while Actinomycetota and Chloroflexota persist below 6cm with higher VWC. This indicates that VWC may be as important as temperature in microbial climate change responses in Arctic mineral soils. Here we describe MAG-based Seqcode type species in the Acidobacteriota, Onstottus arcticum, Onstottus frigus, and Gilichinskyi gelida and in the Actinobacteriota, Mayfieldus profundus.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2024

Synthesis and characterization of isotopically barcoded nickel, molybdenum, and tungsten taggants for intentional nuclear forensics

Intentional nuclear forensics is a concept wherein the deliberate addition of benign and persistent material signatures to nuclear material can be used to reduce the time between the discovery of material outside of regulatory control and determination of its original provenance. One concept within intentional nuclear forensics involves the use of perturbed stable isotopes to generate unique isotope ratio “barcodes” to encode information (e.g., production batch, location, etc.) and track material throughout the nuclear fuel cycle. Synthesis of taggant species of nickel (Ni), molybdenum (Mo), and tungsten (W) was undertaken via a double-spike mechanism, wherein two highly enriched isotopes of interest per elemental taggant were mixed to form an enriched “double-spike” which was subsequently isotopically diluted with bulk material having a natural isotopic composition. Two taggant species perturbing isotopic ratios, alpha (α) and beta (β), for each of Ni, Mo, and W were synthesized. Independent measurements of double spikes and alpha and beta taggant species agreed within uncertainty and are clearly resolvable from natural compositions. High-precision analyses were independently performed by MC-ICP-MS at two U.S. National Laboratories, with consensus values and uncertainties calculated for all samples. Observed isotopic perturbations in the final taggant species measured on the order of hundreds to thousands of permille (‰) with respect to natural for isotope ratios of interest (e.g., 60 Ni/ 58 Ni, 100 Mo/ 98 Mo, 186 W/ 183 W). Discrepancies between modeled and measured isotopic compositions were observed and are largely attributed to imprecise vendor assay values for starting materials. Using measured starting material compositions as inputs for the mixing model improved the level of agreement between predicted and measured α and β taggant isotope ratios. Overall, characterization of all taggant species demonstrates that this “barcode” concept could have viability for use in nuclear forensics. Finally, it is expected that for any two-isotope mixing array dozens of isotopic barcodes could be encoded into a material system and subsequently resolved utilizing modern mass spectrometric methods.

98 NUCLEAR DISARMAMENT, SAFEGUARDS, AND PHYSICAL P↗