Hydrogen Isotope Research Articles

Prediction of performance and turbulence in ITER burning plasmas via nonlinear gyrokinetic profile prediction

Abstract Burning plasma performance, transport, and the effect of hydrogen isotope (H, D, D-T fuel mix) on confinement has been predicted for ITER baseline scenario (IBS) conditions using nonlinear gyrokinetic profile predictions. Accelerated by surrogate modeling (Rodriguez-Fernandez et al 2022 Nucl. Fusion 62 076036), high fidelity, nonlinear gyrokinetic simulations performed with the CGYRO code (Candy et al 2016 J. Comput. Phys. 324 73), were used to predict profiles of Ti , Te , and ne while including the effects of alpha heating, auxiliary power (NBI + ECH), collisional energy exchange, and radiation losses inside of r / a = 0.9. Predicted profiles and resulting energy confinement are found to produce fusion power and gain that are approximately consistent with mission goals ( P fusion = 500 MW at Q = 10) for the baseline scenario and exhibit energy confinement that is within 1σ of the H-mode energy confinement scaling. The power of the surrogate modeling technique is demonstrated through the prediction of alternative ITER scenarios with reduced computational cost. These scenarios include conditions with maximized fusion gain and an investigation of potential resonant magnetic perturbation (RMP) effects on performance with a minimal number of gyrokinetic profile iterations required (3–6). These predictions highlight the stiff ITG nature of the core turbulence predicted in the ITER baseline and demonstrate that Q > 17 conditions may be accessible by reducing auxiliary input power while operating in IBS conditions. Prediction of full kinetic profiles allowed for the projection of hydrogen isotope effects around ITER baseline conditions. The gyrokinetic fuel ion species was varied from H, D, and 50/50 D-T and kinetic profiles were predicted. Results indicate that a weak or negligible isotope effect will be observed to arise from core turbulence in IBS conditions. The resulting energy confinement, turbulence, and density peaking, and the implications for ITER operations will be discussed.

High Compression in Palladium Alloy Metal Foil Pumps

Metal foil pumps (MFPs) are key components in the direct internal recycling inner fuel cycle loop for the recovery of hydrogen isotopes from deuterium-tritium fusion exhaust. Operating under vacuum conditions, they utilize superthermal hydrogen as the feed gas in a process called superpermeation. A notable feature of MFPs is their ability to pump against a pressure gradient. This study examines the compression capabilities of PdAg and PdCu MFPs at low temperatures with a constant feed pressure of 10 Pa. At 75°C, compression ratios exceeding 200 were readily achieved, with downstream pressures exceeding 4500 Pa using PdCu. For both alloys, net fluxes decreased by only ~15% at downstream pressures of 1000 Pa, which offers potential simplifications for the downstream pump train. Performance declined markedly when the temperature was elevated to 200°C. Pump curves were constructed and advocated as the most appropriate manner to assess MFP performance. Separate pressure-driven-permeation experiments at relevant conditions were conducted, providing a direct measurement of the hydrogen dissociation constant k d , which was found to be in good agreement with the previous literature. These measurements were used to predict pump curves and maximum compression ratios by balancing superpermeation with pressure-driven permeation, achieving excellent agreement with experiment. Last, experiments using asymmetric MFPs revealed the detrimental impact that surface impurities have on performance in this system.

Hazard, risk, reliability assessment and improvement of Darlington Tritium Removal Facility (DTRF) cryogenic refrigeration system

Tritium is a radioactive isotope of hydrogen, produced in heavy water, during CANDU reactor operations by neutron absorption. The tritium removal facility at Darlington (DTRF) is used to extract tritium from the heavy water on a continuous basis and concentrates it in preparation for immobilization and storage. There are several internal and external hazards associated with the operation of DTRF, such as fires, onsite transportation accidents, exposure to radioactive materials, explosion due to Hydrogen (H2) and the release of radioactive substances from the Tritium Immobilization System. This paper conducts a risk analysis for the DTRF Cryogenic Refrigeration System, associated with both Low and High Tritium Distillation columns. This study includes hazard identification, consequence analysis and risk estimation. Fault Tree and Event Tree Analysis conducted, system reliability, availability and human reliability was considered. Consequently, methods for risk reduction and integration with improvement to CRS design is discussed.

Au(I)-Catalyzed Regioselective Hydrogen Isotope Labeling of Indoles.

The gold(I)-catalyzed hydrogen isotope exchange reaction on indoles and related heterocycles is described under mild conditions and low catalyst loadings, using CD3OD and D2O as readily available deuterium sources. C3-unsubstituted indoles are labeled at the C3 position with exquisite regioselectivity, while C3-substituted indoles are labeled at the C2 position. The method is also applicable to the regioselective tritiation of indoles. Mechanistic studies revealed the involvement of aurated indoles as key intermediates.

Transition Metal Catalyzed Deuteration via Hydrogen Isotope Exchange

Direct hydrogen isotope exchange represents a distinctive strategy for deuterium labelling, where the protium is directly replaced by deuterium. In this graphic review, we summarized the progress in deuteration via transition metal catalyzed hydrogen isotope exchange. The review was organized according to the mechanism of C-H bond activation in the homogeneous catalysis, and the heterogeneous catalysis was also discussed according to the catalyst type. Representative mechanistic processes were depicted, and proven cases for tritiation were also highlighted.

Deciphering Paleocene‐Eocene Thermal Maximum Climatic Dynamics: Insights From Oxygen and Hydrogen Isotopes in Clay Minerals of Paleosols From the Southern Pyrenees

AbstractThis study focuses on the Paleocene‐Eocene Thermal Maximum (PETM), a hyperthermal event characterized by a rapid increase in global temperature (5–8°C) over 20 ka, in the Southern Pyrenean Foreland Basin. Although there is evidence of increased flood discharge and erosion in the Southern Pyrenees, how paleoclimatic conditions and weathering evolved remains to be assessed. This study focuses on the catchment scale climatological changes recorded in the clay minerals of floodplain paleosols, giving insights into how rainfall affected the weathering regime during and after the hyperthermal event. The oxygen (δ18O) and hydrogen (δD) isotope compositions were analyzed in two clay fractions in paleosols of the Esplugafreda continental section. The clay minerals comprise a dominant smectite‐rich assemblage, which indicates a predominantly seasonal, semi‐arid climate throughout the section. Two positive excursions in the δ18O record during the Pre‐Onset Excursion (POE) and the Syn‐PETM support an increase in air near‐surface temperature. Using the δD and δ18O smectite fractionation factors, we estimate a Mean Annual Air Temperature (MAAT) of 24.2 ± 1.0°C for the POE and 27.0 ± 0.8°C for the Syn‐PETM. The δD values show a relatively stable composition during the climatic disturbance, which suggests that this mid‐latitude catchment was overall characterized by low yearly rainfall, with a peak in extreme events during the body of the PETM and a trend toward aridification during the recovery phase of the PETM, supported by the paleosol morphotype. These climatic conditions suggest a kinetically controlled weathering regime, where physical transport of the sediments played a primary role as a denudation mechanism.

Identification and prevention of gas source in goaf: Stable carbon hydrogen isotope tracer method and numerical simulation of gas flow field

Identification and prevention of gas source in goaf: Stable carbon hydrogen isotope tracer method and numerical simulation of gas flow field

Use of stable isotope combined with intact cell lipidomic by routine MALDI mass spectrometry analysis for rapid drug susceptibility assay in mycobacteria.

Rapid, accurate, and easy-to-perform diagnostic assays are required to address the current need for the diagnosis of resistant pathogens. That is particularly the case for mycobacteria, such as the human pathogen Mycobacterium tuberculosis, which requires up to 2weeks for the determination of the drug susceptibility profile using the conventional broth microdilution method. To address this challenge, we investigated the incorporation of deuterium, the stable isotope of hydrogen, into lipids as a read out of the drug susceptibility profile. Deuterium is incorporated into newly synthesized proteins or lipids in place of hydrogen as bacterial cells grow, increasing the mass of the macromolecules, which can then be observed via matrix-assisted laser desorption ionization time of flight mass spectrometry (MALDI-TOF MS). As proof-of-concept, we used the non-pathogenic Mycobacterium smegmatis mc2155 strain, which is susceptible to the aminoglycoside antibiotic kanamycin, and M.smegmatis mc2155 containing the empty vector pVV16, which is kanamycin-resistant. Bacteria were incubated in a culture medium containing 50% of deuterium oxide (D2O) and either 1 or 2 times the minimal inhibitory concentration (MIC50) of kanamycin. Lipids were then analyzed using the MBT lipid Xtract matrix combined with routine MALDI mass spectrometry in the positive ion mode to evaluate the changes in the lipid profile. Using this approach, we were able to distinguish susceptible from resistant bacteria in less than 5h, a process that would take 72 h using the conventional broth microdilution method. We therefore propose a solution for the rapid determination of drug susceptibility profiles using a phenotypic assay combining D2O stable isotope labelling and lipid analysis by routine MALDI mass spectrometry.

Selective monodeuteration enabled by bisphosphonium catalyzed ring opening processes

The selective incorporation of a deuterium atom into small molecules with high selectivity is highly valuable for medical and chemical research. Unfortunately, this remains challenging due to the complete deuteration caused by commonly used hydrogen isotope exchange strategies. We report the development of a photocatalytic selective monodeuteration protocol utilizing C–C bond as the unconventional functional handle. The synergistic combination of radical-mediated C–C bond scission and deuterium atom transfer processes enables the effective constructions of benzylic CDH moieties with high selectivity for monodeuteration. The combinational use of a bisphosphonium photocatalyst, thiol catalyst, and CH3OD deuteration agent provides operationally simple conditions for photocatalytic monodeuteration. Moreover, the photoinduced electron transfer process of the bisphosphonium photocatalyst is elucidated through a series of spectroscopy experiments, identifying a peculiar back electron transfer process that can be regulated by subsequent nucleophilic additions.

Selective Deuteration and Tritiation of Pharmaceutically Relevant Sulfoximines.

Pharmaceutical-aligned research endeavors continue to diversify, including via the installation of new chemical functionality and non-classical bioisosteres within drug design. With this, an equally high demand emerges for the direct installation of isotopic substituents into these scaffolds within drug discovery programmes, as isotopologues are essential for the elucidation of the biological efficacy and metabolic fate of the active pharmaceutical ingredient (API). The sulfoximine functional group has recently become established as a high-value unit in this context; however, general and effective methods for the synthesis of deuterium (2H, D) and tritium (3H, T) labelled analogues have remained elusive. Herein, we disclose the design and development of the first iridium-catalyzed sulfoximine-directed hydrogen isotope exchange (HIE) systems that permit the site-selective integration of a distinguishing atomic label at aromatic C(sp2)-H and more challenging C(sp3)-H moieties. Moreover, we exemplify the broad applicability of these methods within a spectrum of molecular settings, as well as in the late-stage generation of isotopically-enriched complex bioactive architectures.

Selective Deuteration and Tritiation of Pharmaceutically Relevant Sulfoximines

Pharmaceutical‐aligned research endeavors continue to diversify, including via the installation of new chemical functionality and non‐classical bioisosteres within drug design. With this, an equally high demand emerges for the direct installation of isotopic substituents into these scaffolds within drug discovery programmes, as isotopologues are essential for the elucidation of the biological efficacy and metabolic fate of the active pharmaceutical ingredient (API). The sulfoximine functional group has recently become established as a high‐value unit in this context; however, general and effective methods for the synthesis of deuterium (2H, D) and tritium (3H, T) labelled analogues have remained elusive. Herein, we disclose the design and development of the first iridium‐catalyzed sulfoximine‐directed hydrogen isotope exchange (HIE) systems that permit the site‐selective integration of a distinguishing atomic label at aromatic C(sp2)–H and more challenging C(sp3)–H moieties. Moreover, we exemplify the broad applicability of these methods within a spectrum of molecular settings, as well as in the late‐stage generation of isotopically‐enriched complex bioactive architectures.

Late-Holocene hydroclimatic change and its effect on human activity at Xiada Co on the western Tibetan Plateau

The scarcity of paleoclimate records in the western Tibetan Plateau (TP) hinders our understanding of how environmental evolution affects past human population, agriculture, and animal husbandry. Here, we utilized a range of materials to investigate the impact of climate change on human activities in the Xiada Co basin on the western TP during the Late-Holocene. We presented a continuous compound-specific hydrogen isotope record of sedimentary leaf waxes (δ2Hwax) from a sediment core of Xiada Co, and compared it to XRF core-scanning elements, brGDGT-based mean annual air temperature (MAAT) record, and fecal stanol-based human population proxy record from the same sediment core, as well as archeological evidence from the TP. The δ2Hwax exhibited a sustained increasing trend during the period from 4700 to 900 cal yr BP, followed by a generalized decrease in δ2Hwax values during 900–0 cal yr BP. The multi-proxy analysis of Xiada Co sediments revealed that the δ2Hwax values mainly reflect changes in the ISM precipitation, and are also influenced to some extent by glacier meltwater. Furthermore, a warm and humid climate condition was conducive to human habitation. Appropriate adaptation strategies, such as the herding of cold-tolerant and dry-tolerant sheep and the cultivation of barley in the western TP, led to a surge in population density during 3400–2900 cal yr BP, despite the slightly deteriorated climate background. This study confirmed the importance of choosing the right adaptive strategies to cope with climate change for human survival and development on the Tibetan Plateau.

Exploring hydrogen isotope fractionation in lipid biomolecules of freshwater algae: implications for ecological and paleoenvironmental studies

ABSTRACT Understanding the stable hydrogen isotope (δ 2H) composition and fractionation in lipid biomolecules of primary producers, such as terrestrial and aquatic plants, is crucial for deciphering past environmental conditions, as well as applying compound-specific stable isotope analysis for the study of metabolic and ecological processes. We conducted a new tracer experiment to explore the δ 2H composition of algal fatty acid biomarkers, focusing on freshwater algae, which form the base of aquatic food webs. We selected a range of algal species widely found in freshwater ecosystems and cultivated them under controlled conditions. First, we added 2H2O to ambient water as a tracer to investigate the net hydrogen isotope fractionation during algal lipid synthesis at isotopic equilibrium, which is particularly informative for paleo-geochemical studies. Then, we conducted kinetic experiments to quantify the time needed for algal fatty acids to achieve isotopic steady-state conditions in response to the change in ambient water δ 2H values. Our findings revealed substantial variability in hydrogen isotope fractionation among different algal taxa and various fatty acids. Based on taxa, different fatty acids exhibited faster integration of water hydrogen than others, but they were not necessarily in the order of the biosynthetic pathway. This experiment underscores the complexity of hydrogen isotope fractionation and the requirement for controlled laboratory studies to properly apply compound-specific stable H isotope analysis techniques in ecological and paleo-environmental studies.

Effect of Mechanical Damage on Tritium Permeability Resistance of FeAl/Al2O3 Coating on 316L Stainless Steel

Depositing a tritium permeation barrier on the surface of materials is a key method for reducing tritium permeability. During actual operational processes, the surface of the tritium permeation barrier may experience mechanical damage, such as spalling and scratches. The hydrogen permeability resistance of the coating will degrade due to such forms of mechanical damage. It is a significant engineering challenge to evaluate the impact of these damages on the coating’s tritium resistance. In this experiment, the mechanical damage to the FeAl/Al2O3 tritium permeation barrier on 316L stainless steel was simulated through scratching, debonding, and thermal shock. Subsequently, a hydrogen isotope gas drive permeation (GDP) test was conducted. The influence of the degree of mechanical damage on the coating’s tritium permeation behavior was assessed and discussed. The results indicate that, under the same damage mechanism, the coating’s tritium permeability resistance is positively correlated with the integrity of the coating. Additionally, the impact of scratches on the coating surface is more severe than that of other damage mechanisms.

Hydrogen isotope labeling unravels origin of soil-bound organic contaminant residues in biodegradability testing

Biodegradability testing in soil helps to identify safe synthetic organic chemicals but is still obscured by the formation of soil-bound ‘non-extractable’ residues (NERs). Present-day methodologies using radiocarbon or stable (13C, 15N) isotope labeling cannot easily differentiate soil-bound parent chemicals or transformation products (xenoNERs) from harmless soil-bound biomolecules of microbial degraders (bioNERs). Hypothesizing a minimal retention of hydrogen in biomolecules, we here apply stable hydrogen isotope – deuterium (D) – labeling to unravel the origin of NERs. Soil biodegradation tests with D- and 13C-labeled 2,4-D, glyphosate and sulfamethoxazole reveal consistently lower proportions of applied D than 13C in total NERs and in amino acids, a quantitative biomarker for bioNERs. Soil-bound D thus mostly represents xenoNERs and not bioNERs, enabling an efficient quantification of xenoNERs by just measuring the total bound D. D or tritium (T) labeling could thus improve the value of biodegradability testing results for diverse organic chemicals forming soil-bound residues.

Unlocking the potential of hydrogen isotopes (δ2H) in tracing riverine particulate organic matter sources and dynamics

Unlocking the potential of hydrogen isotopes (δ2H) in tracing riverine particulate organic matter sources and dynamics

Effects of different surface water flow frequencies on water use characteristics of Tamarix ramosissima in the hinterland of the Taklamakan Desert

Tamarix ramosissima is a dominant species in desert ecosystems and an ecological barrier species in arid areas, playing a crucial role in stabilizing dunes and preventing desertification. In this study, river water, groundwater, soil water, and T. ramosissima individual samples were collected from three sites in July and October 2023 at the Daliyaboyi Oasis located at the tail of the Kriya River in the hinterland of the Taklamakan Desert. The three sites are referred to as the center (SE), west (SW), and north (SN) sites within the Daliyaboyi Oasis, and each experienced different flood frequencies. The SE site experienced flooding in July and October, the SW site experienced flooding only in July, and the SN site experienced no flooding in July or October. The spatial and temporal variation in hydrogen and oxygen stable isotopes and line-conditional excess (lc-excess) in water and plant samples were analyzed, and the potential changes in water use of T. ramosissima were analyzed by the hydrogen and oxygen stable isotope and MixSIAR model. The findings indicated that the slope of SWL at the SE, SW, and SN sites was higher in July (6.77, 6.42, and 3.05, respectively) than in October (7.37, 3.30, and 2.14, respectively). The lc-excess value of the SE site did not exhibit seasonal changes; only the lc-excess values of soil water in SW and SN sites showed seasonal changes. MixSIAR results indicated frequent flood events at the SE site, with relatively constant proportions of water source utilization by T. ramosissima in July and October. In addition, shallow soil water (0–60 cm) and deeper soil water (60–80 cm) were the main water sources of T. ramosissima at SE. The SN site was slightly influenced by surface water, resulting in statistically non-significant changes in the water source utilization by T. ramosissima. Indeed, deep soil water (60–200 cm) and groundwater were the sources of water for T. ramosissima at this site. In contrast with October, the SW site experienced flood events in July, resulting in the utilization of water by T. ramosissima from the shallow soil (0–60 cm) and deep soil (60–280 cm) in July and October, respectively. Different surface water flow patterns led to different water use characteristics of T. ramosissima, which further demonstrated that T. ramosissima has high resilience and ecological plasticity. This work provides a useful reference for the implementation of effective ecological water transport measures in the Daliyaboyi Oasis and similar arid habitats.

Robinia pseudoacacia Quickly Adjusts Its Water Uptake after Rainfall in Seasonally Dry Regions

Precipitation is a key factor affecting plant growth and development in seasonally arid regions. However, most of the traditional hydrological methods mainly select typically sunny days for sampling, and the immediate water absorption strategy of plants during and after rainfall is still unclear. This study used stable hydrogen and oxygen isotope technology to study the soil moisture absorption rates of Robinia pseudoacacia and the soil moisture content at different soil layers at different sampling times (0, 6, 12, 18 and 24 h) after rainfall. The results showed that the moisture content of the shallow soil layer decreased, while that of the deep soil layer increased over time after rainfall. R. pseudoacacia mainly utilized water from the 0–20 and 20–40 cm soil layers at 6 h after rainfall, which accounted for 36.52% and 22.25% of the rainfall, respectively. At 24 h, the 40–60, 60–80 and 80–100 cm soil layers contributed 25.25%, 18.44% and 24.45% of the water content, respectively. The shallow soil layer retained more rainfall within 6 h after rain fell, and the water retention ratio of the medium–shallow soil layer (0–60 cm) increased to 48.4%, retaining more water at 14–20 h. At 12 h, the medium–shallow soil layer (0–60 cm), runoff and groundwater constituted 37.1%, 14.4% and 15.7% of the precipitation, respectively, and rainfall retained in the deep soil layer (60–100 cm) accounted for 32.8%. In summary, R. pseudoacacia tends to use a large amount of shallow soil water in seasonally arid regions when precipitation supplements the surface soil moisture content and it utilizes deep soil water when the rainfall infiltrates and recharges the deep soil layer. Since R. pseudoacacia is sensitive to precipitation, it can quickly adjust its water absorption depth range during the short-term rainfall period to absorb as much precipitation as possible.

Ways of Preparing and Using Biologically Active and Medicinal Compounds Labeled with Hydrogen Isotopes (Review)

Ways of Preparing and Using Biologically Active and Medicinal Compounds Labeled with Hydrogen Isotopes (Review)

Groundwater renewal time by environmental tritium isotopes as a tracer for sustainable water resource management

Studying groundwater renewal time is a valuable tool to deepen the comprehension of sustainable groundwater resources specific to arid regions. Tritium is a radioactive isotope of hydrogen often used as an environmental tracer to study groundwater renewal time. The present work reports groundwater renewal times by the environmental tracer tritium to understand sustainable water resources in arid regions. First, groundwater samples were collected from wells in northeastern arid regions of Saudi Arabia. Then, an electrolysis process was employed to significantly increase the tritium level from twenty-five to thirty times the original concentration. Subsequently, the enriched water was analyzed using a liquid scintillation counter under optimized measurement conditions to determine the tritium concentration precisely. Two internationally recognized tritium laboratories conducted independent assessments to validate the estimated tritium levels. The verified tritium concentration was then used to estimate the groundwater renewal time using the Morgenstern and Pimenta curves. The results suggest that most of the monitored wells in the surveyed areas are more than a century old. Conversely, a few monitoring wells exhibit renewal times of several hundred years and may be considered nonrenewable water sources. These studies help to understand the geochemical characteristics of arid regions to ensure the sustainable management and protection of groundwater resources.