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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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All sourcesNASA NTRSDOE OSTI
NASA NTRS2013

Compound Specific Hydrogen Isotope Composition of Type II and III Kerogen Extracted by Pyrolysis-GC-MS-IRMS

The use of Hydrogen (H) isotopes in understanding oil and gas resource plays is in its infancy. Described here is a technique for H isotope analysis of organic compounds pyrolyzed from oil and gas shale-derived kerogen. Application of this technique will progress our understanding. This work complements that of Pernia et al. (2013, this meeting) by providing a novel method for the H isotope analysis of specific compounds in the characterization of kerogen extracted by analytically diverse techniques. Hydrogen isotope analyses were carried out entirely "on-line" utilizing a CDS 5000 Pyroprobe connected to a Thermo Trace GC Ultra interfaced with a Thermo MAT 253 IRMS. Also, a split of GC-separated products was sent to a DSQ II quadrupole MS to make semi-quantitative compositional measurements of the extracted compounds. Kerogen samples from five different basins (type II and III) were dehydrated (heated to 80 C overnight in vacuum) and analyzed for their H isotope compositions by Pyrolysis-GC-MS-TC-IRMS. This technique takes pyrolysis products separated via GC and reacts them in a high temperature conversion furnace (1450 C) which quantitatively forms H2, following a modified method of Burgoyne and Hayes, (1998, Anal. Chem., 70, 5136-5141). Samples ranging from approximately 0.5 to 1.0mg in size, were pyrolyzed at 800 C for 30s. Compounds were separated on a Poraplot Q GC column. Hydrogen isotope data from all kerogen samples typically show enrichment in D from low to high molecular weight compounds. Water (H2O) average deltaD = -215.2 (V-SMOW), ranging from -271.8 for the Marcellus Shale to -51.9 for the Polish Shale. Higher molecular weight compounds like toluene (C7H8) have an average deltaD of -89.7 0/00, ranging from -156.0 for the Barnett Shale to -50.0 for the Monterey Shale. We interpret these data as representative of potential H isotope exchange between hydrocarbons and sediment pore water during formation within each basin. Since hydrocarbon H isotopes readily exchange with water, these data may provide some useful information on gas-water or oil-water interaction in resource plays, and further as a possible indicator of paleo-environmental conditions. Alternatively, our data may be an indication of H isotope exchange with water and/or acid during the kerogen isolation process. Either of these interpretations will prove useful when deciphering H isotope data derived from kerogen analysis. More experiments are planned to discern these two or other possible scenarios.

Socki, Richard A.↗
DOE OSTI2026

Elucidating hydrogen isotope transport mechanisms in proton-conducting ceramics with trapping effects using TMAP8

Hydrogen isotopes play an central role in many science and engineering applications such as fuel cells, hydrogen production, and fusion energy. For these applications, hydrogen separation and extraction applications are pivotal aspects of hydrogen transports, where proton-conducting ceramics (PCCs) have shown great potential. In this study, we propose a new model for hydrogen isotope transport in PCC materials, BaZr 0.9 Y 0.1 O 2.95 (BZY) in particular, which captures behavior in both dry and wet environments. The model expands previous efforts and considers diffusion, trapping, and surface reactions (i.e., dissociation and recombination). We then validate and calibrate the model using deuterium transport measurements from experiments in both dry and wet environments. This study highlights the key role of trapping, often neglected, on hydrogen isotope transport in BZY and other PCC materials. It also explains how the commonly observed discrepancy between dry and wet behavior can be attributed to more active surface reactions and saturated traps due to the increased hydrogen presence under the wet environment. These results provide insights to optimize PCC manufacturing and usage as a hydrogen separation and extraction technology in various fields, emphasizing that lowering the trapping can reduce hydrogen isotope retention. These modeling and calibration efforts are performed using the tritium migration analysis program, version 8 (TMAP8), an open-source application designed for hydrogen isotope transport.

36 - MATERIALS SCIENCE↗
DOE OSTI2021

Hydrogen isotope fractionation using graphene and related 2-D materials. Final report

This report provides a final technical report and listing of products from the research on a research project from Clemson university, focused on use of two-dimensional materials within membranes to accomplish hydrogen ion separations. The project used CVD graphene and related 2D materials to accomplish hydrogen / deuterium / tritium (H/D/T) separation during water electrolysis in proton-exchange-membrane (PEM)-style cells. 2D materials were incorporated into PEM cells at varying places with the aim of accomplishing isotopic sieving through 2D materials by selective hydron transport at high rates and with high selectivity. The project work scope included studies on H/D separation with small-scale cells at Clemson, collaborative work between Clemson and SRNL on computational modeling and tritium separations, and issues associated with scaleup.

07 ISOTOPE AND RADIATION SOURCES↗
NASA NTRS2003

About Tagish Lake as a Potential Parent Body for Polar Micrometeorites; Clues from their Hydrogen Isotopic Compositions

The origin of the Antarctic micrometeorites (AMMs) is still a matter of debate. Their closest meteoritic counterparts are the C2 chondrites, but the match is not perfect, and the parent body(ies) of the AMMs is(are) still to be identified. Tagish Lake is a new meteorite fall which bears similarity with CI1 and CM2 chondrites, but is distinct from both. Based on the mineralogy of phyllosilicates, Noguchi et al. proposed that the phyllosilicate-rich AMMs and the Tagish Lake meteorites could derive from similar asteroids. The hydrogen isotopic compositions of extra-terrestrial samples can be used to get some insight on their origin. The D/H ratios of AMMs and of Tagish Lake have been measured, but using different analytical techniques. They are therefore not directly comparable. We performed additional hydrogen isotopic analyses of fragments of Tagish Lake using the same experimental setup previously used for the measurement of the hydrogen isotopic composition of AMMs. In this work, we could also analyze separately both lithologies of Tagish Lake (carbonate-poor and -rich). The distributions of delta D values measured in the two lithologies of Tagish Lake are very similar, indicating that fluids with similar hydrogen isotopic compositions altered the meteorite on the parent body for the two lithologies. Yet, the hydrogen isotopic composition of Tagish Lake is different from that of AMMs, suggesting that they do not derive from the same parent body.

Engrand, C.↗
NASA NTRS1992

Hydrogen and carbon isotopic composition of volatiles in Nakhla: Implications for weathering on Mars

Gases were collected at 120, 200, 300, 415, and 600 and 850 C. Hydrogen yields for the 600 and 850 C aliquots were measured separately and then the gases were combined for isotopic analysis. CO2 samples collected at the two lowest temperature steps amounted to less than 0.5 mu mole and were not analyzed isotopically. Excluding the 120 C temperature step, the bulk delta D of the sample was + 187 percent. Delta D values increase from -91 percent in the 120 C step to +518 percent in the 315 to 850 C step. The hydrogen content is greatest in the 120 C step and is roughly constant in the 200, 300, and 415 C aliquots. Between 415 C and 850 C, the yield drops off considerably. From 850 C to 950 C, virtually no H2 and only minor CO2 (less than 1 mu mole) were extracted. Using the isotopic analysis from the 300, 415, 600, and 850 C temperature collections, the bulk delta C-13 sub (PDB) is 0.0 percent. The heaviest component (delta C-13 sub (PDB) of +29 percent) was collected between 300 and 415 C. The release of hydrogen at the low temperatures reported here is consistent with the breakdown of the phases that constitute the alteration product between approx. 250 and 650 C. Although not as high as the present Martian atmosphere, the high delta D values are consistent with a Martian origin for the meteorites in question.

Watson, L. L.↗
NASA NTRS2019

Permeation Rate Equations for Hydrogen and Deuterium in a Palladium-Silver Alloy

Mass transfer of a gas through a selective, solid membrane is an effective method for separation of desired species. This selective permeability is evident in the flow of hydrogen and the isotope deuterium through palladium-silver metal alloy media. In this study, based upon Sieverts’s law and the Arrhenius diffusion equation, an empirical correlation was developed to determine the steady-state permeation rate R, dependence on media temperature T, gas supply pressure p(sub S), and gas backpressure p(sub B) on the lower pressure side. Because of an extensive range of experimental conditions and complete reporting of raw data, the research by Ackerman and Koskinas was used as a source for data allowing empirical equation fitting. Unfortunately, those authors reported best-fit equations that poorly represented their own results. To improve the modeling of the original data and demonstrate the quality of the measurements, the current study develops improved hydrogen and deuterium permeation rate equations: P = 4.22×10(exp −6) A[exp(−704/T)](sq. root p(sub S) − sq. root p(sub B))/t for hydrogen P = 2.12×10(exp −6) A[exp(−468/T )](sq. root p(sub S) − sq. root p(sub B))/t for deuterium for values of cross-sectional area A (sq.cm), medium thickness t (cm), pressure p (psia), and temperature T (Kelvin), giving a permeation rate in mole/minute. These equations model permeation rate data more closely than do several other existing literature sources.

Smith, Phillip J.↗
DOE OSTI2025

Real-Time Detection of Hydrogen and Ammonia Isotopologues for Impurity Removal and Recovery of Tritium

To accommodate gas measurements for impurity removal and recovery of tritium, a silver-coated optical or waveguide is employed for collecting Raman scattered signals to determine relative hydrogen and ammonia isotopologue populations in real time. The data and results presented here demonstrate an analytical methodology for the analysis of four ammonia and three hydrogen isotopologues in a hydrogen–deuterium exchange reaction by gas phase Raman spectroscopy. Standard chemometric modeling techniques effectively unravel the signatures of the isotopologues involved observed here; however, a sophisticated quantum chemical approach supports the spectral assignments. An interpretation of the data presented here can emphasize the practicality and reliability of the gaseous monitoring system in complex chemical environments for the hydrogen fuel economy as well as the more distant energy source from a facility that handles tritium. There are still considerable concerns about the measurement of tritium in isotope separation and radiological impurities from gas processing. A common impurity in gas processing is ammonia, which can form readily in the presence of nitrogen and tritium. Substituted ammonia (NQ 3 ), where Q = H, D, or T, is traditionally removed through getters or diffusers along with other non-hydrogen contaminants. A preferable analytical approach is noninvasive and can be deployed for real-time process evaluation in radiological environments.

Ammonia↗
DOE OSTI2022

Developments and Challenges in the Design of the ITER DRGA

We report the ITER Diagnostic Residual Gas Analyzer (DRGA) will measure the distribution of gas species, i.e., deuterium (D), tritium (T), and impurities, in the divertor exhaust stream and in the plasma periphery, with time resolution relevant to fusion plasma–wall particle dynamics. The uniqueness of the DRGA, over previous implementations of plasma dynamics residual gas analysis, is an integrated approach, combining mass and low-temperature plasma-activated optical spectroscopy, in a differentially pumped analysis station. A further unique feature of the ITER divertor-specific DRGA is an ~8-m separation of the analysis station from the sampled pumping duct, while still maintaining a ~1-s response time for hydrogen isotopic concentrations. ITER DRGA final design activities are strongly benefiting from testing of prototypical DRGA components and methods on present fusion devices, most currently on JET and W7-X. DRGA systems are implemented on both these devices and include sensors (and pumping methods) that are directly relevant to the ITER DRGA design. The recent JET-DTE2 campaign has provided the first experience on operating the combined ITER DRGA sensors with D-T plasmas. While enhancing system design for ITER, this experience on operating devices has also revealed additional engineering challenges, which further guide the continuing final design project. Meanwhile, the recent determination that the ITER DRGA, with slight optimization, will resolve the helium isotopes well enough to support an ITER pre-DT, He-3-based heating scheme, has greatly increased ITER Research Program interest in the DRGA and its implementation well ahead of the DT phase.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
NASA NTRS1991

Stable hydrogen and carbon isotope ratios of extractable hydrocarbons in the Murchison meteorite

A fairly fool-proof method to ensure that the compounds isolated from meteorites are truly part of the meteorites and not an artifact introduced by exposure to the terrestrial environment, storage, or handling is presented. The stable carbon and hydrogen isotope ratios in several of the chemical compounds extracted from the Murchison meteorite were measured. The results obtained by studying the amino acids in this meteorite gave very unusual hydrogen and carbon isotope ratios. The technique was extended to the different classes of hydrocarbons and the hydrocarbons were isolated using a variety of separation techniques. The results and methods used in this investigation are described in this two page paper.

Krishnamurthy, R. V.↗
DOE OSTI2022

Improved scaling law for the prediction of deuterium retention in beryllium co-deposits

Hydrogen isotope co-deposition with Be eroded from the first wall is expected to be the main fusion fuel retention mechanism in ITER. Since good fuel accounting is crucial for economic and safety reasons, reliable predictions of hydrogen isotope retention are needed. Furthermore, this study builds upon the well-established empirical De Temmerman scaling law that predicts D/Be ratios in co-deposited layers based on deposition temperature, deposition rate, and deuterium particle energy. Expanding the data used in the original development of the scaling law with an additional dataset obtained with more recent measurements using a different technique to the original De Temmerman approach, allows us to obtain new values for free parameters and improve the prediction capabilities of the new scaling law. In an effort to improve the model even further, scaling with D 2 background pressure was included and a new two-term model derived, describing D retention in low- and high-energy traps separately.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2025

Experimental Setup to Investigate Hydrogen Isotope Retention on Powder Samples as Slag/Dust Proxies for Advanced Fusion Reactors

Slag/dust formation is one of the critical issues regarding tritium retention in advanced fusion reactors. We upgraded an ultrahigh vacuum device, the sample exposure station (SES), to perform temperature-programmed desorption (TPD), also known as thermal desorption spectroscopy, to investigate deuterium (D) retention in powder samples that are utilized as proxies for slag/dust particles formed in fusion reactors. TPD analysis, calibrated for the desorption rate, was successfully performed on commercially available crystalline/amorphous boron (B) powder after D 2 neutral gas or D + ion exposure. We calibrated the B powder temperature measurement for TPD analysis utilizing a D 2 desorption peak from B-D bonding known for its desorption temperature ~700 K. We introduce a separation procedure of observed D TPD signals, convoluted for corresponding D retention pathways, that was necessary for TPD analysis. This is the first report on the retention of D 2 neutral gas to B, and this observation was enabled by utilizing the B powder sample, which has a larger surface area than films commonly used in laboratory experiments. In conclusion, the upgraded SES system will enable us to investigate hydrogen isotope behaviors for powder/dust samples of various elemental compositions, including metals.

Plasma-facing component debris↗
NASA NTRS1997

Observations and Modeling of the Transient General Circulation of the North Pacific Basin

The objective of this study was to clarify the role that interstellar-cloud chemistry played in forming the population of organic molecules presently found in carbonaceous meteorites. This goal was to be achieved by means of defining the isotopic components present in organic and related phases in the meteorites and thereby identify the processes and source reservoirs involved in organic synthesis in the early solar system. Isotopic analysis of separated amino acids from the Murchison meteorite yielded results that are complex and not fully interpretable at this time. Substantial inter-acid variability in D/H ratio was observed, some but not all of which could be attributed to exchange with terrestrial hydrogen. Pronounced, though smaller, variability was also found for N-15/N-14 ratios. For both D/H and N-15/N-14 data, observed meteoritic values were substantially greater than found in terrestrial materials, providing a robust constraint on degrees of possible terrestrial contamination. Also, C-13/C-12 ratios, though falling within the range of data found on earth, significantly exceeded those characteristic of naturally occurring terrestrial amino acids. Inter-acid variability in C-13/C-12 ratios was muted relative to that observed for D/H and N-15/N-14 but still lay well outside of experimental uncertainty. No systematic relationship could be observed between variations in H, C and N isotopes. Two anomalous components were also found during the course of this study. A highly (greater than 6% relative to terrestrial) N-15-depleted, N-rich compound, which has not yet been identified, co-eluted with some amino acids. Clearly the Murchison meteorite sampled nitrogen from a number of highly diverse isotopic reservoirs. In fact, from this and related studies, it is now apparent that the distribution of nitrogen isotopes in the primitive solar system was extremely inhomogeneous. The second anomalous result obtained in the present study was for an extract of 'ammonia' from Murchison. It should be noted that this sample consisted of ammonia that was probably derived from a number of different compounds present in the meteorite itself, possibly including amines and amides, as well as ammonia sensu strictu and ammonium slats. However, the significance of this analysis is that the N-15/N-14 ratio measured was much lower than those found for the meteoritic amino acids (+2% vs around + 9% relative to terrestrial). This raises an important question concerning the source of the ammonia that was involved in synthesis of the amino acids. This issue needs to be explored further.

Kerridge, John F.↗
NASA NTRS2009

A Simple Mechanism for Fractionating Oxygen Isotopes in the Solar Nebula

Lightning in the Solar Nebula is caused by the tribo-electric charging of dust grains carried by massive turbulent flows and driven by the accretion energy in the disk: it has long been one agent assumed responsible for the formation of chondrules. The degree to which charge separation can occur is dependent upon a number of factors, including the concentration of radioactive sources and the total level of ionization in the nebula, and these factors determine the maximum energy likely to be released by a single bolt. While chondrule formation requires a massive discharge, even a small lightning bolt can vaporize grains in the ionized discharge channel. Experimental studies have shown that silica, iron silicate and iron oxide grains formed from a high voltage discharge in hydrogen rich gas containing some oxygen produces solids that are enriched in O-17 and O-18 relative to the composition of the starting gas. Vaporization of silicates produces SiO, metal and free oxygen atoms in each discharge and these species will immediately begin to recondense from the hot plasma. Freshly condensed grains are incrementally enriched in heavy oxygen while the gas is enriched in O-16. Repeated evaporation and condensation of silicates in continuously occurring lightning discharges will monotonically increase the fractionation of oxygen isotopes between the O-17 and O-18 rich dust and the O-16 rich gas. The first mass independently fractionated refractory oxide particles were produced in the lab following the condensation of a flowing gas mixture containing variable amounts of hydrogen, silane, pentacarbonyl iron and oxygen that passed through a high voltage discharge powered by a Tesla coil. While the exact chemical pathway is still uncertain, the most probable reaction mechanisms involve oxidation of the growing refractory clusters by O3, OH or O atoms. This model has some interesting consequences for chemical processes in the early solar nebula. Chemical fractionation of recondensed dust evaporated via lightning discharges should be strongly time dependent. At earlier times, the accretion rate is maximal, thus driving strong turbulence, energetic grain-grain collisions, tribo-electric charging and charge separation, leading to frequent, powerful lightning discharges. As the accretion rate diminishes, turbulence decreases and lightning discharges will become both less powerful and less frequent, thus decreasing the rate of dust-gas fractionation. The most rapid increase in the formation of O-16 poor dust will occur early in nebular history. Generation of fractionated dust should be distributed throughout the inner disk. Once condensed, grain dispersal would average out any significant isotopic anomalies within the inner disk.

Nuth, Joseph A., III↗
DOE OSTI2021

Modeling Summary of ASNF in DOE Sealed Standard Canisters

A pathway for road-ready and final disposition packaging configurations for the aluminum-clad spent nuclear fuel (ANSF) fuel dictates storage within helium backfilled sealed DOE standard canisters. The typical packaging configuration for the 15-foot DOE canisters places 10 advance test reactor (ATR) elements within a Type 1a basket, and three baskets are loaded within each DOE canister. During in-reactor operations and cooling pond storage conditions, oxyhydroxide layers form on the surface of the aluminum clad fuel. These layers produce hydrogen gas over time due to the fuel’s radiation field. As part of the packing procedure, the ATR fuel should be dried to remove any residual physio-/chemi- sorbed water bound to the surface. The results of this modeling will include results at fully saturated and fully dried conditions. In addition, fuels that are currently stored at the Savannah River Site were also studied for their potential for hydrogen and pressure build up. These two additional fuels modeled were the Missouri University Research Reactor (MURR) fuel, which is packaged in the same configuration as the ATR, but with a 10-foot-tall DOE standard canister. This was selected due to its relatively high decay heat compared to other DOE-managed ASNF. The second additional fuel studied with the modeling effort was the High Flux Isotope Reactor (HFIR) fuel. This fuel is modeled as two separate DOE canisters with the inner and outer annulus split for storage. The HFIR was selected for study due to its high aluminum cladding surface area. In the associated experimental work, Task 2 - Oxyhydroxide Layer Radiolytic Gas Generation Resolution, additional tests were completed in a helium environment, and updated G-values for the radiolytic production of hydrogen from the oxyhydroxide layers were provided. These values were 2.92 ×10 -4 µmol/J at 50% relative humidity and 4.12 ×10 -4 µmol/J at 100% relative humidity. These values are lower than the value for Argon that was used in prior modeling results. In addition, prior modeling results have been completed with the G-value applied to just the mass of the corrosion layer, and this has been updated to apply the G-value for hydrogen generation to the full mass of the fuel. These two effects combine to show much smaller pressure and hydrogen build up for the sealed canister model. For a nominal scenario of stored ATR fuel, after 50 years the model results give a 1.36 atm total pressure, 7% mole percent hydrogen, for the upper decay heat, 1.51 atm total pressure, 16% mole percent hydrogen, and for upper decay heat with undried fuel 2.6 atm total pressure, 15% mole percent hydrogen. For the MURR nominal case, the model results give 1.34 atm and 6% hydrogen, for upper decay heat this gives 1.41 atm total pressure with 10.8 % hydrogen, and for upper decay heat with undried fuel, this gives 2.38 atm total pressure with 9.9% hydrogen. The nominal scenario for HFIR fuel gives 1.39 atm total pressure with 9.9% hydrogen, the upper decay heat case gives 1.43 atm with 12.1% hydrogen, and the upper decay heat with undried fuel gives 2.17 atm total pressure with 11.9% hydrogen. These results confirm the ATR scenario bounds the other intact ASNF modeled here. No case modeled yields significant oxygen, and the lower decay heat cases for all fuels modeled have hydrogen concentrations that are under the 4% flammability limit after 50 years of storage. In addition, the modeled pressures for all cases are all significantly below the 500-psi limit for the DOE standard sealed canister.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
NASA NTRS2004

Modeling of Isotope Fractionation in Stratospheric CO2, N2O, CH4, and O3: Investigations of Stratospheric Chemistry and Transport, Stratosphere-Troposphere Exchange, and Their Influence on Global Isotope Budgets

We investigated the isotopic fractionation of CH4 and hydrogen (H2) in the stratosphere by incorporating isotope-specific rate coefficients into the Lawrence Livermore National Laboratory (LLNL) 2D model and comparing the model results with new observations from the NASA ER-2 aircraft (funded through a separate task under the Upper Atmosphere Research Program). The model results reveal that fractionation which occurs in the stratosphere has a significant influence on isotope compositions in the free troposphere, an important point which had previously been ignored, unrecognized or unquantified for many long-lived trace gases, including CH4 and H2 which we have focused our efforts on to date. Our analyses of the model results and new isotope observations have also been used to test how well the kinetic isotope effects are known, at least to within the uncertainties in model chemistry and transport. Overall, these results represent an important step forward in our understanding of isotope fractionation in the atmosphere and demonstrate that stratospheric isotope fractionation cannot be ignored in modeling studies which use isotope observations in the troposphere to infer the global budgets of CH4 (an important greenhouse gas) and of H2 (a gas whose atmospheric budget must be better quantified, particularly before a large human perturbation from fuel cell use is realized). Our analyses of model results and observations from the NASA ER-2 aircraft are briefly summarized separately below for CH4, H2, and H2O and for the contribution of these modeling studies to date to our understanding of isotope fractionation for N2O, CO2, and O3 as well.

Boering, Kristie A.↗
DOE OSTI2023

Production of zirconium-88 via proton irradiation of metallic yttrium and preparation of target for neutron transmission measurements at DICER

Abstract A process for the production of tens to hundreds of GBq amounts of zirconium-88 ( 88 Zr) using proton beams on yttrium was developed. For this purpose, yttrium metal targets (≈20 g) were irradiated in a ~16 to 34 MeV proton beam at a beam current of 100–200 µA at the Los Alamos Isotope Production Facility (IPF). The 88 Zr radionuclide was produced and separated from the yttrium targets using hydroxamate resin with an elution yield of 94(5)% (1σ). Liquid DCl solution in D 2 O was selected as a suitable 88 Zr sample matrix due to the high neutron transmission of deuterium compared to hydrogen and an even distribution of 88 Zr in the sample matrix. The separated 88 Zr was dissolved in DCl and 8 µL of the obtained solution was transferred to a tungsten sample can with a 1.2 mm diameter hole using a syringe and automated filling station inside a hot cell. Neutron transmission of the obtained 88 Zr sample was measured at the Device for Indirect Capture Experiments on Radionuclides (DICER).

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
NASA NTRS2011

Hydrogen Isotope Measurements of Organic Acids and Alcohols by Pyrolysis-GC-MS-TC-IRMS

One possible process responsible for methane generation on Mars is abiotic formation by Fischer-Tropsch-type (FTT) synthesis during serpentinization reactions. Measurement of carbon and hydrogen isotopes of intermediary organic compounds can help constrain the origin of this methane by tracing the geochemical pathway during formation. Of particular interest within the context of this work is the isotopic composition of organic intermediaries produced on the surfaces of mineral catalysts (i.e. magnetite) during hydrothermal experiments, and the ability to make meaningful and reproducible hydrogen isotope measurements. Reported here are results of experiments to characterize the hydrogen isotope composition of low molecular weight organic acids and alcohols. The presence of these organic compounds has been suggested by others as intermeadiary products made during mineral surface catalyzed reactions. This work compliments our previous study characterizing the carbon isotope composition of similar low molecular weight intermediary organic compounds (Socki, et al, American Geophysical Union Fall meeting, Abstr. #V51B-2189, Dec., 2010). Our hydrogen isotope measurements utilize a unique analytical technique combining Pyrolysis-Gas Chromatograph-Mass Spectrometry-High Temperature Conversion-Isotope Ratio Mass Spectrometry (Py-GC-MS-TC-IRMS). Our technique is unique in that it carries a split of the pyrolyzed GC-separated product to a Thermo DSQ-II? quadrupole mass spectrometer as a means of making qualitative and semi-quantitative compositional measurements of separated organic compounds, therefore both chemical and isotopic measurements can be carried out simultaneously on the same sample.

Socki, Richard A.↗
DOE OSTI2024

Direct internal recycling fractions approaching unity

Direct internal recycling (DIR) refers to the process of recovering pure hydrogen isotopes (D/T) from helium and other impurities in the fusion plasma exhaust and directing them back to the fuel injection system. Increasing the exhaust fraction purified through DIR significantly reduces the size and cost of the tritium plant and provides additional benefits including reduced requirements for both the tritium startup inventory and tritium breeding ratio. Metal foil pumps (MFPs) are the dominant technology for this separation, relying on the concept of superpermeation. We recently demonstrated that PdCu foils operated at low temperature provide both exceptional flux and resilience to helium absorption as the DIR fraction is increased. Herein we design and demonstrate continuous and semi-batch DIR processes using PdCu MFPs. Under continuous processing, stable performance was observed for DIR fractions up to 92 %. In addition, we demonstrate a semi-batch process capable of extending the DIR fraction to unity (> 99.8 %). Under the experimental conditions described within a PdCu MFP area of ~22 m 2 would be sufficient to process the fusion exhaust with 92 % DIR fraction at expected flowrates of 100 Pa·m 3 ·s -1 for a future fusion power plant.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗