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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 235 records · Page 13
All sourcesNASA NTRSDOE OSTI
NASA NTRS2013

The Origin of Carbon-bearing Volatiles in Surprise Valley Hot Springs in the Great Basin: Carbon Isotope aud Water Chemistry Characterizations

There are numerous hydrothermal fields within the Great Basin of North America, some of which have been exploited for geothermal resources. With methane and other carbon-bearing compounds being observed, in some cases with high concentrations, however, their origins and formation conditions remain unknown. Thus, studying hydrothermal springs in this area provides us an opportunity to expand our knowledge of subsurface (bio)chemical processes that generate organic compounds in hydrothermal systems, and aid in future development and exploration of potential energy resources as well. While isotope measurement has long been used for recognition of their origins, there are several secondary processes that may generate variations in isotopic compositions: oxidation, re-equilibration of methane and other alkanes with CO2, mixing with compounds of other sources, etc. Therefore, in addition to isotopic analysis, other evidence, including water chemistry and rock compositions, are necessary to identify volatile compounds of different sources. Surprise Valley Hot Springs (SVHS, 41º32'N, 120º5'W), located in a typical basin and range province valley in northeastern California, is a terrestrial hydrothermal spring system of the Great Basin. Previous geophysical studies indicated the presence of clay-rich volcanic and sedimentary rocks of Tertiary age beneath the lava flows in late Tertiary and Quaternary. Water and gas samples were collected for a variety of chemical and isotope composition analyses, including in-situ pH, alkalinity, conductivity, oxidation reduction potential (ORP), major and trace elements, and C and H isotope measurements. Fluids issuing from SVHS can be classified as Na-(Cl)-SO4 type, with the major cation and anion being Na+ and SO4 2-, respectively. Thermodynamic calculation using ORP and major element data indicated that sulfate is the most dominant sulfur species, which is consistent with anion analysis results. Aquifer temperatures at depth estimated by both dissolved SiO2 and Na-K-Ca geothermometers are in the range of 125.0 to 135.4 oC, and higher than the values measured at orifices (77.3 to 90.0 oC). CO2 and homologs of straight chain alkanes (C1-C5) were identified in gas samples. Carbon isotope values of alkanes increase with carbon numbers. The 13C fractionation between CO2 and dissolved inorganic carbon suggests they are out of carbon isotope equilibrium. The hypothesis regarding the formation of carbon-bearing compounds in SVHS may involve two processes: 1) Under high heat flow conditions which are caused by regional faulting and crustal extension, original high molecular weight organic compounds (kerogens) in clay-rich rocks decomposed to generate methane and other alkane homologs. 2) The SVHS area is associated with outflow structures, and distant from the heat source. Anaerobic oxidation of methane (AOM) with sulfate at shallow depth (< 90 oC) is suggested as being responsible for the generation of CO2 in SVHS.

Fu, Qi↗
DOE OSTI2020

Transition Metal Nitrides as Promising Catalyst Supports for Tuning CO/H 2 Syngas Production from Electrochemical CO 2 Reduction

The electrochemical carbon dioxide reduction reaction (CO 2 RR) to produce synthesis gas (syngas) with tunable CO/H 2 ratios has been studied by supporting Pd catalysts on transition metal nitride (TMN) substrates. Combining experimental measurements and density functional theory (DFT) calculations, Pd-modified niobium nitride (Pd/NbN) is found to generate much higher CO and H 2 partial current densities and greater CO Faradaic efficiency than Pd-modified vanadium nitride (Pd/VN) and commercial Pd/C catalysts. In-situ X-ray diffraction identifies the formation of PdH in Pd/NbN and Pd/C under CO 2 RR conditions, whereas the Pd in Pd/VN is not fully transformed into the active PdH phase. DFT calculations show that the stabilized *HOCO and weakened *CO intermediates on PdH/NbN are critical to achieving higher CO 2 RR activity. This work suggests that NbN is a promising substrate to modify Pd, resulting in an enhanced electrochemical conversion of CO 2 to syngas with a potential reduction in precious metal loading.

25 ENERGY STORAGE↗
NASA NTRS2013

The Origin of Carbon-bearing Volatiles in Surprise Valley Hot Springs in the Great Basin: Carbon Isotope and Water Chemistry Characterizations

There are numerous hydrothermal fields within the Great Basin of North America, some of which have been exploited for geothermal resources. With methane and other carbon-bearing compounds being observed, in some cases with high concentrations, however, their origins and formation conditions remain unknown. Thus, studying hydrothermal springs in this area provides us an opportunity to expand our knowledge of subsurface (bio)chemical processes that generate organic compounds in hydrothermal systems, and aid in future development and exploration of potential energy resources as well. While isotope measurement has long been used for recognition of their origins, there are several secondary processes that may generate variations in isotopic compositions: oxidation, re-equilibration of methane and other alkanes with CO2, mixing with compounds of other sources, etc. Therefore, in addition to isotopic analysis, other evidence, including water chemistry and rock compositions, are necessary to identify volatile compounds of different sources. Surprise Valley Hot Springs (SVHS, 41 deg 32'N, 120 deg 5'W), located in a typical basin and range province valley in northeastern California, is a terrestrial hydrothermal spring system of the Great Basin. Previous geophysical studies indicated the presence of clay-rich volcanic and sedimentary rocks of Tertiary age beneath the lava flows in late Tertiary and Quaternary. Water and gas samples were collected for a variety of chemical and isotope composition analyses, including in-situ pH, alkalinity, conductivity, oxidation reduction potential (ORP), major and trace elements, and C and H isotope measurements. Fluids issuing from SVHS can be classified as Na-(Cl)-SO4 type, with the major cation and anion being Na+ and SO4(2-), respectively. Thermodynamic calculation using ORP and major element data indicated that sulfate is the most dominant sulfur species, which is consistent with anion analysis results. Aquifer temperatures at depth estimated by both dissolved SiO2 and Na-K-Ca geothermometers are in the range of 125.0 to 135.4 C, and higher than the values measured at orifices (77.3 to 90.0 C). CO2 and homologs of straight chain alkanes (C1-C5) were identified in gas samples. Carbon isotope values of alkanes increase with carbon numbers. The C-13 fractionation between CO2 and dissolved inorganic carbon suggests they are out of carbon isotope equilibrium. The hypothesis regarding the formation of carbon-bearing compounds in SVHS may involve two processes: 1) Under high heat flow conditions which are caused by regional faulting and crustal extension, original high molecular weight organic compounds (kerogens) in clay-rich rocks decomposed to generate methane and other alkane homologs. 2) The SVHS area is associated with outflow structures, and distant from the heat source. Anaerobic oxidation of methane (AOM) with sulfate at shallow depth (< 90 C) is suggested as being responsible for the generation of CO2 in SVHS.

Fu, Qi↗
DOE OSTI2022

Redox chemistry of plutonium and plutonium surrogates in vitrified nuclear wastes

Lanthanide borosilicate glasses containing Pu and the analog element, Ce, were subjects of an X-ray absorption spectroscopy investigation to quantify the +3/+4 ratio of the redox-sensitive element. The data show that the dominant oxidation states are +4 for Pu and +3 for Ce. The data also indicate that the reductive potential of glasses can be quantified, although allowances must be made for glass composition, from a solution chemistry method adapted to glass chemistry. These data can therefore be used to formulate glass compositions and processing schedules that lead to knowledge of the oxidation state of Pu in melts. Furthermore, the data show that Ce is a poor analog for Pu behavior in melt and that the suitability of surrogates can be evaluated by this method. The methods demonstrated in this paper can be used to estimate the oxidation states of a range of multi-valent elements as functions of temperature and composition with data from only a single redox couple.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2022

Oxygen–Chlorine Chemisorption Scaling for Seawater Electrolysis on Transition Metals: The Role of Redox

To clarify what controls species oxidation selectivity in seawater electrolysis, density functional theory (DFT) is used to identify chemisorption enthalpy trends and scaling relations for the simplest relevant adsorbates (O, Cl, and H) on relevant surfaces of 3d transition metals, as well as Pd and Pt, in face-centered-cubic and, if different, their ground-state crystal structures. Approximations are tested for electron exchange-correlation (XC) and van der Waals interactions to assess their ability to reproduce experimental adsorption enthalpies of H and O on Pt(111). The vdW-uncorrected generalized gradient approximation to XC of Perdew, Burke, and Ernzerhof (PBE) agrees most closely with experiments. Using DFT-PBE thereafter, it is determined that the O chemisorption enthalpy on this wide range of transition-metal surfaces is proportional to the sum of first and second atomic ionization energies, akin to a Born–Haber cycle for a redox reaction, indicating that metal redox activity controls O chemisorption strength. Then it is shown that the O and Cl chemisorption enthalpies are strongly correlated, suggesting that the transition metals considered will oxidize unselectively water and Cl – . This strong correlation appears also for crystal reduction potentials of binary oxides and chlorides, indicating a fundamental challenge for future seawater electrode materials design.

08 HYDROGEN↗
DOE OSTI2024

Elucidate the Thermal Degradation Mechanism of Y6‐Based Organic Solar Cells by Establishing Structure‐Property Correlation

Abstract Organic solar cells (OSCs) achieved performance booming benefiting from the emerging of non‐fullerene acceptors, while inadequate device stability hampers their further application. At present, the prevalent belief attributes the inevitable thermal degradation of OSC device to morphological instability caused by excessive phase separation and crystallization in the active layer during device operation. However, it is inapplicable for state‐of‐art Y6‐based devices which strongly degrade before large‐scale morphology change. Herein, an alternative degradation mechanism is elucidated wherein molecular orientation change and demixing induced performance degradation in Y6‐based devices. Distinct from IT‐4F‐based counterpart, Y6‐based devices suffer severe thermal degradation dominated by open‐circuit voltage (V OC ) and fill factor (FF) losses. TheV OC loss is attributed to molecular orientation transition of polymer donors from edge‐on to face‐on, leading to a strong built‐in potential reduction and increase in non‐radiative loss due to energy level shifting. As forFFdecay, discontinuous acceptor phases result in electron mobility decrease by over orders of magnitude, originating from the increased molecular stacking and phase separation. This work reveals the thermal degradation mechanism for Y6‐based devices and correlates the photoelectric properties with morphology instability, which will offer guidance for improving the stability of high‐performance OSCs.

Chemistry↗
DOE OSTI2020

Single‐Site, Single‐Metal‐Atom, Heterogeneous Electrocatalyst: Metal–Organic‐Framework Supported Molybdenum Sulfide for Redox Mediator‐Assisted Hydrogen Evolution Reaction

Abstract Synthesis of single‐site catalysts, whereby the local structure and surrounding chemical environments are identical, has been challenging, particularly in heterogeneous catalysis, as the support often presents spectrum of chemically distinct binding sites. Yet, the above criteria are crucial in attributing the apparent catalytic performance to the structural motif. The presented work augments on our previous work using monometallic molybdenum sulfide tethered within a zirconium‐based metal‐organic framework (MOF), NU‐1000; the monometallic nature enables all presented sites to be catalytically addressable. As the molybdenum sulfide species resided within two distinct pores (micro‐ and mesopores) of the MOF support, we have imparted uniformity in the local chemical environment by reducing the pore heterogeneity down to a single mesopore. Single‐site and single‐atom nature of the candidate catalyst was established via X‐ray diffraction measurements. Redox mediators were implemented, which, under reductive potentials, provide reduced species; they can effectively deliver the necessary reducing equivalences to the catalytic units that can otherwise not be addressed electrochemically due to the low electron mobility within the framework. Our results indicate the micropore‐allocated molybdenum sulfide is approximately four times more active as that in mesopores, whereas its catalytic mechanism is identical, underscoring the importance of controlling chemical environment beyond the active site.

Noh, Hyunho↗
DOE OSTI2025

Differentiating Ligand Tailoring and Cation Incorporation as Strategies for Tuning Heterobimetallic Cerium Complexes

Tuning of redox-active complexes featuring metals with high coordination numbers by incorporation of secondary redox-inactive cations has received far less attention than it deserves. Here, appending moderate steric bulk to a tripodal ligand framework has been tested for its influence on secondary-cation-driven structural and electrochemical tuning of cerium, a lanthanide that tends to adopt high coordination numbers. A quasi -C 3 -symmetric cerium(III) complex denoted [Ce] has been prepared that features pendant benzyloxy groups, and this work demonstrates that this species offers a site capable of binding single Na + or Ca 2+ ions. Electrochemical and UV-visible spectroscopic studies reveal equilibrium binding affinity of [Ce] for Na + in acetonitrile solvent, contrasting with tight binding of all cations in all other previously studied systems of this type. The modulated cation binding can be attributed to the bulky benzyloxy groups, which impact the thermodynamics of cation binding but do not impede the formation of cerium centers with coordination number 8 upon binding of either Na + or Ca2 + . Finally, the Ce(IV/III) reduction potential was found to be tunable under the equilibrium binding conditions, highlighting the potentially significant role that controlled structural changes can play in modulating the solution properties of heterobimetallic complexes.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2026

Electron-Deficient Phenazines: Synthesis, Structures, Redox, and Optoelectronic Properties in the Gas Phase, in Solution, and in the Solid State

High-temperature gas-phase reactions of 1,4-C4F8I2 with phenazine (PHNZ) afforded new thermally- and air-stable derivatives with cyclo-C4F8 substituents, viz. 1,2-PHNZ(C4F8), 2,3-PHNZ(C4F8), 1,2:6,7-PHNZ(C4F8)2, 1,2:7,8-PHNZ(C4F8)2, and 1,2:8,9-PHNZ(C4F8)2. Reactions in the presence of Cu powder resulted in reductive-defluorination/aromatization of some of the cyclo-C4F8 substituents to produce 2,3-PHNZ(C4F4), 2,3-PHNZ(C4HF3), and 1,2:6,7-PHNZ(C4F8)(C4F4), which are formally tri- or tetrafluoro derivatives of benzo[a]phenazine. Single-crystal X-ray diffraction structures of these compounds demonstrate the planarity of 2,3-PHNZ(C4F4) and 2,3-PHNZ(C4HF3) and ordered p-stacking in 1,2-PHNZ(C4HF3), 1,2-PHNZ(C4F4), 1,2-PHNZ(C4F8), and 2,3-PHNZ(C4F8). Low-temperature gas-phase photoelectron spectra of the PHNZ(C4F8)1,2 compounds show that they are strong electron acceptors, with the three PHNZ(C4F8)2 isomers having electron affinities exceeding that of C60. Cyclic voltammetry in acetonitrile show that the five PHNZ(C4F8)1,2 compounds exhibit reversible one-electron reductions with large positive shifts in their reduction potentials relative to unsubstituted PHNZ. Spectroelectrochemical absorption and EPR spectra of PHNZ(C4F8)1,2- • anion radicals and extensive DFT calculations revealed the significant role that the different substitution patterns have on determining the optoelectronic properties of the PHNZ(C4F8)1,2 derivatives and PHNZ(C4F8)1,2- • anion radicals. Time-resolved microwave conductivity measurements and photoluminescence spectra of blends of the PHNZ(C4F8)1,2 derivatives with the donor poly(3-hexylthiophene) (P3HT) were recorded to assess the possible use of the new compounds in optoelectronic devices.

Balser, Sebastian↗
DOE OSTI2022

Highly Reversible Sodium Metal Battery Anodes via Alloying Heterointerfaces

As a promising pathway toward low-cost, long-duration energy storage, rechargeable sodium batteries are of increasing interest. Batteries that incorporate metallic sodium as anode promise a high theoretical specific capacity of 1166 mAh g –1 , and low reduction potential of –2.71 V. The high reactivity and poor electrochemical reversibility of sodium anodes render sodium metal anode (SMA) cells among the most challenging for practical implementation. Here, the failure mechanisms of Na anodes are investigated and the authors report that loss of morphological control is not the fundamental cause of failure. Rather, it is the inherently poor anchoring/root structure of electrodeposited Na to the electrode substrate that leads to poor reversibility and cell failure. Poorly anchored Na deposits are prone to break away from the current collector, producing orphaning and poor anode utilization. Thin metallic coatings in a range of chemistries are proposed and evaluated as SMA substrates. Based on thermodynamic and ion transport considerations, such substrates undergo reversible alloying reactions with Na and are hypothesized to promote good root growth—regardless of the morphology. Among the various options, Au stands out for its ability to support long Na anode lifetime and high reversibility (Coulombic Efficiency > 98%), for coating thicknesses in the range of 10–1000 nm. Finally, as a first step toward evaluating practical utility of the anodes, their performance in Na||SPAN cells with N:P ratio close to 1:1 is evaluated.

25 ENERGY STORAGE↗
DOE OSTI2022

Temperature-Dependent Thermal and Mechanical Properties of a Wire Arc Additively Manufactured Low Transformation Temperature Steel

Recent research has studied the use of low transformation temperature (LTT) martensite steel as feedstock for wire arc additive manufacturing (WAAM) and low tensile residual stresses or compressive residual stresses were detected in the printed walls. These residual stress states help to improve printed product properties such as fatigue strength and corrosion resistance. However, the thermal and mechanical properties of WAAM printed LTT martensite steel walls are largely unknown. In this work, a printed LTT martensite steel was characterized for its thermal, metallurgical, and mechanical behavior at room and elevated temperatures. The temperature-dependent specific heat capacity, thermal expansion, atomic lattice spacing, and tensile properties were measured during both heating and cooling and related to observed microstructural features and computational thermodynamics predictions. These results revealed a large hysteresis in the martensitic transformation, with a martensite start temperature of 240 °C and austenite start temperature of 680 °C. Additional thermal cycles and specimen orientation did not affect the printed specimen austenite and martensite transformations. However, it was observed that the printed metal may exhibit tempering embrittlement at about 350 °C but further studies are needed to confirm that. Further, these results suggest that a temperature control of 250 °C to 350 °C during WAAM is needed to maximize the stress reduction potential of the LTT250 martensite steel. Opportunities for future implementation of LTT martensite steels and optimization of additive manufacturing process conditions are identified.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Performance assessment of active insulation systems in residential buildings for energy savings and peak demand reduction

Active insulation systems (AISs) in buildings are envelopes that integrate thermal insulation, thermal energy storage, and controls. Although different designs for AISs have been proposed in the literature, a comprehensive analysis of feasible AISs is lacking. This paper discusses the energy performance, peak demand reduction potential, and performance characteristics of an AIS that uses a concrete wall as thermal mass sandwiched between two solid-state thermal switches (STSs). These STSs change their thermal conductivity using an on/off metal switch to create or break a thermal bridge across the STS. This paper first describes the experimental setup, used to determine the ratio of thermal resistance during R-high (low thermal conductivity) and R-low (high thermal conductivity) states of the STSs. This ratio was then used in whole-building energy simulations to evaluate the performance of AIS walls across different climate zones with/without a freeze timer of 60 min. The timer was added to reduce the number of switches of STSs from one state to another, and hence the energy needed for these switches. Analysis of the switching frequency and interval of STSs, thermal conductivity of walls, impact of wall orientation, and heat transfer through the wall from the use of AIS at different climate zones/locations were performed. The simulation results show that the AIS can achieve energy savings ranging from ~980 to 2,290 kWh in a single-family home with a floor area of ~220 m 2 compared with an IECC 2018 baseline. We found the energy savings was higher in dry climate zones which represent 17% of residential buildings in the United States, compared to humid or marine climate.

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗
DOE OSTI2024

Decarbonization of heat pump dual fuel systems using a practical model predictive control: Field demonstration in a small commercial building

In the transition from fossil fuel to electrified heating, a concerning trend is emerging in certain regions of the US. Owners of buildings with gas-based systems leave them in place after adding heat pumps (HPs). Existing control solutions for these hybrid (dual fuel) systems are rudimentary and fall short of realizing the full carbon reduction potential of these systems. Model predictive control (MPC) is often regarded as the benchmark for achieving optimal control in integrated systems. However, in the case of small-medium commercial buildings (SMCBs), the control and communication infrastructure required to facilitate the implementation of such advanced controls is often lacking. This paper presents a field implementation of easy-to-deploy MPC for a dual fuel heating system consisting of HPs and a gas-fired furnace (GF) for SMCBs. The control system is deployed on an open-source middleware platform and utilizes low-cost sensor devices to be used for real SMCBs without major retrofits. Here, we demonstrated this MPC in a real office building with 5 HPs and 1 GF for 2 months. The test results showed that MPC reduced 27% of cost while completely eliminating GF usage by shifting 23% of the thermal load from occupied-peak time to non-occupied-non-peak times.

29 ENERGY PLANNING, POLICY, AND ECONOMY↗
DOE OSTI2025

Global techno-economic and life cycle greenhouse gas emissions assessment of solar and wind based renewable hydrogen production

This study conducts a global assessment of renewable hydrogen production pathways, focusing on techno-economic performance and life cycle greenhouse gas (GHG) emissions. It evaluates standalone solar photovoltaic (PV), wind, and hybrid PV/wind systems, integrated with proton exchange membrane (PEM) electrolyzers, through multi-objective optimization and considering embodied emissions in manufacturing PV, wind and electrolyzers. Results identify optimal configurations to minimize levelized cost of hydrogen (LCOH) and carbon intensity (CI) of hydrogen, showing potential reductions of cost and CI by 2030. Standalone PV systems can achieve LCOH values smaller than 6.5 USD/kg H 2 and CI less than 2.5 kg CO 2 eq/kg H 2 in regions with high solar irradiance, such as North Africa, the Middle East and Chile. Wind systems in regions such as Middle East, North Africa, Australia and Central United States achieve LCOH below 5 USD/kg H 2 and CI under 1.5 kg CO 2 eq/kg H 2 . Hybrid systems emerge as the optimal solution for minimizing both the LCOH and CI by maximizing the use of renewable energy. Moreover, the results also indicate that, with the technological advancements, future reduction in the capital cost of renewable energy systems and the PEM electrolyzer as well as the trade of coproduct O 2 could drive the LCOH of all the RES-based hydrogen systems below 1 USD/kg H 2 and the CI below zero in different regions as Middle East, North Africa and Central United State

08 HYDROGEN↗
DOE OSTI2026

Processing iridium foil targets for the production of radioplatinum isotopes

Dissolving noble metals remains challenging because of their high reduction potentials and tendency to passivate as oxides. This barrier is acute for iridium metal targets used to produce platinum radioisotopes, where post-irradiation processing is costly and hazardous with conventional routes. Here, we report a rapid alkali-fusion method that converts Ir metal directly into chloride media compatible with downstream separations. In the process, an Ir foil is fused with Na 2 O 2 and KCl at temperatures above the KCl melting point; the molten salt enhances heat transfer and facilitates O 2− /Na + transport to the Ir surface, overcoming Ir's oxidation resistance. The fused cake is then cooled and leached in 10 M HCl, yielding Ir in solution without specialized microwave digestion or HF. Pt separation from bulk Ir was evaluated using extraction-chromatography resins. A newly formulated ionic-liquid resin containing Cyphos IL 104 (E104) was compared with two commercial resins (TrisKem TK200 and TK201). All resins achieved >90 % Ir recovery. Pt co-recovery depended on resin chemistry: TK200 recovered 85.9 % Pt, TK201 recovered 54.1 % Pt, and E104 recovered 72.9 % Pt. This study introduces a fast, scalable dissolution route for solid Ir targets and demonstrates resin choices that tune Ir/Pt separation, lowering the barrier to routine production and purification of Pt radioisotopes.

07 ISOTOPE AND RADIATION SOURCES↗
DOE OSTI2023

Effect of water droplet growth dynamics on electrode current in fuel-cell catalyst layers

Fuel cells are a promising next-generation energy-conversion technology designed to replace internal combustion engines in transportation applications. However, much work remains to optimize them. Operation at high humidities causes liquid water droplet formation on Pt catalyst particles during oxygen reduction, potentially impeding reactant arrival to the reactive electrode. In this work, four different cases of water droplet growth in fuel-cell catalyst layers are considered: pinned or advancing droplets on a bare Pt surface, advancing droplets on a Nafion film, and water-layer growth in carbon nanopores. Transient drop growth is captured with a combination of mass, species mass, and momentum balances, and the subsequent limiting current is determined via oxygen diffusion and Tafel kinetics. Further, water droplets are found not to be mass-transfer limiting due to the relatively large liquid-gas area compared to the Pt nanoparticle. Mass-transfer-limited behavior is calculated in carbon nanopores.

25 ENERGY STORAGE↗