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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 919 records · Page 51
All sourcesNASA NTRSDOE OSTI
DOE OSTI2017

Surface Structure Dependence of the Dry Dehydrogenation of Alcohols on Cu(111) and Cu(110)

The non-oxidative dehydrogenation of alcohols is considered as an important method to produce aldehydes for the chemical industry and hydrogen gas. However, current industrial processes are oxidative, meaning that the aldehydes are formed along with water, which, in addition to being less energy efficient, poses separation problems. Herein the production of aldehydes from methanol and ethanol on clean and dry Cu(111) and Cu(110) surfaces was investigated in order to understand the catalytic anhydrous dehydrogenation of alcohols. We report both ethanol and methanol preferentially react under ultrahigh vacuum conditions at surface defects to yield acetaldehyde and formaldehyde, respectively, in the absence of surface oxygen and water. The amount of alkoxide reaction intermediates measured by scanning tunneling microscopy, and aldehyde and hydrogen products detected by temperature programmed reaction, are increased by inducing more defects in the Cu substrates with Ar ion sputtering. This work also reveals that the Cu model surfaces are not poisoned by the reaction and exhibit 100% selectivity for alcohol dehydrogenation to aldehyde and hydrogen.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2018

DMOF-1 as a Representative MOF for SO 2 Adsorption in Both Humid and Dry Conditions

The mixed-ligand metal–organic framework (MOF) DMOF-1 has been successfully synthesized via ligand: 2,3,5,6-tetramethylterephthalic acid (TM), 9,10-anthracenedicarboxylic acid (ADC), 1,4-naphthalenedicarboxylic acid (NDC), 2,5-dimethyl terephthalic acid (DM), and metal (Zn, Cu, Ni, Co) substitutions to develop structure–property relationships for adsorption of water and SO 2 , an acid gas commonly found in flue gas streams at ppm-level concentrations. The substitution of bulky ligands, TM and ADC, resulted in not only improved water stability but also stability toward dry SO 2 , whereas substitution with NDC and DM did not provide water or SO 2 stability. ADC-functionalized Zn–DMOF exhibited the greatest stability under humid SO 2 exposure of the ligand-functionalized materials that were tested. Metal substitution of Cu into the DMOF–TM structure resulted in the greatest stability of the M–DMOF–TM samples upon exposure to humid SO 2 , and Ni–DMOF–TM provided the second most stable material. Finally, these results follow the prediction of the Irving–Williams series of metal node/ligand bond strengths.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Steering the Methane Dry Reforming Reactivity of Ni/La 2 O 3 Catalysts by Controlled In Situ Decomposition of Doped La 2 NiO 4 Precursor Structures

The influence of A- and/or B-site doping of Ruddlesden-Popper perovskite materials on the crystal structure, stability, and dry reforming of methane (DRM) reactivity of specific A 2 BO 4 phases (A = La, Ba; B = Cu, Ni) has been evaluated by a combination of catalytic experiments, in situ X-ray diffraction, X-ray absorption spectroscopy (XAS), X-ray photoelectron spectroscopy (XPS), and aberration-corrected electron microscopy. At room temperature, B-site doping of La 2 NiO 4 with Cu stabilizes the orthorhombic structure ( Fmmm ) of the perovskite, while A-site doping with Ba yields a tetragonal space group ( I 4/ mmm ). We observed the orthorhombic-to-tetragonal transformation above 170 °C for La 2 Ni 0.9 Cu 0.1 O 4 and La 2 Ni 0.8 Cu 0.2 O 4 , slightly higher than for undoped La 2 NiO 4 . Loss of oxygen in interstitial sites of the tetragonal structure causes further structure transformations for all samples before decomposition in the temperature range of 400 °C-600 °C. Controlled in situ decomposition of the parent or A/B-site doped perovskite structures in a DRM mixture (CH 4 :CO 2 = 1:1) in all cases yields an active phase consisting of exsolved nanocrystalline metallic Ni particles in contact with hexagonal La 2 O 3 and a mixture of (oxy)carbonate phases (hexagonal and monoclinic La 2 O 2 CO 3 , BaCO 3 ). Differences in the catalytic activity evolve because of (i) the in situ formation of Ni-Cu alloy phases (in a composition of >7:1 = Ni:Cu) for La 2 Ni 0.9 Cu 0.1 O 4 , La 2 Ni 0.8 Cu 0.2 O 4 , and La 1.8 Ba 0.2 Ni 0.9 Cu 0.1 O 4 , (ii) the resulting Ni particle size and amount of exsolved Ni, and (iii) the inherently different reactivity of the present (oxy)carbonate species. Based on the onset temperature of catalytic DRM activity, the latter decreases in the order of La 2 Ni 0.9 Cu 0.1 O 4 ~ La 2 Ni 0.8 Cu 0.2 O 4 ≥ La 1.8 Ba 0.2 Ni 0.9 Cu 0.1 O 4 > La 2 NiO 4 > La 1.8 Ba 0.2 NiO 4 . Simple A-site doped La 1.8 Ba 0.2 NiO 4 is essentially DRM inactive. The Ni particle size can be efficiently influenced by introducing Ba into the A site of the respective Ruddlesden-Popper structures, allowing us to control the Ni particle size between 10 nm and 30 nm both for simple B-site and A-site doped structures. Hence, it is possible to steer both the extent of the metal-oxide-(oxy)carbonate interface and its chemical composition and reactivity. Counteracting the limitation of the larger Ni particle size, the activity can, however, be improved by additional Cu-doping on the B-site, enhancing the carbon reactivity. Exemplified for the La 2 NiO 4 based systems, we show how the delicate antagonistic balance of doping with Cu (rendering the La 2 NiO 4 structure less stable and suppressing coking by efficiently removing surface carbon) and Ba (rendering the La 2 NiO 4 structure more stable and forming unreactive surface or interfacial carbonates) can be used to tailor prospective DRM-active catalysts.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

Ion and Water Dynamics in the Transition from Dry to Wet Conditions in Salt-Doped PEG

The influence of the water content on ion and water transport mechanisms in polymer membranes under low to moderate hydration conditions remains poorly understood. In this study, we combine ion and water diffusivity (PFG-NMR) measurements with atomistic molecular dynamics simulations to better understand transport processes in hydrated salt-doped poly(ethylene glycol). Above the water percolation threshold, the experimental and simulated diffusivities are in good agreement with the free volume transport models. At low hydration levels, unlike dry systems, ion diffusion cannot be described by polymer segmental dynamics alone. We rationalize such observations by the interplay between ion–water and ion–polymer solvation of cations and between ion–water and cation–anion interactions for anions. Further, we demonstrate that a two-state model combining ion–water solvation and free volume transport can describe water dynamics across the entire hydration range of interest. Here, our findings provide a more encompassing analysis of ion and water transport in hydrated polyelectrolytes, specifically in the low hydration regime.

36 MATERIALS SCIENCE↗
DOE OSTI2023

High-Resolution X-ray Spectromicroscopy Reveals Process-Structure Correlations in sub-5-μm Diameter Carbon Nanotube-Polymer Composite Dry-Spun Yarns

A persistent lack of detailed and quantitative structural analysis of these hierarchical carbon nanotube (CNT) ensembles precludes establishing processing-structure-property relationships that are essential to enhance macroscale performance (e.g., in mechanical, electrical, thermal applications). Here, in this work, we use scanning transmission X-ray microscopy (STXM) to analyze the hierarchical, twisted morphology of dry-spun CNT yarns and their composites, quantifying key structural characteristics such as density, porosity, alignment, and polymer loading. As the yarn twist density increases (15,000 to 150,000 turns per meter), the yarn diameter decreased (4.4–1.4 μm) and density increased (0.55–1.26 g·cm –3 ), as intuitively expected. Yarn density, ρ, ubiquitously scaled with diameter d according to ρ ~ d –2 for all parameters studied here. Spectromicroscopy probes with 30 nm resolution and elemental specificity were employed to analyze the radial and longitudinal distribution of the oxygen-containing polymer content (~30% weight fraction), demonstrating nearly perfect filling of the voids between CNTs with a vapor-phase polymer coating and cross-linking process. These quantitative correlations highlight the intimate connections between processing conditions and yarn structure with important implications for translating the nanoscale properties of CNTs to the macroscale.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2018

NCAR Release of CAM‐SE in CESM2.0: A Reformulation of the Spectral Element Dynamical Core in Dry‐Mass Vertical Coordinates With Comprehensive Treatment of Condensates and Energy

Abstract It is the purpose of this paper to provide a comprehensive documentation of the new NCAR (National Center for Atmospheric Research) version of the spectral element (SE) dynamical core as part of the Community Earth System Model (CESM2.0) release. This version differs from previous releases of the SE dynamical core in several ways. Most notably the hybrid sigma vertical coordinate is based on dry air mass, the condensates are dynamically active in the thermodynamic and momentum equations (also referred to as condensate loading), and the continuous equations of motion conserve a more comprehensive total energy that includes condensates. Not related to the vertical coordinate change, the hyperviscosity operators and the vertical remapping algorithms have been modified. The code base has been significantly reduced, sped up, and cleaned up as part of integrating SE as a dynamical core in the CAM (Community Atmosphere Model) repository rather than importing the SE dynamical core from High‐Order Methods Modeling environment as an external code.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2021

Evaluation of the Causes of Wet-Season Dry Biases Over Amazonia in CAM5

This study investigates the causes of pronounced low precipitation bias over Amazonia in the Community Atmosphere Model version 5 (CAM5), a common feature in many global climate models. Our analysis is based on a suite of 3-day long hindcasts starting every day at 00Z from 1997 to 2012 and an AMIP simulation for the same period. The Amazonia dry bias appears by the second day in the hindcasts and is very robust for all the seasons with the largest bias magnitude during the wet season (December–February). The bias pattern and magnitude do not change much during different dynamical wind regimes on sub-seasonal time scales. We further classify the diurnal cycle of precipitation near the LBA sites from observations and hindcasts into three convective regimes: no precipitation, late afternoon deep convection, and nighttime deep convection. CAM5 can only simulate the late afternoon convective regime and completely fails to simulate the nighttime convection, which is mostly from propagating convective systems originating from remote locations. CAM5 mainly underestimates precipitation in the late afternoon and nighttime convective regimes, which occur during ~67% of wet season days and account for ~75% of accumulated precipitation amount in observations. The persistent warm temperature bias and slightly higher moisture below 850 mb likely trigger deep convection too frequently, resulting in an earlier but weaker rainfall peak in the diurnal cycle. Finally, shallow convection may not effectively transport moisture from boundary layer to the free atmosphere, which also leads to weaker deep convection events.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2026

Root Dynamics Mitigate Warm and Dry Biases over the Central United States

The central United States frequently exhibits warm and dry biases in simulations of summertime conditions, a persistent feature that remains unresolved. While previous studies linked these biases to misrepresented surface energy exchanges, the role of belowground processes remains poorly understood. Here, we demonstrate that inadequate representation of root water uptake in land surface models contributes to this bias. Using both offline Noah-MP and coupled WRF-Noah-MP simulations with static and dynamic root water uptake schemes, we show that the inclusion of dynamic root processes reduces 2-m air temperature biases and enhances precipitation, primarily by increasing the rain rate of convective systems. Offline and coupled simulations further reveal that the cooling effects and precipitation increases are amplified through positive land-atmosphere feedback, active only in the coupled model. These findings highlight an important role of root in modulating land-atmosphere interactions and underscore the need to refine root-zone processes to improve regional atmospheric simulations.

Yang, Zhao (ORCID:0000000288027130)↗
DOE OSTI2026

High-Resolution LiDAR Observations for Coupled Effects of Dry-Air Entrainment and Haze-Cloud Interactions on Cloud Vertical Structure

This study demonstrates the high-resolution profiling of cloud microphysics in a laboratory chamber using Time-Correlated Single Photon Counting (TCSPC) LiDAR. We present a novel retrieval method to derive vertical extinction (𝜎) profiles, constrained by in situ measurements, to diagnose responses to dry-air entrainment. In clean clouds, the LiDAR signals and retrieved 𝜎 remain relatively uniform, with entrainment effects confined to the upper layer. In contrast, polluted clouds exhibit strong vertical variability and a transition to a water-vapor-limited state. Entrainment significantly enhances the haze number concentration (𝑁ℎ), particularly near the bottom, creating highly height-dependent extinction profiles for polluted clouds. Our results highlight the capability of high-resolution LiDAR in capturing fine-scale vertical inhomogeneities. This approach provides a robust framework for quantifying how aerosol loading modulates entrainment sensitivity, offering new insights into the transition between buffered and water-vapor-limited regimes.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2023

Balancing elementary steps enables coke-free dry reforming of methane

Balancing kinetics, a crucial priority in catalysis, is frequently achieved by sacrificing activity of elementary steps to suppress side reactions and enhance catalyst stability. Dry reforming of methane (DRM), a process operated at high temperature, usually involves fast C-H activation but sluggish carbon removal, resulting in coke deposition and catalyst deactivation. Studies focused solely on catalyst innovation are insufficient in addressing coke formation efficiently. Herein, we develop coke-free catalysts that balance kinetics of elementary steps for overall thermodynamics optimization. Beginning from a highly active cobalt aluminum oxide (CoAl 2 O 4 ) catalyst that is susceptible to severe coke formation, we substitute aluminum (Al) with gallium (Ga), reporting a CoAl 0.5 Ga 1.5 O 4 -R catalyst that performs DRM stably over 1000 hours without observable coke deposition. We find that Ga enhances DRM stability by suppressing C-H activation to balance carbon removal. A series of coke-free DRM catalysts are developed herein by partially substituting Al from CoAl 2 O 4 with other metals.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Tuning metal-support interactions in nickel–zeolite catalysts leads to enhanced stability during dry reforming of methane

Ni-based catalysts are highly reactive for dry reforming of methane (DRM) but they are prone to rapid deactivation due to sintering and/or coking. In this study, we present a straightforward approach for anchoring dispersed Ni sites with strengthened metal-support interactions, which leads to Ni active sites embedded in dealuminated Beta zeolite with superior stability and rates for DRM. The process involves solid-state grinding of dealuminated Beta zeolites and nickel nitrate, followed by calcination under finely controlled gas flow conditions. By combining in situ X-ray absorption spectroscopy and ab initio simulations, it is elucidated that the efficient removal of byproducts during catalyst synthesis is conducted to strengthen Ni–Si interactions that suppress coking and sintering after 100 h of time-on-stream. Transient isotopic kinetic experiments shed light on the differences in intrinsic turnover frequency of Ni species and explain performance trends. This work constructs a fundamental understanding regarding the implication of facile synthesis protocols on metal-support interaction in zeolite-supported Ni sites, and it lays the needed foundations on how these interactions can be tuned for outstanding DRM performance.

36 MATERIALS SCIENCE↗
DOE OSTI2026

Weak, shallow, dry convection over Angola increases offshore stratocumulus cloud droplet number concentrations

Boundary-layer cloud interactions involving shortwave-absorbing aerosols remain one of the least understood aerosol influences on climate. Here, we find the highest stratocumulus cloud droplet number concentrations over the southeast Atlantic occur when agricultural fires coincide with synoptically-weakened surface warming over Angola, occurring June-early August. Dry convection fills a shallow continental boundary layer with smoke, and a nighttime (local solar time 2-9) land breeze transports the aerosol into the marine boundary layer. Offshore aerosol transport is strengthened by low-level easterlies from a continental pressure high southeast of Angola. Simultaneously, the South Atlantic subtropical high is weaker, allowing extensive dispersal of aerosol offshore into the boundary layer, obscuring cloud brightening from shipping. Meteorological co-variation at synoptic scales compensates for cloud brightening by the smoke. Outgoing shortwave radiation increases by 15–20% of the monthly mean in June and July when offshore droplet numbers are less but the stratocumulus deck is more developed.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2015

Fluoride-free synthesis of a Sn-BEA catalyst by dry gel conversion

Sn containing molecular sieves with BEA topology (Sn-BEA) are active Lewis catalysts for a large variety of redox reactions. However, the synthesis of Sn-BEA often requires the use of toxic chemicals (e.g. hydrofluoric acid). In this study, we demonstrated that an active Sn-BEA catalyst can be directly synthesized in a non-fluoride medium via a dry gel conversion method with the aid of seed crystals. It was shown that seeding of zeolite BEA crystals can facilitate crystal growth and lead to BEA topology with framework Sn. Furthermore, it was found that ion-exchange with ammonium ions is indispensable to retain the crystal structure during calcination. The catalytic activity of the Sn-BEA catalyst was evaluated by the isomerization of glucose and reaction of pyruvaldehyde in the aqueous phase, and compared with the conventional hydrophobic Sn-BEA synthesized in a fluoride medium. The catalytic activity of the Sn-BEA synthesized in the absence of fluoride was found to be lower than that of the conventional Sn-BEA for catalyzing the isomerization of glucose in the aqueous phase, which could be attributed to its hydrophilic surface. For the reaction of pyruvaldehyde in the aqueous phase, the Sn-BEA synthesized in this study showed similar activity to the conventional hydrophobic Sn-BEA, indicating that the catalytic activity of Sn-BEA catalysts largely depends on the type of reactions. The current work provides the first example of direct preparation of a Sn-BEA catalyst in a caustic medium.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2015

Sulfur-resistant and regenerable Ni/Co spinel-based catalysts for methane dry reforming

Oxide-supported metal catalysts were prepared in this study by thermal impregnation of highly crystalline and highly-faceted starting spinels of the form (M 0.75 Mg 0.25 )Al 2 O 4 , where M = Ni, Co, or Cu and mixtures thereof. In situ reduction at 900°C extracts the transition metals from the oxide, and the resulting catalysts contain metal crystallites with particle sizes of ~100 nm and exceedingly low dispersion, but show high activity for dry reforming of methane with turnover frequencies as large as 3.9 at 850°C. The Ni 0.37 5Cu 0.375 Mg 0.25 Al 2 O 4 catalyst shows stable methane conversion out to 12 hours on stream without performance-degrading coking. For the Ni/Co catalysts, the reforming activity and sulfur tolerance are both functions of the Ni/Co ratio and the synthesis temperature of the starting spinel, with Ni 0.375 Co 0.375 Mg 0.25 Al 2 O 4 synthesized at 1500°C displaying fast reaction kinetics even in the presence of 20 ppm H 2 S. High reforming activity is attributed to long linear lengths of high-perfection facet edges and corners on the metal crystallites. Sulfur tolerance seems to be improved by a combination of the oxygen storage capacity of the defective spinel support and its faceting that provides additional reaction sites for activation of CO 2 .

36 MATERIALS SCIENCE↗