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At least 145 records · Page 8
All sourcesNASA NTRSDOE OSTI
DOE OSTI2025

Intrinsically Bifunctional and Tunable Tungsten Carbide Catalysts Enable Efficient PVC-Compatible Polyolefin Hydrocracking

Hydrocracking is a promising route for the chemical recycling of polyolefins (PO), converting them into short hydrocarbons over bifunctional catalysts with metal sites for hydrogenation and dehydrogenation, and Brønsted acid sites (BAS) for isomerization and C–C bond cleavage. However, PO feedstocks containing polyvinyl chloride (PVC) can release chlorine (Cl) under reaction conditions, deactivating conventional noble metal/zeolite catalysts. Moreover, the lack of site intimacy and the presence of micropores within conventional catalysts create challenges around the transport of high-molecular-weight, sterically encumbered polymer intermediates. Here, in this study, we report tungsten carbides (W x C) as a novel type of bifunctional catalysts that address these challenges. W/W 2 C phases on W x C offer “metal” sites, and −OH on WO x species introduces BAS in close proximity. The “metal”:BAS ratio can be tuned through carburization temperature, leading to a volcano-shaped activity trend reflecting the requirement for metal–BAS balance. Kinetic data demonstrate that each PO chain undergoes sequential cleavage, while trends in cracking ideality and selectivity follow those in short-alkane hydrocracking. On the per-BAS basis, W x C is more efficient than conventional bifunctional catalysts by more than an order of magnitude, due to enhanced polymer transport. They maintain or show increased activity with 10 wt % PVC in the substrate. This work establishes transition-metal carbides as earth-abundant bifunctional catalysts with unique site proximity and heteroatom compatibility. These features, along with the broad structure space for rational tuning, make them promising options to tackle specific challenges that polymer feedstocks present in hydrocracking.

Nwachukwu, Uchenna C. [Univ. of Akron, OH (United ↗
DOE OSTI2025

Tailoring the Selective Oxidation of Hydroxyl-Containing Compounds via Precisely Tuning the Hydrogen-Bond Strength of Catalyst H-Bond Acceptors

The unique performance of the enzyme is mainly achieved via weak interactions between the “outer coordination sphere” and the substrate. Inspired by this process, we developed 3D encapsulated-structure catalysts with hydrogen-bond engineering on the shell, which mimics the “outer coordination sphere” of an enzyme. Various hydrogen bond acceptors (C=O, S=O, and N–O groups) are imparted in the shell. Concentration-dependent 1H NMR, inverse-phase gas Chromatography (IGC) measurements, and DFT calculations underscore that the hydrogen bond strength between the acceptor groups and alcohol follows the order of C=O < S=O < N–O. The hydroxyl compound oxidation rate vs the hydrogen bond strength follows a volcano behavior, reminiscent of Sabatier’s principle. The performance variation among catalysts is attributed to the adsorption strength of the substrate. The proposed bioinspired design principle expands the scope of encapsulated catalysts, enabling fine regulation of catalytic activity through precise microenvironment control via weak interactions with substrates.

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

Robust Multiyear Climate Impacts of Volcanic Eruptions in Decadal Prediction Systems

Abstract Major tropical volcanic eruptions have a large impact on climate, but there have only been three major eruptions during the recent relatively well‐observed period. Models are therefore an important tool to understand and predict the impacts of an eruption. This study uses five state‐of‐the‐art decadal prediction systems that have been initialized with the observed state before volcanic aerosols are introduced. The impact of the volcanic aerosols is found by subtracting the results of a reference experiment where the volcanic aerosols are omitted. We look for the robust impact across models and volcanoes by combining all the experiments, which helps reveal a signal even if it is weak in the models. The models used in this study simulate realistic levels of warming in the stratosphere, but zonal winds are weaker than the observations. As a consequence, models can produce a pattern similar to the North Atlantic Oscillation in the first winter following the eruption, but the response and impact on surface temperatures are weaker than in observations. Reproducing the pattern, but not the amplitude, may be related to a known model error. There are also impacts in the Pacific and Atlantic Oceans. This work contributes toward improving the interpretation of decadal predictions in the case of a future large tropical volcanic eruption.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2021

Anthropogenic Perturbations to the Atmospheric Molybdenum Cycle

Abstract Molybdenum (Mo) is a key cofactor in enzymes used for nitrogen (N) fixation and nitrate reduction, and the low availability of Mo can constrain N inputs, affecting ecosystem productivity. Natural atmospheric Mo aerosolization and deposition from sources such as desert dust, sea‐salt spray, and volcanoes can affect ecosystem function across long timescales, but anthropogenic activities such as combustion, motor vehicles, and agricultural dust have accelerated the natural Mo cycle. Here we combined a synthesis of global atmospheric concentration observations and modeling to identify and estimate anthropogenic sources of atmospheric Mo. To project the impact of atmospheric Mo on terrestrial ecosystems, we synthesized soil Mo data and estimated the global distribution of soil Mo using two approaches to calculate turnover times. We estimated global emissions of atmospheric Mo in aerosols (<10 μm in diameter) to be 23 Gg Mo yr −1 , with 40%–75% from anthropogenic sources. We approximated that for the top meter of soil, Mo turnover times range between 1,000 and 1,000,000 years. In some industrialized regions, anthropogenic inputs have enhanced Mo deposition 100‐fold, lowering the soil Mo turnover time considerably. Our synthesis of global observational data, modeling, and a mass balance comparison with riverine Mo exports suggest that anthropogenic activity has greatly accelerated the Mo cycle, with potential to influence N‐limited ecosystems.

Wong, Michelle Y.↗
DOE OSTI2021

Radio Frequency Characteristics of Volcanic Lightning and Vent Discharges

In this study, we analyze the pulse width and spectral content of vent discharges and volcanic lightning flashes. We made measurements of electrical activity with a broadband very high frequency antenna (20–80 MHz) during an explosive eruption of Sakurajima volcano on November 8, 2019. The individual impulses that comprise vent discharges and volcanic lightning were analyzed to determine the fundamental width of the impulses and the rate of fall-off of their energy spectral density. The results show that vent discharges are more similar to volcanic lightning than they are different. Here, the mean pulse width for both vent discharges and volcanic lightning was 50 ns. Both types of electrical activity had similar spectral content; the average slope of the amplitude spectra was –3.4 for both. Further, examination of the pulse width and spectral slope distributions showed that while the distributions of volcanic lightning and vent discharges are statistically distinct from each other, the distribution of vent discharges is a subset of the distribution of volcanic lightning.

58 GEOSCIENCES↗
DOE OSTI2021

Spectral Element Modeling of Acoustic to Seismic Coupling Over Topography

Acoustic waves in the atmosphere are commonly recorded on seismometers as they couple into the ground. These signals, here called ground coupled airwaves, are not commonly considered in numerical modeling of infrasound propagation, which often assumes a rigid unmeshed boundary. Starting from an analytically-tractable spherical wave model, we analyze how the coupling of an acoustic wave into a planar elastic halfspace changes over a wide range of scenarios. We use energy admittance to quantify acoustic to seismic coupling over both a planar elastic halfspace and meshed topography. Our spectral element and analytic calculations have different maxima as a function of incidence angle, with very high admittance values for near-vertical incidence (maximum ≈78%). Energy admittance calculations at shallow incidence angles are much smaller (less than 1%). In simulations over the complex topography of Sakurajima Volcano, we attribute the variable spatial pattern of energy admittance to changes in earth parameters between each model. The observed pressure difference over the simulated 15 km region appears to be < 2%. While this value is relatively small, the cumulative addition over 100s of km and multiple acoustic bounce points may be significant. Acoustic to seismic coupling along the propagation path may bias long distance yield estimates, particularly when infrasound propagates over regions with steep topography or particularly slow seismic velocities, such as alluvial planes.

58 GEOSCIENCES↗
DOE OSTI2021

Synthetic Evaluation of Infrasonic Multipole Waveform Inversion

Acoustic source inversions estimate the mass flow rate of volcanic explosions or yield of chemical explosions and provide insight into potential source directionality. However, the limitations of applying these methods to complex sources and their ability to resolve a stable solution have not been investigated in detail. We perform synthetic infrasound waveform inversions that use 3-D Green’s functions for a variety of idealized and realistic deployment scenarios using both a flat plane and Yasur volcano, Vanuatu as examples. We investigate the ability of various scenarios to retrieve the input source functions and relative amplitudes for monopole and multipole (monopole and dipole) inversions. Infrasound waveform inversions appear to be a robust method to quantify mass flow rates from simple sources (monopole) using deployments of infrasound sensors placed around a source, but care should be taken when analyzing and interpreting results from more complex acoustic sources (multipole) that have significant directional components. In the examples we consider the solution is stable for monopole inversions with a signal-to-noise ratio greater than five and the dipole component is small. For most scenarios investigated, the vertical dipole component of the multipole explosion source is poorly constrained and can impact the ability to recover the other source term components. Because multipole inversions are ill-posed for many deployments, a low residual does not necessarily mean the proper source vector has been recovered. Synthetic studies are able to help investigate the limitations and place bounds on information that may be missing using monopole and multipole inversions for potentially directional sources.

58 GEOSCIENCES↗
DOE OSTI2021

Observations Show Charge Density of Volcanic Plumes is Higher Than Thunderstorms

We analyze slow electric field change and lightning mapping measurements to provide insight into the characteristics of volcanic lightning and the associated implications on charging processes and the charge structure of a Vulcanian eruption plume. Data were obtained during a multi-instrumental field campaign at Sakurajima volcano in 2015 when the Showa crater was active. We combine the electric field change and lightning mapping data from one explosive eruption on June 6, 2015 to identify individual flashes. From this, we interpret the flash type and polarity. In addition, the long-time constant of the electric field change instrument allowed measurement of the quasi-static field associated with charge separation in the eruption plume. We find that both intracloud and cloud-to-ground discharges occurred, and the polarity of cloud-to-ground discharges were all negative. The quasi-static field measurement showed the plume carried a net negative charge. We calculate both the total charge transferred by cloud-to-ground discharges and the net charge density of the eruption plume. We find that cloud-to-ground discharges transfer an average of –0.41C per flash and the net charge density was –33C/ km 3 . Here, the percent error is at least 200%, due to uncertainty in the antenna gain. We show that these estimates are consistent with lightning that is 100 m in length. Further, the average flash rate during the first 8 s following the onset of eruption was five flashes per second. After that time, the flash rate abruptly decreased, which may be related to the end of gas-thrust forcing.

58 GEOSCIENCES↗
DOE OSTI2022

Stability of a Mixed–Valence Hydrous Iron–Rich Oxide: Implications for Water Storage and Dynamics in the Deep Lower Mantle

Incorporation of water into mantle compositions can have significant effects on the phase relations in the systems. Here, we synthesized an iron-rich hexagonal hydrous phase (referred to as "HH1-phase") under the high pressure-temperature (P-T) conditions of the deep lower mantle and determined the crystal structure of the HH1-phase at 79 GPa using the multigrain crystallography method. The chemical formula obtained was Fe 12.76 O 18 H x (x ~ to 4.5) in the Fe-O-H system. To demonstrate the role of HH1-phase for water storage in multicomponent systems relevant to mantle compositions, we investigated the stability of HH1-phase in both MgO-rich pyrolitic and SiO 2 -rich basaltic compositions. Our results indicate that the HH1-phase serves as major water storage in a pyrolitic composition, whereas the Al-rich CaCl 2 -type δ-phase and SiO 2 phase are major water storage phases in a SiO 2 -rich basaltic composition. Incorporation of considerable amounts of SiO 2 , MgO, and Al 2 O 3 into the HH1-phase expands its stability field from 98 GPa in the Fe-Al-O-H system to at least 108 GPa (corresponding to similar to 2,400 km depth) in the Mg-Si-Al-Fe-O-H system. Plumes of hot upwelling rock rooted at the base of the lower mantle have been proposed as a possible origin of hotspot volcanoes. The hydrous Fe-rich HH1-phase, if included into the material of upwelling plumes, will decompose on its rising to the upper part of the lower mantle and release water. Our results should provide constraints on water storage in the deep lower mantle and have implications for deep mantle dynamics.

58 GEOSCIENCES↗
DOE OSTI2024

Characterizing the Atmospheric Mn Cycle and Its Impact on Terrestrial Biogeochemistry

Abstract The role of manganese (Mn) in ecosystem carbon (C) biogeochemical cycling is gaining increasing attention. While soil Mn is mainly derived from bedrock, atmospheric deposition could be a major source of Mn to surface soils, with implications for soil C cycling. However, quantification of the atmospheric Mn cycle, which comprises emissions from natural (desert dust, sea salts, volcanoes, primary biogenic particles, and wildfires) and anthropogenic sources (e.g., industrialization and land‐use change due to agriculture), transport, and deposition, remains uncertain. Here, we use compiled emission data sets for each identified source to model and quantify the atmospheric Mn cycle by combining an atmospheric model and in situ atmospheric concentration measurements. We estimated global emissions of atmospheric Mn in aerosols (<10 μm in aerodynamic diameter) to be 1,400 Gg Mn year −1 . Approximately 31% of the emissions come from anthropogenic sources. Deposition of the anthropogenic Mn shortened Mn “pseudo” turnover times in 1‐m‐thick surface soils (ranging from 1,000 to over 10,000,000 years) by 1–2 orders of magnitude in industrialized regions. Such anthropogenic Mn inputs boosted the Mn‐to‐N ratio of the atmospheric deposition in non‐desert dominated regions (between 5 × 10 −5 and 0.02) across industrialized areas, but that was still lower than soil Mn‐to‐N ratio by 1–3 orders of magnitude. Correlation analysis revealed a negative relationship between Mn deposition and topsoil C density across temperate and (sub)tropical forests, consisting with atmospheric Mn deposition enhancing carbon respiration as seen in in situ biogeochemical studies.

Environmental Sciences & Ecology↗
DOE OSTI2023

Episodic Magma Hammers for the 15 January 2022 Cataclysmic Eruption of Hunga Tonga‐Hunga Ha'apai

Understanding the forces and magma system dynamics on timescales of seconds to minutes remains challenging. In the January 2022 phreatoplinian Hunga Tonga-Hunga Ha'apai eruption, four remarkably similar seismic subevents within a 5-min interval occurred during the intensifying early eruptive phase. The subevents are similar in waveforms and durations (~25 s each). Each subevent begins with an unusual negative P-wave polarity which is inferred, using full-wave seismic modeling, to be caused by an upward single-force mechanism at the volcano created by a magma hammer likely in response to magma flow blockage/constriction during the early part of the eruption as discharge rapidly increased over orders of magnitude with concomitant conduit geometry evolution and instability. Our proposed episodic magma hammer model is consistent with thermodynamic and phase properties of the magmatic mixture, and yields an estimate of conduit mass flow in agreement with vent discharge rates derived from satellite imagery of plume heights.

58 GEOSCIENCES↗
DOE OSTI2023

Examining Infrasound Propagation at High Spatial Resolution Using a Nodal Seismic Array

Infrasound—acoustic waves in the atmosphere below 20 Hz—is a useful monitoring tool. Topography and atmospheric structure strongly control infrasound propagation, and at common source–receiver distances neither of these effects can be ignored when quantitative source constraints are sought. Detailed spatial measurements of the infrasound wavefield would inform propagation models and improve source estimates. However, the “large-N” deployment strategy now well-known in seismology has not yet been realized for infrasound studies. Here, we use the 900-node seismic array from the 2014 Imaging Magma Under St. Helens (iMUSH) experiment as a proxy for a large-N infrasound network, by leveraging acoustic–seismic coupled arrivals. The active-source component of iMUSH consisted of 23 shallowly buried explosions around Mount Saint Helens volcano; these explosions produced epicentral infrasound recorded on the nodes. We find that the bulk presence of ground-coupled infrasound on the nodes is controlled by wind noise and source–receiver distance, with observed arrivals for eight explosions. Explosions with the most extensive coupling produce complex spatial waveform patterns across the array. These patterns are related to both topographic and atmospheric propagation effects, as well as spatially variable site (coupling) effects. We compare our observations to simple topographic diffraction and high-resolution wind advection models, and full-wave numerical simulations. We find strong spatial correlations between (a) coupled arrival strength and modeled topographic obstruction and (b) coupled arrival time and along-path winds. Our seismoacoustic analyses and results are applicable to other existing and future nodal seismic data sets and can expand the utility of such deployments.

58 GEOSCIENCES↗
DOE OSTI2024

Volatiles and Redox Along the East African Rift

Abstract The upper mantle under the Afar Depression in the East African Rift displays some of the slowest seismic wave speeds observed globally. Despite the extreme nature of the geophysical anomaly, lavas that erupted along the East African Rift record modest thermal anomalies. We present measurements of major elements, H 2 O, S, and CO 2 , and Fe 3+ /ΣFe and S 6+ /ΣS in submarine glasses from the Gulf of Aden seafloor spreading center and olivine‐, plagioclase‐, and pyroxene‐hosted melt inclusions from Erta Ale volcano in the Afar Depression. We combine these measurements with literature data to place constraints on the temperature, H 2 O, andfO 2 of the mantle sources of these lavas as well as the initial and final pressures of melting. The Afar mantle plume is C/FOZO/PHEM in isotopic composition, and we suggest that this mantle component is damp, with 852 ± 167 ppm H 2 O, not elevated infO 2 compared to the depleted MORB mantle, and has temperatures of ∼1401–1458°C. This is similar infO 2 and H 2 O to the estimates of C/FOZO/PHEM in other locations. Using the moderate H 2 O contents of the mantle together with the moderate thermal anomaly, we find that melting begins at around 93 km depth and ceases at around 63 km depth under the Afar Depression and at around 37 km depth under the Gulf of Aden, and that ∼1%–29% partial melts of the mantle can be generated under these conditions. We speculate that the presence of melt, and not elevated temperatures or high H 2 O contents, are the cause for the prominent geophysical anomaly observed in this region.

Geochemistry & Geophysics↗
DOE OSTI2024

Seismic Features Predict Ground Motions During Repeating Caldera Collapse Sequence

Abstract Applying machine learning to continuous acoustic emissions, signals previously deemed noise, from laboratory faults and slowly slipping subduction‐zone faults, demonstrates hidden signatures are emitted that describe physical details, including fault displacement and friction. However, no evidence currently exists to demonstrate that similar hidden signals occur during seismogenic stick‐slip on earthquake faults—the damaging earthquakes of most societal interest. We show that continuous seismic emissions emitted during the 2018 multi‐month caldera collapse sequence at the Kı̄lauea volcano in Hawai'i contain hidden signatures characterizing the earthquake cycle. Multi‐spectral data features extracted from 30 s intervals of the continuous seismic emission are used to train a gradient boosted tree regression model to predict the GNSS‐derived contemporaneous surface displacement and time‐to‐failure of the upcoming collapse event. This striking result suggests that at least some faults emit such signals and provide a potential path to characterizing the instantaneous and future behavior of earthquake faults.

58 GEOSCIENCES↗
DOE OSTI2025

Structure of the Ecuadorian Upper Plate From a Joint Seismic‐Gravity Inversion

The Ecuadorian portion of the South American subduction zone presents an interesting case study in the structure and complex evolution of an upper plate. There are outstanding questions about its tectonic history, composition, and magmatic processes. While previous studies have employed ambient noise tomography to image the Ecuadorian upper plate, surface wave inversions alone often lack sensitivity at relevant shallow depths. This limitation can be overcome with an independent, complementary data set, such as gravity. We have jointly inverted Rayleigh wave phase velocities and Bouguer gravity anomalies to provide a more detailed seismic velocity model of the Ecuadorian upper plate. Our joint inversion has yielded several key improvements from previous models. First, we observe much shallower slow velocities beneath major basins (the Manabí, Progreso, and Gulf of Guayaquil), better aligning with expected basin structure. Second, we identify a high-velocity block beneath the entire forearc, corresponding to the Piñon Terrane, with velocities suggesting the presence of ultramafic material. Third, we highlight a new narrow swath of slow velocities beneath the Ecuadorian Andes, which closely follows the active volcanoes along the Eastern Cordillera. The extent of these slow velocities coincides with the termination of active arc volcanism and the predicted location of the subducted Carnegie Ridge. The predicted compositions for the mid to lower crust in the region preclude a purely compositional explanation for these velocities, suggesting that some level of partial melt is necessary.

Birkey, Andrew [Univ. of Delaware, Newark, DE (Uni↗
DOE OSTI2020

Electronic parameters in cobalt-based perovskite-type oxides as descriptors for chemocatalytic reactions

Perovskite-type transition metal (TM) oxides are effective catalysts in oxidation and decomposition reactions. Yet, the effect of compositional variation on catalytic efficacy is not well understood. The present analysis of electronic characteristics of B-site substituted LaCoO3 derivatives via in situ X-ray absorption spectroscopy (XAS) establishes correlations of electronic parameters with reaction rates: TM t2g and eg orbital occupancy yield volcano-type or non-linear correlations with NO oxidation, CO oxidation and N2O decomposition rates. Covalent O 2p-TM 3d interaction, in ultra-high vacuum, is a linear descriptor for reaction rates in NO oxidation and CO oxidation, and for N2O decomposition rates in O2 presence. Covalency crucially determines the ability of the catalytically active sites to interact with surface species during the kinetically relevant step of the reaction. The nature of the kinetically relevant step and of surface species involved lead to the vast effect of XAS measurement conditions on the validity of correlations.

Science & Technology - Other Topics↗
DOE OSTI2024

Emergence of decadal linkage between Western Australian coast and Western–central tropical Pacific

Abstract The impact of interbasin linkage on the weather/climate and ecosystems is significantly broader and profounder than that of only appearing in an individual basin. Here, we reveal that a decadal linkage of sea surface temperature (SST) has emerged between western Australian coast and western–central tropical Pacific since 1985, associated with continuous intensification of decadal variabilities (8–16 years). The rapid SST changes in both tropical Indian Ocean and Indo-Pacific warm pool in association to greenhouse gases and volcanoes are emerging factors resulting in enhanced decadal co-variabilities between these two regions since 1985. These SST changes induce enhanced convection variability over the Maritime Continent, leading to stronger easterlies in the western–central tropical Pacific during the warm phase off western Australian coast. The above changes bring about cooling in the western–central tropical Pacific and strengthened Leeuwin Current and anomalous cyclonic wind off western Australian coast, and ultimately resulting in enhanced coupling between these two regions. Our results suggest that enhanced decadal interbasin connections can offer further understanding of decadal changes under future warmer conditions.

Science & Technology - Other Topics↗
DOE OSTI2025

Automatic speech recognition predicts contemporaneous earthquake fault displacement

Abstract Significant progress has been made in probing the state of an earthquake fault by applying machine learning to continuous seismic waveforms. The breakthroughs were originally obtained from laboratory shear experiments and numerical simulations of fault shear, then successfully extended to slow-slipping faults. Here we apply the Wav2Vec-2.0 self-supervised framework for automatic speech recognition to continuous seismic signals emanating from a sequence of moderate magnitude earthquakes during the 2018 caldera collapse at the Kīlauea volcano on the island of Hawai’i. We pre-train the Wav2Vec-2.0 model using caldera seismic waveforms and augment the model architecture to predict contemporaneous surface displacement during the caldera collapse sequence, a proxy for fault displacement. We find the model displacement predictions to be excellent. The model is adapted for near-future prediction information and found hints of prediction capability, but the results are not robust. The results demonstrate that earthquake faults emit seismic signatures in a similar manner to laboratory and numerical simulation faults, and artificial intelligence models developed for encoding audio of speech may have important applications in studying active fault zones.

58 GEOSCIENCES↗