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At least 1,549 records · Page 86

Radiolytic Impacts of Energetic Electron Irradiation on Enceladus and Mimas

Episodic overturn of the south polar terrain on Enceladus would convey radio lytic oxidants from surface irradiation by Saturn's inner magnetospheric electrons to the putative underlying polar sea and contribute to CO2 and other gas production driving the visibly active cryovolcanism. Low duty cycle of active episodes below 1 - 10 percent would raise the relative importance of the continuous radiolytic chemical energy input for mass and heat outflow, e.g. as compared to heating by gravitational tides. The "Pac-Man" thermal anomaly on Mimas most likely arises from leading-trailing asymmetry of electron irradiation and resultant radio lytic processing of the moon ice to a few centimeters of depth. The Mimas thermal anomaly distribution suggests a relatively stable surface unmodified by Enceladus-like geologic overturn or cryovolcanic activity. In both cases, the heavily irradiated skin depth corresponds to the sensible thermal layer probed by Cassini infrared measurements. Neutral gas and dust emissions from Enceladus limit energetic ion and plasma electron fluxes in the inner magnetosphere, thereby governing the irradiation of Mimas and other Saturn moons.

Cooper, J. F.↗

Biogeochemical Impact of Long-Range Transported Dust over Northern South China Sea

Transpacific transport and impact of Asian dust aerosols have been well documented (e.g., results from ACE-Asia and regional follow-on campaigns), but little is known about dust invasion to the South China Sea (SCS). On 19-21 March 2010, a fierce Asian dust storm affected large areas from the Gobi deserts to the West Pacific, including Taiwan and Hong Kong. As a pilot study of the 7-SEAS (Seven South East Asian Studies) in the northern SCS, detailed characteristics of long-range transported dust aerosols were first observed by a comprehensive set of ground-based instruments deployed at the Dongsha islands (20deg42'52" N, 116deg43'51" E). Aerosol measurements such as particle mass concentrations, size distribution, optical properties, hygroscopicity, and vertical profiles help illustrate the evolution of this dust outbreak. Our results indicate that these dust particles were mixed with anthropogenic and marine aerosols, and transported near the surface. Satellite assessment of biogeochemical impact of dust deposition into open oceans is hindered by our current inability in retrieving areal dust properties and ocean colors over an extensive period of time, particularly under the influence of cloudy conditions. In this paper, we analyze the changes of retrieved Chlorophyll-a (Chl-a) concentration over the northern SCS, considered as oligotophic waters in the spring, from long-term SeaWiFS measurements since 1997. Over the past decade, six long-range transported dust events are identified based on spatiotemporal evolutions of PM10 measurements from regional monitoring stations, with the aid of trajectory analysis. Multi-year composites of Chl-a imagery for dust event and non-dust background during March-April are applied to overcome insufficient retrievals of Chl-a due to cloudy environment. Due to anthropogenic modification within a shallow boundary layer off the densely populated and industrial southeast coast of China, the iron ion activation of deliquescent dust particles enhances the efficiency of fertilization for biological productivity. Compared to the West Pacific, the marine ecosystem in the northern SCS is much more susceptible to the biogeochemical impact of long-range transported Asian dust.

Tsay, Si-Chee↗

Huygens Crater: Insights into Noachian Volcanism, Stratigraphy, and Aqueous Processes

Huygens crater is a well preserved peak ring structure on Mars centered at 13.5 deg S, 55.5 deg E in the Noachian highlands between Terras Tyrrhena and Sabaea near the NW rim of Hellas basin. With a diameter of approximately 470 km, it uplifted and exhumed pre-Noachian crustal materials from depths greater than 25 km, penetrating below the thick, ubiquitous layer of Hellas ejecta. In addition, Huygens served as a basin for subsequent aqueous activity, including erosion/deposition by fluvial valley networks and subsurface alteration that is now exposed by smaller impacts. Younger mafic-bearing plains that partially cover the basin floor and surrounding intercrater areas were likely emplaced by later volcanism.

Ackiss, S. E.↗

Universal Scaling Laws for Solar and Stellar Atmospheric Heating: Catalog of Power-law Index between Solar Activity Proxies and Various Spectral Irradiances

The formation of extremely hot outer atmospheres is one of the most prominent manifestations of magnetic activity common to late-type dwarf stars, including the Sun. It is widely believed that these atmospheric layers, the corona, transition region, and chromosphere, are heated by the dissipation of energy transported upwards from the stellar surface by the magnetic field. This is signified by the spectral line fluxes at various wavelengths, scaled with power-law relationships against the surface magnetic flux over a wide range of formation temperatures, which are universal to the Sun and Sunlike stars of different ages and activity levels. This study describes a catalog of power-law indices between solar activity proxies and various spectral line fluxes. Compared to previous studies, we expanded the number of proxies, which now includes the total magnetic flux, total sunspot number, total sunspot area, and the F10.7 cm radio flux, and further enhanced the number of spectral lines by a factor of 2. This provides the data to study in detail the flux–flux scaling laws from the regions specified by the temperatures of the corona (log(T/K) = 6–7) to those of the chromosphere (log(T/K) ∼ 4), as well as the reconstruction of various spectral line fluxes of the Sun in the past, F-, G-, and K-type dwarfs, and the modeled stars.

Stellar coronae↗

Opinion: Aerosol Remote Sensing Over the Next Twenty Years

More than two decades ago, aerosol remote sensing underwent a revolution with the launch of the Terra and Aqua satellites. Advancement continued via additional launches carrying new passive and active sensors. Capable of retrieving parameters characterizing aerosol loading, rudimentary particle properties and in some cases aerosol layer height, the satellite view of Earth’s aerosol system came into focus.The modeling communities have made similar advances. Now the efforts have continued long enough that we can see developing trends in both remote sensing and modeling communities, allowing us to speculate about the future and how the community will approach aerosol remote sensing twenty years from now. We anticipate technology that will replace today’s standard multi-wavelength radiometers with hyperspectral and/or polarimetry all viewing in multiple angles.These will be supported by advanced active sensors with the ability to measure profiles of aerosol extinction in addition to backscatter. The result will be greater insight into aerosol particle properties. Algorithms will move from being primarily physically-based to include an increasing degree of Machine Learning methods, but physically-based techniques will not go extinct. However, the practice of applying algorithms to a single sensor will be in decline. Retrieval algorithms will encompass multiple sensors and all available ground measurements into a unifying framework, and these inverted products will be ingested directly into assimilation systems, becoming “cyborgs”: half observations, half model. In twenty years we will see a true democratization in space with nations large and small, private organizations and commercial entities of all sizes launching space sensors. With this increasing amount of data and aerosol products available, there will be a lot of bad data. User communities will organize to set standards and the large national space agencies will lead the effort to maintain quality by deploying and maintaining validation ground networks and focused field experiments. Through it all, interest will remain high in the global aerosol system and how that system affects climate, clouds, precipitation and dynamics, air quality, the environment and public health, transport of pathogens and fertilization of ecosystems, and how these processes are adapting to a changing climate.

aerosol remote sensing↗

Operando leaching of pre-incorporated Al and mechanism in transition-metal hybrids on carbon substrates for enhanced charge storage

Insufficient exposure and utilization of active sites often induces an inferior reactivity for transition-metal-based two-dimensional (2D) materials. In response, we for the first time propose a universal "nano-tailoring" strategy to incorporate abundant defects and active sites into low-crystallinity nanosheets by electrochemically leaching of Al species. With MnAl layered double hydroxides (LDHs) as a representative example, potassium-birnessite MnO 2 (AK-MnO 2 ) with oxygen vacancies and abundant edge sites is successfully produced. The oxygen vacancies are shown to help optimize the electron-transfer and ion-adsorption capability. These integrated advantages endow the AK-MnO 2 with a high capacitance value of 239 F g –1 at 100 A g –1 . By further combining with soft X-ray absorption spectroscopy techniques, we unravel that the reducibility of M 2+ in M 2+ Al-LDH serves as the key descriptor for the reconstruction rate. Here, this "nano-tailoring" strategy can provide some important implications and clues to manipulating 2D materials for efficient energy storage and conversion.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Mo Atom Rearrangement Drives Layer-Dependent Reactivity in Two-Dimensional MoS 2

Two-dimensional (2D) materials offer a valuable platform for manipulating and studying chemical reactions at the atomic level, owing to the ease of controlling their microscopic structure at the nanometer scale. While extensive research has been conducted on the structure-dependent chemical activity of 2D materials, the influence of structural transformation during the reaction has remained largely unexplored. In this work, we report the layer-dependent chemical reactivity of MoS 2 during a nitridation atomic substitution reaction and attribute it to the rearrangement of Mo atoms. Our results show that the chemical reactivity of MoS 2 decreases as the number of layers is reduced in the few-layer regime. In particular, monolayer MoS 2 exhibits significantly lower reactivity compared with its few-layer and multilayer counterparts. Atomic-resolution transmission electron microscopy (TEM) reveals that MoN nanonetworks form as reaction products from monolayer and bilayer MoS 2 , with the continuity of the MoN crystals increasing with layer number, consistent with the local conductivity mapping data. The layer-dependent reactivity is attributed to the relative stability of the hypothetically formed MoN phase, which retains the number of Mo atomic layers present in the precursor. Specifically, the low chemical reactivity of monolayer MoS 2 is attributed to the high energy cost associated with Mo atom diffusion and migration necessary to form multilayer Mo lattices in the thermodynamically stable MoN phase. In conclusion, this study underscores the critical role of lattice rearrangement in governing chemical reactivity and highlights the potential of 2D materials as versatile platforms for advancing the understanding of materials chemistry at the atomic scale.

Chemical reactivity↗

Three-dimensional vortical structures of transition in plane channel flow

Three-dimensional visualization of flwo field structures in transitional plane channel flow obtained from a numerical simulation are presented at two Reynolds numbers. It is revealed that at the one-spike stage, independent of Reynolds number, the flow is characterized by a multi-layer vortex system. In the upper layer, total vorticity vector plots indicate a high-shear layer dominated by spanwise vorticity, whereas the middle layer (corresponding approximately to the critical layer) forms a vortex loop (alpha-vortex) consisting of strong streamwise and spanwise vorticity components. At the three-spike stage, the breakdown of the vortical structure proceeds in a manner similar to frontal relaminarization of turbulent spots. This process is accompanied by intense vortex lift-up activity near the wall which seems to originate at the legs of the vortex loop trailing the high-shear layer. Finally, at the five-spike stage, it is shown that high-vorticity regions (vortical structures) develop into horseshow eddies in planes inclined to the main flow direction.

Biringen, S.↗

Accuracy in Resolving the First Hydration Layer on a Transition-Metal Oxide Surface: Experiment (AP-XPS) and Theory

Understanding the equilibrium conditions at the metal oxide/aqueous interface is a key component toward visualizing the structure of water in confined environments and differentiating the catalytic activity of transition-metal oxides. While ambient pressure X-ray photoelectron spectroscopy (AP-XPS) has been the primary technique to investigate the formation of a hydration layer on many surfaces, results over the extended relative humidity (RH) range accessible experimentally have not been compared quantitatively to theoretical predictions. With the use of first-principles theoretical methods and accumulated knowledge of AP-XPS spectral analysis, we do so here for a model surface, TiO 2 -terminated undoped SrTiO 3 (100) (STO). The measured distribution of OH and H 2 O coverages from vacuum up to the first hydration layer is in good agreement with a static density functional theory (DFT) configuration involving partial dissociation of H 2 O per Ti-atom mediated by H-bonding. Furthermore, ab initio molecular dynamics (AIMD) simulations at 300 K for select coverages (1/4, 1/2, and 1 ML) test the role of fluctuations and entropy in the competition between adsorption and dissociation with coverage. This comparison between theory and experiment for OH and H 2 O coverages on STO provides a foundation for a more quantitative assessment of the first hydration layer and associated competition between adsorption, dissociation, and H-bonding on transition-metal oxide surfaces.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Survey of microphysical properties of marine boundary-layer clouds in the Western North Atlantic

Oceanic low level clouds strongly affect the atmospheric radiation budget. Uncertainties in their microphysical properties and cover currently limit the accuracy of climate predictions. Further, studies quantifying the relative importance of aerosol and dynamics on cloud properties in specific meteorological regimes are poorly constrained by observations in the Western North Atlantic boundary layer. Low level clouds were measured during the Aerosol Cloud meTereology Interactions oVer the western ATlantic Experiment (ACTIVATE) campaign in winter and summer 2020. The two NASA LaRC research aircraft HU-25 Falcon and UC-12 B-200 King Air conducted 35 simultaneous flights to investigate aerosol-cloud interactions of maritime clouds and their impact on radiation. Number concentration, liquid water content, ice water content, and particle size distribution in the size range of 3 µm to 1460 µm in diameter were measured with the fast forward scattering cloud probe (FCDP) and 2-dimensional optical array imaging probe (2D-S) onboard the Falcon. Here, we present an overview of late winter (February-March) and late summer (August-September) oceanic cloud properties in the region 65°W to 80°W and 30°N to 40°N. We compare cloud properties in these two seasons and investigate their dependence on meteorological parameters and aerosol abundance. In a case study, we present cloud observations in a cold air outbreak event on 1 March 2020 with a specific focus on mixed-phase clouds.

microphysical properties↗

Selective CO 2 electrocatalysis at the pseudocapacitive nanoparticle/ordered-ligand interlayer

Enzymes feature the concerted operation of multiple components around an active site, leading to exquisite catalytic specificity. Realizing such configurations on synthetic catalyst surfaces remains elusive. In this article, we report a nanoparticle/ordered-ligand interlayer that contains a multi-component catalytic pocket for high-specificity CO 2 electrocatalysis. The nanoparticle/ordered-ligand interlayer comprises a metal nanoparticle surface and a detached layer of ligands in its vicinity. This interlayer possesses unique pseudocapacitive characteristics where desolvated cations are intercalated, creating an active-site configuration that enhances catalytic turnover by two orders and one order of magnitude against a pristine metal surface and nanoparticle with tethered ligands, respectively. The nanoparticle/ordered-ligand interlayer is demonstrated across several metals with up to 99% CO selectivity at marginal overpotentials and onset overpotentials of as low as 27 mV, in aqueous conditions. Furthermore, in a gas-diffusion environment with neutral media, the nanoparticle/ordered-ligand interlayer achieves nearly unit CO selectivity at high current densities (98.1% at 400 mA cm -2 ).

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Observed variability in the Fraunhofer line spectrum of solar flux, 1975 - 1980

Over the five years double-pass spectrometer observations of the Sun-as-a-star revealed significant changes in line intensities. The photospheric component weakened linearly with time 0 to 2.3%. From a lack of correlation between these line weakenings and solar activity indicators like sunspots and plage, a global variation of surface properties is inferred. Model-atmosphere analysis suggests a slight reduction in the lower-photospheric temperature gradient corresponding to a 15% increase in the mixing length within the granulation layer. Chromospheric lines such as Ca II H and K, Ca II 8543 and the CN band head weaken synchronously with solar activity. Thus, the behavior of photospheric and chromospheric lines is markedly different, with the possibility of secular change for the former.

Livingston, W.↗

Interconnected nanoconfining pore networks enhance catalyst CO 2 interaction in electrified reactive capture

Systems that sequentially capture and upgrade CO 2 from air to fuels/fuel-intermediates, such as syngas and ethylene, rely on an energy-intensive CO 2 release process. Electrified reactive capture systems transform CO 2 obtained directly from carbonate capture liquid into products. Previous reactive capture systems show a decline in Faradaic efficiencies (FE) at current densities above 200 mA/cm 2 . Here we show the chemical origins of this problem, finding that prior electrocatalyst designs failed to arrest, activate, and reduce in situ-generated CO 2 (i-CO 2 ) before it traversed the catalyst layer and entered the tailgas stream. We develop a templated synthesis to define pore structures and the sites of Ni single atoms, and find that carbon-nitrogen-based nanopores are effective in accumulating i-CO 2 via short-range, non-electrostatic interactions between CO 2 molecules and the nanochannel walls. These interactions confine and enrich i-CO 2 within the pores, enhancing its binding and activation. We report as a result carbonate electrolysis at 300 mA/cm 2 with FE to CO of 50% ± 3%, and with <1% CO 2 in the tailgas outlet stream. This corresponds to a projected energy efficiency (EE) to 2:1 syngas of 46% at 300 mA/cm 2 when H 2 is added using a water electrolyzer.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Active Aerodynamic Load Control for Wind Turbines

The goal of this project was to develop and demonstrate an advanced dielectric barrier discharge (DBD) plasma actuator technology. We set out to demonstrate the efficacy and impact of the new actuator technology as a key component of an active load control system for wind turbines. A DBD plasma actuator consists of a thin layer of dielectric material separating a pair of offset electrodes. One of those electrodes is embedded between the dielectric layer and a non-conductive substrate, while the other is exposed to air. When driven by an appropriate high voltage waveform, the device ionizes the air near the surface of the dielectric and adjacent to the exposed electrode. Collisions between the ions in the plasma and neutral air molecules result in a wall-jet – a region of induced air velocity that can be used to modify the flow around a lifting body. Use of the device near the trailing edge of a wind turbine blade, designed in such a way as to amplify the effects of the flow-modifying device, can result in large changes to the global forces experienced by the blade. Because of the fast response time of the device, it can allow the turbine to react in real time to changes in the wind associated with turbulence, wind shear, gusts, and the like, when paired with appropriate sensors and control algorithms. The goal of this project was to increase the capacity of the device to induce velocity on its surface at the levels required by large, utility-scale wind turbines. The first technical goal was to increase the induced velocity from the current industry-best of about 4 m/s to 10 m/s by modifying the electrical waveform used to drive the device and by introducing a semi-conductive surface coating to control electrostatic charge build-up on the surface. The second goal was to use the device to modify the lift on a representative airfoil in a wind tunnel, demonstrating a reduction in lift coefficient of 0.2 or better. The third goal was to produce an actuator-induced velocity of 20 m/s. Alongside our partners at the University of Texas at Dallas, we also applied modern, advanced design methods to optimize the impact of the technology on the design of wind turbines. We also had planned to install a segmented, active load control system on a test turbine to demonstrate the ability to reduce unsteady aerodynamic forces on the turbine associated with changes in the wind. The highest induced velocity achieved during this research was 11 m/s. However, practical design constraints limited the change in lift coefficient to about 0.12 for a representative airfoil in the wind tunnel at a Reynolds number of 400,000. The primary conclusion is that the plasma actuator control authority remains insufficient for practical purposes when extrapolated to Reynolds numbers over 1 million. The potential impact of the active lift control concept was evaluated through detailed simulations for three wind turbine sizes: a 3.4MW onshore turbine, a 10MW offshore turbine, and a 15MW offshore turbine. A feedback control system was designed for each turbine within two scenarios: one where the active lift control is used as a retrofit capability on the baseline design, and the other where the designers were permitted to “upscale” the turbines in order increase annual energy production. The levelized cost of energy was then evaluated for the range of turbine sizes and design configuration. It was found that the LCOE reduction associated with active lift control fell in the range of 0.7% to 7.2%, with the highest reduction associated with upscaling the 3.4MW turbine.

17 WIND ENERGY↗

Low Temperature Activation of Methane on Metal-Oxides and Complex Interfaces: Insights from Surface Science

The abundance of inexpensive, natural gas has transformed the energy landscape, whereby revealing new possibilities for sustainable chemical technologies or impacting those that have relied on traditional fossil fuels. The primary component, methane, is underutilized and wastefully exhausted, leading to anthropogenic global warming. Historically, the manipulation of methane remained “ clavis aurea ,” an insurmountable yet rewarding challenge and thus the focus of intense research. This is primarily due to an inability to dissociate C–H bonds in methane selectively, which requires a high energy penalty and is an essential prerequisite for the direct conversion of methane into a large set of value-added products. The discovery of such processes would promise an energy gainful use of natural gas benefiting several essential chemical processes associated with C1 chemistry. This first C–H bond dissociation step of the methane molecule appears in numerous catalytic mechanisms as the rate-determining step or most essential barrier sequence for all subsequent steps that follow in the production of C–C, C–O, or C x –H y –O z bonds found in value added products. A main goal is to catalytically reduce the energy barrier for the first C–H bond dissociation to be able to achieve the activation of methane at low or moderate temperatures. As such there is great value in understanding the fundamental nature of the active sites responsible for bond breaking or formation and thus be able to facilitate better control of this chemistry, leading to the development of new technologies for fuel production and chemical conversion. Surface science studies offer enhanced perspectives for a careful manipulation of bonds over the last layer atoms of catalyst surfaces, an essential factor for the design of atomically precise catalysts and unravelling of the reaction mechanism. With the advent of new surface imaging, spectroscopy, and in situ tools, it has been possible to decipher the surface chemistry of complex materials systems and further our understanding of atomic active sites on the surfaces of metals, oxides, and carbides or metal–oxide and metal–carbide interfaces. The once considered near impossible step of C–H bond activation is now observed at low temperatures with high propensity over a collection of oxide, metal–oxide, and metal–carbide systems in a conventional or inverse configuration (oxide or carbide on metal). The enabling of C–H activation at low temperature has opened interesting possibilities for the specific production of chemicals such as methanol directly from methane, a step toward facile synthesis of liquid fuels. We highlight the most recent of these results and present the key aspects of active site configurations engineered from surface science studies which enable such a simple reactive event through careful manipulation of the last surface layer of atoms found in the catalyst structure. New concepts which help in the activation and conversion of methane are discussed.

36 MATERIALS SCIENCE↗

Elucidating the Structural and Electronic Effects of Ni and Mn Cationic Incorporation on CoOOH for Efficient Benzyl Alcohol Electrooxidation

Transition-metal oxyhydroxides such as CoOOH are promising low-cost electrocatalysts for the selective electrooxidation of organic molecules, yet the influence of ubiquitous transition-metal impurities on their performance and durability remains poorly understood. Here, we experimentally probed the individual and synergistic electrochemical and structural effects of Ni and Mn incorporations into model CoOOH electrocatalysts toward an efficient benzyl alcohol oxidation reaction (BAOR). Comprehensive electrochemical, microscopic, and spectroscopic analyses reveal that Ni incorporation enhances charge-transfer kinetics and overall activity through the formation of catalytically active Ni 3+ sites, whereas Mn exhibited a more complex but interesting role. At the early stages of operation, Mn 4+ acts as a stabilizing surface layer that mitigates catalyst degradation but partially blocks Co sites before they undergo gradual leaching. The concurrent incorporation of both Ni and Mn yields a trimetallic 2NMC@NF electrocatalyst that integrates the activity benefits of Ni with the stability conferred by Mn, achieving 92.9% benzyl alcohol conversion and 91.4% Faradaic efficiency after 24 h at 1.5 V vs RHE. These findings elucidate how trace Ni and Mn impurities, often introduced from electrolytes or external sources, can modulate the lattice and electronic structure of CoOOH, offering a design strategy for enhancing both activity and long-term stability in electrocatalytic organic oxidation.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗