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At least 883 records · Page 49

Atomically Dispersed Au-(OH) x Species Bound on Titania Catalyze the Low-Temperature Water-Gas Shift Reaction

We report a new method for stabilizing appreciable loadings (~1 wt %) of isolated gold atoms on titania and show that these catalyze the low-temperature water-gas shift reaction. The method combines a typical gold deposition/precipitation method with UV irradiation of the titania support suspended in ethanol. Dissociation of H 2 O on the thus-created Au–O–TiO x sites is facile. At higher gold loadings, nanoparticles are formed, but they were shown to add no further activity to the atomically bound gold on titania. Removal of this “excess” gold by sodium cyanide leaching leaves the activity intact and the atomically dispersed gold still bound on titania. The new materials may catalyze a number of other reactions that require oxidized active metal sites.

Yang, Ming↗

A Nanocavitation Approach to Understanding Water Capture, Water Release, and Framework Physical Stability in Hierarchically Porous MOFs

Chemically stable metal–organic frameworks (MOFs) featuring interconnected hierarchical pores have proven to be promising for a remarkable variety of applications. Nevertheless, the framework’s susceptibility to capillary-force-induced pore collapse, especially during water evacuation, has often limited practical applications. Methodologies capable of predicting the relative magnitudes of these forces as functions of the pore size, chemical composition of the pore walls, and fluid loading would be valuable for resolution of the pore collapse problem. Here, we report that a molecular simulation approach centered on evacuation-induced nanocavitation within fluids occupying MOF pores can yield the desired physical-force information. Here, the computations can spatially pinpoint evacuation elements responsible for collapse and the chemical basis for mitigation of the collapse of modified pores. Experimental isotherms and difference-electron density measurements of the MOF NU-1000 and four chemical variants validate the computational approach and corroborate predictions regarding relative stability, anomalous sequence of pore-filling, and chemical basis for mitigation of destructive forces.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Dynamic crossover in deeply cooled water confined in MCM-41 at 4 kbar and its relation to the liquid-liquid transition hypothesis

With quasi-elastic neutron scattering, we study the single-particle dynamics of the water confined in a hydrophilic silica material, MCM-41, at 4 kbar. A dynamic crossover phenomenon is observed at 219 K. We compare this dynamic crossover with the one observed at ambient pressure and find that (a) above the crossover temperature, the temperature dependence of the characteristic relaxation time at ambient pressure exhibits a more evident super-Arrhenius behavior than that at 4 kbar. Especially, at temperatures below about 230 K, the relaxation time at 4 kbar is even smaller than that at ambient pressure. This feature is different from many other liquids. (b) Below the crossover temperature, the Arrhenius behavior found at ambient pressure has a larger activation energy compared to the one found at 4 kbar. We ascribe the former to the difference between the local structure of the low-density liquid (LDL) phase and that of the high-density liquid (HDL) phase, and the latter to the difference between the strength of the hydrogen bond of the LDL and that of the HDL. Therefore, we conclude that the phenomena observed in this paper are consistent with the LDL-to-HDL liquid-liquid transition hypothesis.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Effect of the Water and Barrier Submersion Depths on the Characteristics of a High-Voltage Discharge Propagating over a Water Surface

This work continues the series of studies of pulsed high-voltage discharges propagating over liquid surfaces in the presence of barriers. In this work, the influence of the barrier position relative to the air electrode on the discharge voltage in the stage of the completed discharge is analyzed. The effect of the water depth and barrier submersion depth on the propagation of a pulsed discharge is studied.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Central Valley Water Resources: Improving California Groundwater Assessments using GRACE and InSAR Datasets for Water Resource Management

California’s Central Valley is one of the most productive agricultural areas in the world, producing approximately $20 billion in crops annually. The recent California droughts of 2007-2010 and 2012-2019 resulted in increased groundwater pumping in the Central Valley to adequately irrigate farmland. Overdrafting of the Central Valley aquifer results in groundwater depletion, land subsidence, and permanent loss of groundwater storage. In 2014, depletion of groundwater led the state of California to enact the Sustainable Groundwater Management Act (SGMA),requiring critically overdrafted, high, and medium priority sub-basins to reach sustainable levels of groundwater pumping and recharge by 2042. SGMA allows local Groundwater Sustainability Agencies (GSAs) the authority to create Groundwater Sustainability Plans (GSPs) at the sub-basin level. To assist California’s Department of Water Resources (DWR), this project quantified groundwater change and land subsidence in Central Valley sub-basins with sparse or unreliable well and Geographic Positioning Systems (GPS) data. This was done using NASA’s Gravity Recovery and Climate Experiment (GRACE), GRACE FollowOn (GRACE-FO), and interferograms derived from Sentinel-1 C-band Synthetic Aperture Radar (C-SAR) and Advanced Land Observing Satellite 2 (ALOS-2)Phased Array L-band Synthetic Aperture Radar 2 (PALSAR-2). Time series of the GRACE and InSAR data were compared with well and GPS data in data-dense sub-basins to determine the feasibility of these datasets for groundwater storage and subsidence monitoring. We found that GRACE and InSAR data are effective tools for determining groundwater change and land subsidence and can be used on their own to monitor sub-basins in the absence of well and GPS data

Water Resources↗

Central Valley Water Resources: Improving California Groundwater Assessments using GRACE and InSAR Datasets for Water Resource Management

California’s Central Valley is one of the most productive agricultural areas in the world, producing approximately $20 billion in crops annually. The recent California droughts of 2007-2010 and 2011-2017 resulted in increased groundwater pumping in the Central Valley to adequately irrigate farmland. Overdrafting of the Central Valley aquifer results in groundwater depletion, land subsidence, and permanent loss of groundwater storage. In 2014, depletion of groundwater led the state of California to enact the Sustainable Groundwater Management Act (SGMA), requiring critically overdrafted, high, and medium priority sub-basins to reach sustainable levels of groundwater pumping and recharge by 2042. SGMA allows local Groundwater Sustainability Agencies the authority to create Groundwater Sustainability Plans at the sub-basin level. To assist California’s Department of Water Resources, this project quantified groundwater change and land subsidence in Central Valley sub-basins with sparse or unreliable well and GPS data. This was done using NASA’s Gravity Recovery and Climate Experiment (GRACE), GRACE Follow-On (GRACE-FO), and interferograms derived from Sentinel-1 C-band Synthetic Aperture Radar (C-SAR) and Advanced Land Observing Satellite 2 (ALOS-2) Phased Array L-band Synthetic Aperture Radar 2 (PALSAR-2). Time series of the GRACE and InSAR data were compared with well and GPS data in data-dense sub-basins to determine the feasibility of these datasets for groundwater storage and subsidence monitoring. We found thatGRACE and InSAR data are effective tools for determining groundwater change and land subsidence and can be used on their own to monitor sub-basins in the absence of well and GPS data.

Water Resources↗

Hawaii Water Resources: Monitoring the Impact of Land-Based Sources of Pollution on Water Quality Along the Coast of West Maui, Hawai'i, to Assess Coral Reef Condition

West Maui is at risk of losing ecosystem services provided by coral reefs due to land-based sources of pollution (LBSP). In 2011, the US Coral Reef Task Force (USCRTF) identified the West Maui watershed as a priority watershed (along with its sub-watersheds of Wahikuli, Honokōwai, Kahana, Honokahua, and Honolua) after decades of coral decline, giving rise to the multi-agency West Maui Ridge to Reef (R2R) Initiative. The DEVELOP Hawai’i Water Resources team partnered with the R2R Initiative and the Hawai’i Department of Land and Natural Resources Division of Aquatic Resources (DLNR-DAR) to address the need for better watershed management practices. The team provided the partners with a Google Earth Engine tool that displays land use and land cover changes (LULCC) in the five watersheds and detects near-shore turbidity, chlorophyll-a (chl-a), and sea surface temperature using Landsat 4 Thematic Mapper (TM), Landsat 5 TM, Landsat 7 Enhanced Thematic Mapper Plus (ETM+), Landsat 8 Operational Land Imager (OLI), Terra Moderate Resolution Imaging Spectroradiometer (MODIS), and Aqua MODIS. Team members used ancillary data provided by the R2R Initiative and the USGS Pacific Coastal and Marine Science Center (PCMSC) to validate satellite parameter values. The land cover analysis captured a general trend of increasing impervious cover and decreasing vegetated cover from 1989 to 2019; however, the extent of this change varied between each watershed. This analysis, coupled with the tool, can help project partners continually monitor terrestrial and marine patterns associated with coral decline.

Water Resources↗

The Isotopic Composition of Molecular Water Formed by Hydrogen Reduction of Iron Oxides: A Proxy for Endogenous Water Formed From Solar Wind Implantation

Many workers have successfully utilized a variety of lunar materials to infer the sources and processing history of volatiles on the Moon. In situ techniques via NanoSIMS have enabled a plethora of hydrogen isotope measurements of isolated grains in regolith and apatite within igneous rocks, revealing an extraordinarily large range of δD values from ~ -900 to +1000‰. The lowest of these δD values are related to the incorporation of solar wind hydrogen, which is pure 1 H. Exposure to solar wind results in structural damage to crystalline phases, forming ubiquitous tens-to-hundreds of nanometer thick amorphous rims on mature regolith grains. Solar wind implantation of H + is also is also thought to result in the formation of nanophase Fe 0 (npFe), a quantitative metric of surface exposure time (e.g., Is/FeO). The formation of npFe can be generally described via the reaction: Fe 2+ O + H 2 = Fe 0 + H 2 O, resulting in the formation of endogenous molecular water reservoirs.

lunar water↗

Statistical characteristics of cloud variability. Part 1: Retrieved cloud liquid water path at three ARM sites: Observed cloud variability at ARM sites

Statistical characteristics of cloud variability are examined for their dependence on averaging scales and best representation of probability density function with the decade-long retrieval products of cloud liquid water path (LWP) from the tropical western Pacific (TWP), Southern Great Plains (SGP), and North Slope of Alaska (NSA) sites of the Department of Energy’s Atmospheric Radiation Measurement Program. The statistical moments of LWP show some seasonal variation at the SGP and NSA sites but not much at the TWP site. It is found that the standard deviation, relative dispersion (the ratio of the standard deviation to the mean), and skewness all quickly increase with the averaging window size when the window size is small and become more or less flat when the window size exceeds 12 h. On average, the cloud LWP at the TWP site has the largest values of standard deviation, relative dispersion, and skewness, whereas the NSA site exhibits the least. Correlation analysis shows that there is a positive correlation between the mean LWP and the standard deviation. The skewness is found to be closely related to the relative dispersion with a correlation coefficient of 0.6. The comparison further shows that the log normal, Weibull, and gamma distributions reasonably explain the observed relationship between skewness and relative dispersion over a wide range of scales.

54 ENVIRONMENTAL SCIENCES↗

Seven years of aerosol scattering hygroscopic growth measurements from SGP: Factors influencing water uptake: Aerosol Scattering Hygroscopic Growth

Long-term measurements of changes in the aerosol scattering coefficient hygroscopic growth at the U.S. Department of Energy Southern Great Plains site provide information on the seasonal as well as size and chemical dependence of aerosol hygroscopic growth. Annual average sub 10 um fRH values (the ratio of aerosol scattering at 85%/40% RH) were 1.75 and 1.87 for the gamma and kappa fit algorithms, respectively. The study found higher growth rates in the winter and spring seasons that correlated with high aerosol nitrate mass fraction. FRH, exhibited strong, but differing correlations with the scattering Ångström exponent and backscatter fraction, two optical size-dependent parameters. The aerosol organic fraction had a strong influence, with fRH decreasing with increases in the organic mass fraction and absorption Ångström exponent and increasing with the aerosol single scatter albedo. Uncertainty analysis if the fit algorithms revealed high uncertainty at low scattering coefficients and slight increases in uncertainty at high RH and fit parameters values.

Jefferson, A.↗

Multiscale model based design of an energy–intensified novel adsorptive reactor process for the water gas shift reaction

In this work, an adsorptive reactor (AR) process is considered that can energetically intensify the water gas shift reaction (WGSR). To best understand AR process behavior, a multiscale, dynamic, process model is developed. This multiscale model enables the quantification of catalyst and adsorbent effectiveness factors within the reactor environment, obliviating the commonly employed assumption that these factors are constant. Simulations of the AR's alternating adsorption-reaction/desorption operation, using the proposed model, illustrate rapid convergence to a long-term periodic solution. The obtained simulation results quantify the influence of key operating conditions and design parameters (e.g., reactor temperature/pressure, W cat /F CO , W ad /F CO , F H2O /F CO ratios, and pellet size) on the AR's behavior. Finally, they also demonstrate, for pellet diameters used at the industrial scale, significant temporal and axial variation of the catalyst/adsorbent pellet effectiveness factors. Finally, the energetic intensification benefits of the proposed AR process over conventional WGSR packed-bed reactors are quantified.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗