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DOE OSTI2021

Microfracture-pore structure characterization and water-rock interaction in three lithofacies of the Lower Eagle Ford Formation

The microfracture-pore structures and water-rock interactions of eight samples of three typical lithofacies (three limestone, three wackestone, and two mudstone) from the Lower Eagle Ford Formation have been investigated using an integrated methodology. The methods used were X-ray diffraction (XRD), total organic carbon (TOC) content, pyrolysis, thin-section petrography, scanning electron microscopy (SEM), mercury intrusion porosimetry (MIP), spontaneous water imbibition, and water vapor & nitrogen physisorption. Petrophysical properties such as organic richness, maturity, mineral composition, types and patterns of microfractures and pores, porosity, pore-throat size distribution, pore size distribution, pore connectivity, water adsorption and desorption behavior were determined from these methods, and the results compared among the three lithofacies. For example, the three limestone EAS samples and three wackestone DM samples show a low porosity range from 2.02–3.35%, whereas the two mudstone VRU samples exhibit a much large average porosity of 11.7% by MIP results. Nitrogen physisorption results show that pore size distributions have a good similarity in N2 adsorption volume for the samples with similar lithology. Microfractures are morphologically divided into seven types, with their definitions & pictorial examples presented and possible formation mechanisms proposed. In addition, the water vapor physisorption behavior and their controlling factors are discussed. Here, the water adsorption capacity shows a positive relationship (R 2 = 0.90) with clay content and a negative relationship (R 2 = 0.99) with carbonate content. In general, this integrated study of microfracture-pore structure characterization and water-rock interaction provides some insights of water vapor adsorption behavior in different lithofacies and whether microfractures could be an important pathway for fluid flow.

58 GEOSCIENCES↗

DOE OSTI2023

THE IMPACT OF OXIDATION-INDUCED DEGRADATION ON MATERIALS USED IN HYDROGEN-FIRED MICROTURBINES

Hydrogen-fueled microturbines are being considered as part of the future green microgrid. However, the use of hydrogen as a fuel presents new challenges for selection and development of suitable high temperature materials for hydrogen combustion. The burning of hydrogen is expected to result in higher operating temperatures and higher than typically observed water vapor contents in exhaust gases than after burning natural gas. In the present work, foil specimens of various Fe- and Ni-based alloys were oxidized in air + 10vol.% H2O and air + 60vol.% H2O for up to 5,000 h at 700 °C to simulate the exhaust atmosphere of natural gas and hydrogen-fueled microturbines. The impact of alloy composition and water vapor content on the oxidation/ volatilization induced loss of wall thickness was experimentally evaluated. Enhanced external oxidation and volatilization of Cr¬2O3 and Ti-doped Cr2O3 scales was observed in 60 % H2O compared to 10% H2O. No significant impact of the higher water vapor content was observed on Al2O3 scales formed on Fe-based alumina forming alloys. Lifetime modeling was employed to predict the combined effects of water vapor content, gas flow rates, temperature and alloy composition on the oxidation-induced lifetime of the investigated materials

Romedenne, Marie↗

DOE OSTI2025

Atmospheric River Detection Under Changing Seasonality and Mean-State Climate: ARTMIP Tier 2 Paleoclimate Experiments

Atmospheric rivers (ARs) are filamentary structures within the atmosphere that account for a substantial portion of poleward moisture transport and play an important role in Earth's hydroclimate. However, there is no one quantitative definition for what constitutes an atmospheric river, leading to uncertainty in quantifying how these systems respond to global change. This study seeks to better understand how different AR detection tools (ARDTs) respond to changes in climate states utilizing single-forcing climate model experiments under the aegis of the Atmospheric River Tracking Method Intercomparison Project (ARTMIP). We compare a simulation with an early Holocene orbital configuration and another with CO2 levels of the Last Glacial Maximum to a preindustrial control simulation to test how the ARDTs respond to changes in seasonality and mean climate state, respectively. We find good agreement among the algorithms in the AR response to the changing orbital configuration, with a poleward shift in AR frequency that tracks seasonal poleward shifts in atmospheric water vapor and zonal winds. In the low CO2 simulation, the algorithms generally agree on the sign of AR changes, but there is substantial spread in their magnitude, indicating that mean-state changes lead to larger uncertainty. This disagreement likely arises primarily from differences between algorithms in their thresholds for water vapor and its transport used for identifying ARs. These findings warrant caution in ARDT selection for paleoclimate and climate change studies in which there is a change to the mean climate state, as ARDT selection contributes substantial uncertainty in such cases.

Atmospheric river, paleoclimate↗

DOE OSTI2021

Ground-based temperature and humidity profiling: combining active and passive remote sensors

Abstract. Thermodynamic profiles in the planetary boundary layer (PBL) are important observations for a range of atmospheric research and operational needs. These profiles can be retrieved from passively sensed spectral infrared (IR) or microwave (MW) radiance observations or can be more directly measured by active remote sensors such as water vapor differential absorption lidars (DIALs). This paper explores the synergy of combining ground-based IR, MW, and DIAL observations using an optimal-estimation retrieval framework, quantifying the reduction in the uncertainty in the retrieved profiles and the increase in information content as additional observations are added to IR-only and MW-only retrievals. This study uses ground-based observations collected during the Perdigão field campaign in central Portugal in 2017 and during the DIAL demonstration campaign at the Atmospheric Radiation Measurement Southern Great Plains site in 2017. The results show that the information content in both temperature and water vapor is higher for the IR instrument relative to the MW instrument (thereby resulting in smaller uncertainties) and that the combined IR + MW retrieval is very similar to the IR-only retrieval below 1.5 km. However, including the partial profile of water vapor observed by the DIAL increases the information content in the combined IR + DIAL and MW + DIAL water vapor retrievals substantially, with the exact impact vertically depending on the characteristics of the DIAL instrument itself. Furthermore, there is a slight increase in the information content in the retrieved temperature profile using the IR + DIAL relative to the IR-only; this was not observed in the MW + DIAL retrieval.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2021

The Amazon Water Cycle: Perspectives from Water Budget Closure and Ocean Salinity

Global and regional water cycle includes precipitation, water vapor divergence, and change of column water vapor in the atmosphere, and land surface evapotranspiration, terrestrial water storage change, and river discharge, which is linked to ocean salinity near the river mouth. The water cycle is a crucial component of the Earth system, and numerous studies have addressed its individual components (e.g., precipitation). Here we assess, for the first time, if remote sensing and reanalysis datasets can accurately and self-consistently portray the Amazon water cycle. This is further assisted with satellite ocean salinity measurements near the mouth of the Amazon River. The widely used practice of taking the mean of an ensemble of datasets to represent water cycle components (e.g., precipitation) can produce large biases in water cycle closure. Additionally, closure is achieved with only a small subset of data combinations (e.g., ERA5 precipitation and evapotranspiration plus GRACE satellite terrestrial water storage), which rules out the lower precipitation and higher evapotranspiration estimates, providing valuable constraints on assessments of precipitation, evapotranspiration, and their ratio. The common approach of using the Óbidos stream gauge (located hundreds of kilometers from the river mouth) multiplied by a constant (1.25) to represent the entire Amazon discharge is found to misrepresent the seasonal cycle, and this can affect the apparent influence of Amazon discharge on tropical Atlantic salinity.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2020

COMBLE-Isotopic Links to Atmospheric Water’s Sources (ISLAS) Snow Sampling 2020 Field Campaign Report

Within the European Research Council (ERC)-funded project entitled Isotopic Links to Atmospheric Water’s Sources (ISLAS), researchers from the University of Bergen, Norway, used the stable isotope composition of atmospheric water vapor and precipitation to obtain information about the sources and transport processes of water vapor within arctic weather systems. In particular, during cold-air outbreak conditions, evaporation and precipitation occur in close proximity within the study area. With evaporation studied at a single location (Ny-Ålesund), ISLAS researchers wanted to be able to sample the resulting precipitation at several downstream locations. The U.S. Department of Energy Atmospheric Radiation Measurement (ARM) Cold-Air Outbreaks in the Marine Boundary Layer Experiment (COMBLE) site was one of those locations, included in an entire network of precipitation sampling stations reaching from Ny-Ålesund, where water vapor isotope measurements are conducted near the surface, to Longyearbyen, Tromsø, Andenes, Ålesund, and Bergen. Daily precipitation samples, enhanced by more frequent sampling during intense operational periods (IOPs), were conducted during four weeks from 20 February to 20 March 2020. The contribution from the ARM mobile facility (AMF) observatory, deployed at ANX (Andenes, Norway) during COMBLE, was valuable to understand the spatial coherence of water isotope signals from arctic and extratropical weather systems.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2021

MicroPulse DIAL (MPD) – a diode-laser-based lidar architecture for quantitative atmospheric profiling

Abstract. Continuous water vapor and temperature profiles are critically needed for improved understanding of the lower atmosphere and potential advances in weather forecasting skill. Ground-based, national-scale profiling networks are part of a suite of instruments to provide such observations; however, the technological method must be cost-effective and quantitative. We have been developing an active remote sensing technology based on a diode-laser-based lidar technology to address this observational need. Narrowband, high-spectral-fidelity diode lasers enable accurate and calibration-free measurements requiring a minimal set of assumptions based on direct absorption (Beer–Lambert law) and a ratio of two signals. These well-proven quantitative methods are known as differential absorption lidar (DIAL) and high-spectral-resolution lidar (HSRL). This diode-laser-based architecture, characterized by less powerful laser transmitters than those historically used for atmospheric studies, can be made eye-safe and robust. Nevertheless, it also requires solar background suppression techniques such as narrow-field-of-view receivers with an ultra-narrow bandpass to observe individual photons backscattered from the atmosphere. We discuss this diode-laser-based lidar architecture's latest generation and analyze how it addresses a national-scale profiling network's need to provide continuous thermodynamic observations. The work presented focuses on general architecture changes that pertain to both the water vapor and the temperature profiling capabilities of the MicroPulse DIAL (MPD). However, the specific subcomponent testing and instrument validation presented are for the water vapor measurements only. A fiber-coupled seed laser transmitter optimization is performed and shown to meet all of the requirements for the DIAL technique. Further improvements – such as a fiber-coupled near-range receiver, the ability to perform quality control via automatic receiver scanning, advanced multi-channel scalar capabilities, and advanced processing techniques – are discussed. These new developments increase narrowband DIAL technology readiness and are shown to allow higher-quality water vapor measurements closer to the surface via preliminary intercomparisons within the MPD network itself and with radiosondes.

Spuler, Scott M.↗

DOE OSTI2023

Numerical Study of Coupled Water and Vapor Flow, Heat Transfer, and Solute Transport in Variably-Saturated Deformable Soil During Freeze-Thaw Cycles

As climate change intensifies, soil water flow, heat transfer, and solute transport in the active, unfrozen zones within permafrost and seasonally frozen ground exhibit progressively more complex interactions that are difficult to elucidate with measurements alone. For example, frozen conditions impede water flow and solute transport in soil, while heat and mass transfer are significantly affected by high thermal inertia generated from water-ice phase change during the freeze-thaw cycle. To assist in understanding these subsurface processes, the current study presents a coupled two-dimensional model, which examines heat conduction-convection with water-ice phase change, soil water (liquid water and vapor) and groundwater flow, advective-dispersive solute transport with sorption, and soil deformation (frost heave and thaw settlement) in variably saturated soils subjected to freeze-thaw actions. This coupled multiphysics problem is numerically solved using the finite element method. The model's performance is first verified by comparison to a well-documented freezing test on unsaturated soil in a laboratory environment obtained from the literature. Then based on the proposed model, we quantify the impacts of freeze-thaw cycles on the distribution of temperature, water content, displacement history, and solute concentration in three distinct soil types, including sand, silt and clay textures. The influence of fluctuations in the air temperature, groundwater level, hydraulic conductivity, and solute transport parameters was also comparatively studied. The results show that (a) there is a significant bidirectional exchange between groundwater in the saturated zone and soil water in the vadose zone during freeze-thaw periods, and its magnitude increases with the combined influence of higher hydraulic conductivity and higher capillarity; (b) the rapid dewatering ahead of the freezing front causes local volume shrinkage within the non-frozen region when the freezing front propagates downward during the freezing stage and this volume shrinkage reduces the impact of frost heave due to ice formation. This gradually recovers when the thawed water replenishes the water loss zone during the thawing stage; and (c) the profiles of soil moisture, temperature, displacement, and solute concentration during freeze-thaw cycles are sensitive to the changes in amplitude and freeze-thaw period of the sinusoidal varying air temperature near the ground surface, hydraulic conductivity of soil texture, and the initial groundwater levels. Our modeling framework and simulation results highlight the need to account for coupled thermal-hydraulic-mechanical-chemical behaviors to better understand soil water and groundwater dynamics during freeze-thaw cycles and further help explain the observed changes in water cycles and landscape evolution in cold regions.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2022

Vacuum freezing nucleated liquid water for purifying brackish water

A method of purifying brackish water includes mixing brackish water with a nucleating agent, forming nucleated liquid water and distributing droplets of the nucleated liquid water inside a vacuum chamber, vacuum freezing the droplets of the nucleated liquid water in the vacuum chamber. The method further includes the droplets forming pure water vapor, nucleated ice, and remaining brackish water, mixing and liquifying the pure water vapor and the nucleated ice, forming a mixture of purified liquid water and the nucleating agent. The method further includes separating the mixture of purified liquid water and the nucleating agent, forming purified liquid water and the nucleating agent.

Cao, Fangyu↗

DOE OSTI2024

Integrated experimental studies of pore structure and fluid uptake in the Bossier Shale in eastern Texas, USA

Within the Haynesville-Bossier Shale complex, the Bossier Shale has not been extensively studied by either industry and academia, despite it being an unconventional gas reservoir and a potential caprock for carbon storage in the underlaying Haynesville Shale. The lack of knowledge of the complex pore structures and fluid-rock interactions hinders the effective extraction of gas and the characterization of fluid reservoirs and sealing capacity. Integrated experimental studies of pore structure and fluid-rock interactions were conducted in seven Bossier Shale core samples collected in eastern Texas. Petrographic, geochemical, and petrophysical properties such as mineral composition, organic richness, thermal maturity, porosity, pore/pore throat diameter distribution, water-accessible pores, liquid water imbibition, and water vapor adsorption were characterized using complementary approaches of thin-section petrography, scanning electron microscopy, X-ray diffraction, total organic matter, pyrolysis, mercury intrusion porosimetry, nuclear magnetic resonance, (Ultra-) small angle X-rays scattering as well as small angle neutron scattering with deuterated liquids and contrast variation. Further, the results show that the thermally mature Bossier Shales are composed of mixed argillaceous mudstone, mixed mudstone, and mixed carbonate mudstone. The shale contains both organic and inorganic pores, with porosities of 3.24-9.37 %, pore-to-throat ratios of 1.65 to 19.4, and water-accessible pores accounting for 28.7-72.6 % of total pores. Approaches of liquid water imbibition and water vapor adsorption, with and without direct contact of water with shale samples, indicate that liquid water first enters the nano-sized pores under high capillary pressures, and water vapor adsorption is mainly controlled by both clay minerals and pores with diameters less than 10 nm. These findings contribute to a better understanding of pore structures and water-shale interactions and their controlling factors in the Bossier Shale.

58 GEOSCIENCES↗

DOE OSTI2023

Refractivity Observations from Radar Phase Measurements: The 22 May 2002 Dryline Case during IHOP Project

The dryline, often associated with the development of severe storms in the Southern Great Plains of the United States of America, is a boundary layer phenomenon that occurs when a warm and moist air mass from the Gulf of Mexico meets a hot and dry air mass from the southwest desert area. An accurate knowledge of the water vapor spatio-temporal variability in the lower part of the atmosphere is crucial for a better understanding of the evolution of the dryline. The tropospheric refractivity, directly related to water vapor content, is a proxy for the water vapor content of the troposphere. It has already been demonstrated that the refractivity and the refractivity vertical gradient can be jointly estimated from radar phase measurements. In fact, it has been shown that using kriging interpolation techniques, accurate refractivity maps within the coverage area of the radar can be obtained with high temporal resolution. In this paper, a detailed analysis of the time series of radar-based refractivity maps obtained during a dryline that occurred on the afternoon of 22 May 2002 during the International H 2 O Project is presented. Comparisons between the time series of radar refractivity maps, obtained with the NCAR S-Pol radar, and the refractivity measurements derived from automatic ground-based weather stations and the AERI instrument, placed at different locations within the coverage area of the NCAR S-Pol radar, demonstrate the accuracy of radar refractivity estimates even for highly variable conditions, both in time and space, in the troposphere. Correlation coefficients higher than 0.95 are obtained in all weather station locations. Regarding the RMSE, errors less than 6 N-units are obtained for all cases, being even as low as 2.92 N-units at some locations.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2020

Atomic-Scale Dynamic Interaction of H 2 O Molecules with Cu Surface

Atomic-scale interaction of water vapor with metal surfaces beyond surface adsorption under technologically relevant conditions remains mostly unexplored. Using aberration-corrected environmental transmission electron microscopy, we reveal the dynamic surface activation of Cu by H 2 O at elevated temperature and pressure. In this study, we find a structural transition from flat to corrugated surface for the Cu(011) under low water-vapor pressure. Increasing the water-vapor pressure leads to the surface reaction of Cu with dissociated H 2 O, resulting in the formation of a metastable “bilayer” Cu-O-H phase. Corroborated by density functional theory and ab initio molecular dynamics calculations, the cooperative O and OH interaction with Cu is responsible for the formation and subsurface propagation of this phase.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2024

Cloud response to co-condensation of water and organic vapors over the boreal forest

Abstract. Accounting for the condensation of organic vapors along with water vapor (co-condensation) has been shown in adiabatic cloud parcel model (CPM) simulations to enhance the number of aerosol particles that activate to form cloud droplets. The boreal forest is an important source of biogenic organic vapors, but the role of these vapors in co-condensation has not been systematically investigated. In this work, the environmental conditions under which strong co-condensation-driven cloud droplet number enhancements would be expected over the boreal biome are identified. Recent measurement technology, specifically the Filter Inlet for Gases and AEROsols (FIGAERO) coupled to an iodide-adduct chemical ionization mass spectrometer (I-CIMS), is utilized to construct volatility distributions of the boreal atmospheric organics. Then, a suite of CPM simulations initialized with a comprehensive set of concurrent aerosol observations collected in the boreal forest of Finland during spring 2014 is performed. The degree to which co-condensation impacts droplet formation in the model is shown to be dependent on the initialization of temperature, relative humidity, updraft velocity, aerosol size distribution, organic vapor concentration, and the volatility distribution. The predicted median enhancements in cloud droplet number concentration (CDNC) due to accounting for the co-condensation of water and organics fall on average between 16 % and 22 %. This corresponds to activating particles 10–16 nm smaller in dry diameter that would otherwise remain as interstitial aerosol. The highest CDNC enhancements (ΔCDNC) are predicted in the presence of a nascent ultrafine aerosol mode with a geometric mean diameter of ∼ 40 nm and no clear Hoppel minimum, indicative of pristine environments with a source of ultrafine particles (e.g., via new particle formation processes). Such aerosol size distributions are observed 30 %–40 % of the time in the studied boreal forest environment in spring and fall when new particle formation frequency is the highest. To evaluate the frequencies with which such distributions are experienced by an Earth system model over the whole boreal biome, 5 years of UK Earth System Model (UKESM1) simulations are further used. The frequencies are substantially lower than those observed at the boreal forest measurement site (< 6 % of the time), and the positive values, peaking in spring, are modeled only over Fennoscandia and the western parts of Siberia. Overall, the similarities in the size distributions between observed and modeled (UKESM1) are limited, which would limit the ability of this model, or any model with a similar aerosol representation, to project the climate relevance of co-condensation over the boreal forest. For the critical aerosol size distribution regime, ΔCDNC is shown to be sensitive to the concentrations of semi-volatile and some intermediate-volatility organic compounds (SVOCs and IVOCs), especially when the overall particle surface area is low. The magnitudes of ΔCDNC remain less affected by the more volatile vapors such as formic acid and extremely low- and low-volatility organic compounds (ELVOCs and LVOCs). The reasons for this are that most volatile organic vapors condense inefficiently due to their high volatility below the cloud base, and the concentrations of LVOCs and ELVOCs are too low to gain significant concentrations of soluble mass to reduce the critical supersaturations enough for droplet activation to occur. A reduction in the critical supersaturation caused by organic condensation emerges as the main driver of the modeled ΔCDNC. The results highlight the potential significance of co-condensation in pristine boreal environments close to sources of fresh ultrafine particles. For accurate predictions of co-condensation effects on CDNC, also in larger-scale models, an accurate representation of the aerosol size distribution is critical. Further studies targeted at finding observational evidence and constraints for co-condensation in the field are encouraged.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2024

Data/code for Mlawer et al. 2024 (A more transparent infrared window)

The infrared window region (780–1,250 cm –1 , 12.8 to 8.0 μm) is of great importance to Earth's climate due to its high transparency and thermal energy. We present here a new investigation of the transparency of this spectral region based on observations by interferometers of downwelling surface radiance at two DOE Atmospheric Radiation Measurement program sites. We focus on the dominant source of absorption in this region, the water vapor continuum, and derive updated values of spectral absorption coefficients for both the self and foreign continua. Our results show that the self continuum is too strong in the previous version of Mlawer-Tobin_Clough-Kneizys-Davies (MT_CKD) water vapor continuum model, a result that is consistent with other recent analyses, while the foreign continuum is too weak in MT_CKD. In general, the weaker self continuum derived in this study results in an overall increase in atmospheric transparency in the window, although in atmospheres with low amounts of water vapor the transparency may slightly decrease due to the increase in foreign continuum absorption. These continuum changes lead to a significant decrease in downwelling longwave flux at the surface for moist atmospheres and a modest increase in outgoing longwave radiation. The increased fraction of surface-leaving radiation that escapes to space leads to a notable increase (~5–10%) in climate feedback, implying that climate simulations that use the new infrared window continuum will show somewhat less warming than before. This study also points out the possibly important role that aerosol absorption may play in the longwave radiative budget.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2024

A More Transparent Infrared Window

58 GEOSCIENCES↗

DOE OSTI2023

Moisture-driven CO 2 pump for direct air capture

Direct Air Capture, the chemical separation of carbon dioxide (CO 2 ) from air, is considered a necessary approach to generate negative carbon emissions and in turn limit global warming, though energetic and monetary costs must continue to decline to meet the needed gigaton scale. The promise of energy-efficient and continuous carbon dioxide membrane separation has only recently been investigated with the development of facilitated chemical transport and novel electrochemically driven methods. This work demonstrates the potential for continuous pumping of CO 2 from air using commercial anion exchange membranes driven solely by a water vapor gradient. A reactive transport model that couples ionic transport with moisture sensitive bicarbonate chemistry in charged polymers, also termed moisture swing sorption, was developed alongside experimentally measured equilibrium and transport properties of CO 2 and water vapor in Fumasep FAA-3 to determine the mass transport limits of such a system. The results show that the commercial membrane is kinetically limited by the moisture sensitive chemistry, enabling a CO 2 current of 1.1 μmol/m 2 • s. In diffusion limited materials, a CO 2 pumping flux can reach 11 μmol/m 2 • s in and peak performance is expected with a dry air relative humidity around 50% pumping into a saturated water vapor permeate. In all configurations, water loss becomes the major cost in such a separation and must be managed through optimal polymer design or water recovery mechanisms. The work demonstrates the applicability of a new driving force, the evaporation of water, to meet the energetic demand of CO 2 separation from air.

36 MATERIALS SCIENCE↗

DOE OSTI2023

Climate response to off-equatorial stratospheric sulfur injections in three Earth system models – Part 2: Stratospheric and free-tropospheric response

The paper constitutes Part 2 of a study performing a first systematic inter-model comparison of the atmospheric responses to stratospheric aerosol injection (SAI) at various single latitudes in the tropics, as simulated by three state-of-the-art Earth system models – CESM2-WACCM6, UKESM1.0, and GISS-E2.1-G. Building on Part 1 (Visioni et al., 2023) we demonstrate the role of biases in the climatological circulation and specific aspects of the model microphysics in driving the inter-model differences in the simulated sulfate distributions. We then characterize the simulated changes in stratospheric and free-tropospheric temperatures, ozone, water vapor, and large-scale circulation, elucidating the role of the above aspects in the surface SAI responses discussed in Part 1. We show that the differences in the aerosol spatial distribution can be explained by the significantly faster shallow branches of the Brewer–Dobson circulation in CESM2, a relatively isolated tropical pipe and older tropical age of air in UKESM, and smaller aerosol sizes and relatively stronger horizontal mixing (thus very young stratospheric age of air) in the two GISS versions used. We also find a large spread in the magnitudes of the tropical lower-stratospheric warming amongst the models, driven by microphysical, chemical, and dynamical differences. These lead to large differences in stratospheric water vapor responses, with significant increases in stratospheric water vapor under SAI in CESM2 and GISS that were largely not reproduced in UKESM. For ozone, good agreement was found in the tropical stratosphere amongst the models with more complex microphysics, with lower stratospheric ozone changes consistent with the SAI-induced modulation of the large-scale circulation and the resulting changes in transport. In contrast, we find a large inter-model spread in the Antarctic ozone responses that can largely be explained by the differences in the simulated latitudinal distributions of aerosols as well as the degree of implementation of heterogeneous halogen chemistry on sulfate in the models. The use of GISS runs with bulk microphysics demonstrates the importance of more detailed treatment of aerosol processes, with contrastingly different stratospheric SAI responses to the models using the two-moment aerosol treatment; however, some problems in halogen chemistry in GISS are also identified that require further attention. Overall, our results contribute to an increased understanding of the underlying physical mechanisms as well as identifying and narrowing the uncertainty in model projections of climate impacts from SAI.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2022

Insights into dual-functional modification for water stability enhancement of mesoporous zirconium metal–organic frameworks

The stability of metal–organic frameworks (MOFs) in water affects their ability to function as chemical catalysts, their capacity as adsorbents for separations in water vapor presence, and their usefulness as recyclable water harvesters. Here, we have examined water stability of four node-modified variants of the mesoporous MOF, NU-1000, namely formate-, Acac-, TFacac-, and Facac-NU-1000, comparing these with node-accessible NU-1000. These NU-1000 variants present ligands grafted to NU-1000's hexa-Zr(IV)-oxy nodes by displacing terminal aqua and hydroxo ligands. Facac-NU-1000, containing the most hydrophobic ligands, showed the greatest water stability, being able to undergo at least 20 water adsorption/desorption cycles without loss of water uptake capacity. Computational studies revealed dual salutary functions of installed Facac ligands: (1) enhancement of framework mechanical stability due to electrostatic interactions; and (2) transformation and shielding of the otherwise highly hydrophilic nodes from H-bonding interactions with free water, presumably leading to weaker channel-stressing capillary forces during water evacuation – consistent with trends in free energies of dehydration across the NU-1000 variants. Water harvesting and hydrolysis of chemical warfare agent simulants were examined to gauge the functional consequences of modification and mechanical stabilization of NU-1000 by Facac ligands. The studies revealed a harvesting capacity of ~1.1 L of water vapor per gram of Facac-NU-1000 per sorption cycle. They also revealed retention of catalytic MOF activity following 20 water uptake and release cycles. This study provides insights into the basis for node-ligand-engendered stabilization of wide-channel MOFs against collapse during water removal.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗