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NASA NTRS2004

Relating Satellite-Based Contrail Detection to NWA Output

Contrail-induced cloud cover has been shown to be a significant factor in regional climate change over the United States of America. As air traffic increases, the potential for globally significant impacts also rises. To better understand and predict these potential climatic effects, it is necessary to develop models that can accurately represent contrail properties based on ambient atmospheric variables including temperature, relative humidity and winds. Several high-resolution numerical weather analyses (NWA) including the 20-km Rapid Update Cycle (RUC) and the University of Oklahoma Center for Analysis and Prediction of Storms Advanced Regional Prediction System (ARPS) can provide the temperature, humidity and wind information necessary to diagnose contrail formation. One outstanding problem that must be addressed to achieve a realistic simulation of contrails is the large uncertainties in upper tropospheric relative humidity (UTH) in numerical weather analyses. Current numerical weather analyses tend to underestimate UTH due to large dry biases in the balloon soundings used to construct the analyses. To evaluate each of the models, we match several months of contrail properties derived from satellite and surface observations to the NWA-derived humidity, vertical velocity, wind shear and atmospheric stability. The relationships between several contrail properties (including optical depth and areal contrail coverage) and the NWA-derived statistics will be analyzed to determine under which atmospheric conditions widespread contrail outbreaks are favored.

Duda, David P.↗

NASA NTRS1994

Patterns in the sky: Natural visualization of aircraft flow fields

The objective of the current publication is to present the collection of flight photographs to illustrate the types of flow patterns that were visualized and to present qualitative correlations with computational and wind tunnel results. Initially in section 2, the condensation process is discussed, including a review of relative humidity, vapor pressure, and factors which determine the presence of visible condensate. Next, outputs from computer code calculations are postprocessed by using water-vapor relationships to determine if computed values of relative humidity in the local flow field correlate with the qualitative features of the in-flight condensation patterns. The photographs are then presented in section 3 by flow type and subsequently in section 4 by aircraft type to demonstrate the variety of condensed flow fields that was visualized for a wide range of aircraft and flight maneuvers.

Campbell, James F.↗

NASA NTRS1981

Dependence of tropospheric temperature on the parameterization of cumulus convection in the GLAS model of the general circulation

Analysis of the simulation of seasonal change by the GLAS model of the general circulation reveals deficiencies in the simulation of tropospheric temperature and of convective cloud cover. These interrelated deficiencies are due to a spurious doubling from January to July in the convective cloud cover of the Northern Hemisphere. The spurious doubling, in turn, is due to the oversensitivity of cumulus convection, in the GLAS model, to the specific humidity of the lower atmosphere. The oversensitivity is enhanced by a feedback mechanism which perpetuates the existence of deep, penetrative convective clouds at certain preferred locations. The cumulus parameterization scheme has been modified to more realistically relate the onset of cumulus convection to the relative humidity of the lower atmosphere. The modified parameterization has improved the simulation of tropospheric temperature, planetary albedo and convective cloud cover as well as their seasonal variations. Comparison of this experiment with its control has shown a high degree of interrelation among these fields in the GLAS model and has demonstrated the sensitivity of the atmospheric heat budget to the design of the cumulus parameterization scheme. Also, the modification to the cumulus scheme has demonstrated a plausible mechanism to explain the correlation between convective cloud cover and relative humidity in the real atmosphere.

Helfand, H. M.↗

DOE OSTI2021

Influence of Ions on the Size Dependent Morphology of Aerosol Particles

The study of aerosol particles composed of mixtures of organic and inorganic compounds provides insights for understanding chemistry in the atmosphere as well as information about phase transitions of systems under confinement. In the submicron size regime, we have previously found that liquid-liquid phase separation can be inhibited at sufficiently small particle diameters leading to phase separated particles at larger sizes and homogeneous particles below a threshold diameter. In this paper, we have investigated the influence of cations and anions in the inorganic compound (NH 4 + , Na + , SO 4 2- , HSO 4 - , and Cl-) on the phase separation of submicron aerosol particles. Each of five salts were studied with two different organic compounds. Surprisingly, a strong dependence on the identity of the cation is evident in the size dependence of the particle morphology and no dependence on the anion was found. Sodium containing samples exhibit phase separation in particles below 20 nm in diameter whereas ammonium containing samples cease to undergo phase separation in particles between 45 and 65 nm in diameter. The separation relative humidity for supermicron droplets also depends on the identity of the cation in the inorganic component if the anion is the same across the salts compared. In addition, the correlation between the separation relative humidity and size dependence was investigated and displays a trend, but is not a dominant feature of the data. We explain the results in terms of hard and soft ions, where the harder cation (Na + ) leads to phase separation down to smaller sizes while the softer cation (NH 4 + ) prevents phase separation and causes particles up to a larger diameter to remain homogenous. This study has implications for atmospheric chemistry in regions dominated by sea spray aerosol, which contains sodium as the primary cation, when compared to continental aerosol, where ammonium is an abundant cation. Additionally, these findings can be used to understand the influence of cations on the phase transitions of confined materials.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2021

Estimation of secondary organic aerosol viscosity from explicit modeling of gas-phase oxidation of isoprene and α -pinene

Abstract. Secondary organic aerosols (SOA) are major components of atmospheric fine particulate matter, affecting climate and air quality. Mounting evidence exists that SOA can adopt glassy and viscous semisolid states, impacting formation and partitioning of SOA. In this study, we apply the GECKO-A (Generator of Explicit Chemistry and Kinetics of Organics in the Atmosphere) model to conduct explicit chemical modeling of isoprene photooxidation and α-pinene ozonolysis and their subsequent SOA formation. The detailed gas-phase chemical schemes from GECKO-A are implemented into a box model and coupled to our recently developed glass transition temperature parameterizations, allowing us to predict SOA viscosity. The effects of chemical composition, relative humidity, mass loadings and mass accommodation on particle viscosity are investigated in comparison with measurements of SOA viscosity. The simulated viscosity of isoprene SOA agrees well with viscosity measurements as a function of relative humidity, while the model underestimates viscosity of α-pinene SOA by a few orders of magnitude. This difference may be due to missing processes in the model, including autoxidation and particle-phase reactions, leading to the formation of high-molar-mass compounds that would increase particle viscosity. Additional simulations imply that kinetic limitations of bulk diffusion and reduction in mass accommodation coefficient may play a role in enhancing particle viscosity by suppressing condensation of semi-volatile compounds. The developed model is a useful tool for analysis and investigation of the interplay among gas-phase reactions, particle chemical composition and SOA phase state.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2025

Environmental Controls on Water Vapor Deuterium Excess in the Coastal Boundary Layer: An Information Theory Perspective

We use information theory to quantify the environmental controls on water vapor deuterium excess (D-excess) in coastal Southern California from June 2023 through February 2024. Using Shannon entropy, mutual information (MI), and joint mutual information, metrics that capture both linear and nonlinear relationships, we identify the most informative variables and variable combinations governing D-excess across contrasting marine and continental regimes. Relative humidity with respect to sea surface temperature (RHS) is consistently the strongest individual predictor, explaining up to 27% of D-excess variability during marine conditions but only 10% in continental air masses. The Relative humidity(RHS) + sea surface temperature (SST) combination demonstrates synergistic effects, where their joint influence (explaining up to 36% of D-excess variability) exceeds what either variable achieves individually, confirming their coupled influence on deuterium excess. Wind direction complements RHS most effectively during continental conditions. The best three-variable combination (RHS + SST + Planetary Boundary Layer height) explains 38% of D-excess variability in marine air, while no combination exceeds 20% explanatory power during continental periods. Information theory shows that heteroscedasticity in D-excess relationships indicates regime shifts in controlling processes and quantifies fundamental constraints on predictor variables: some environmental factors like surface pressure or water vapor flux contain insufficient information content to explain D-excess variability regardless of their physical relevance. These results highlight the different predictability limits between marine and continental regimes, challenging the adequacy of linear models and providing a rigorous framework for quantifying the information content of isotope-climate relationships with implications for both modern and paleoclimate applications.

information theory↗

NASA NTRS2000

Operational Assimilation of GOES Data into a Mesoscale Model

A technique has been developed for assimilating GOES-derived skin temperature tendencies and insolation into the surface energy budget equation of a mesoscale model so that the simulated rate of temperature change closely agrees with the satellite observations. A critical assumption of the technique is that the availability of moisture (either from the soil or vegetation) is the least known term in the model's surface energy budget. Therefore, the simulated latent heat flux, which is a function of surface moisture availability, is adjusted based upon differences between the modeled and satellite- observed skin temperature tendencies. An advantage of this technique is that satellite temperature tendencies are assimilated in an energetically consistent manner that avoids energy imbalances and surface stability problems that arise from direct assimilation of surface shelter temperatures. The fact that the rate of change of the satellite skin temperature is used rather than the absolute temperature means that sensor calibration is not as critical. The technique has been employed on a semi-operational basis at the Global Hydrology and Climate Center (GHCC) within the Penn State/National Center for Atmospheric Research (PSU/NCAR) Mesoscale Model (MM5) since 1 November 1998. We performed the assimilation on a model grid centered over the Southeastern US. In addition, a control run without assimilation was performed to provide insight into the performance of the assimilation technique. Bulk verification statistics (BIAS and RMSE) of surface air temperature and relative humidity of more than 250 case days has been performed to date. Results show that assimilation of the satellite data results reduces both the bias and RMSE for simulations of surface air temperature and relative humidity. We are working with forecasters at the National Weather Service Forecast Office located in Birmingham, AL to evaluate the impact of the assimilation on precipitation forecasts. In addition, work is currently underway to determine the ability of both the assimilation technique and Early Eta to sense the significant changes that occur in both leaf expansion and soil moisture conditions during the Spring-Summer of 1999. This will be accomplished via examination of the simulated surface energy budgets from both modeling systems.

Lapenta, William↗

NASA NTRS2005

Nighttime Cirrus Detection using Atmospheric Infrared Sounder Window Channels and Total Column Water Vapor

A method of cirrus detection at nighttime is presented that utilizes 3.8 and 10.4 (micro)m infrared (IR) window brightness temperature differences (dBT) and total column precipitable water (PW) measurements. This technique is applied to the Atmospheric Infrared Sounder (AIRS) and Advanced Microwave Sounding Unit A (AMSU-A) instrument suite on board EOS-Aqua, where dBT is determined from sets of carefully selected AIRS window channels, while PW is derived from the synergistic AIRS and AMSU-A water vapor retrievals. Simulated and observed dBT for a particular value of PW are not constant; several physical factors impact dBT, including the variability in temperature and relative humidity profiles, surface emissivity, instrument noise, and skin/ near-surface air temperature differences. We simulate clear-sky dBT over a realistic range of PWs using 8350 radiosondes that have varying temperature and relative humidity profiles. Thresholds between cloudy and uncertain sky conditions are derived once the scatter in the clear-sky dBT is determined. Simulations of optically thin cirrus indicate that this technique is most sensitive to cirrus optical depth in the 10 (micro)m window of 0.1-0.15 or greater over the tropical and subtropical oceans, where surface emissivity and skin/near-surface air temperature impacts on the IR radiances are minimal. The method at present is generally valid over oceanic regions only, specifically, the tropics and subtropics. The detection of thin cirrus, and other cloud types, is validated using observations at the Atmospheric Radiation Measurement (ARM) program site located at Manus Island in the tropical western Pacific for 89 coincident EOS-Aqua overpasses. Even though the emphasis of this work is on the detection of thin cirrus at nighttime, this technique is sensitive to a broad cloud morphology. The cloud detection technique agrees with ARM-detected clouds 82-84% of the time, which include thin cirrus, as well as other cloud types. Most of the disagreements are well explained by AIRS footprint-scale heterogeneity compared to ARM point measurements, cirrus overlying lower-layer water clouds, possible mixed phase microphysics in midlevel clouds, and significant IR channel noise for cold BT scenes over deep convective towers.

Atmospheric Radiation Measurement (RAM)↗

DOE OSTI2024

Effect of Drying on Corrosion Mitigation of Hanford Transfer Lines

Radioactive waste is stored in underground, carbon-steel double-shell tanks at the Department of Energy Hanford site. The waste is transferred between the tanks and other assets using the transfer lines spanning throughout the various tank farms at Hanford. The transfer lines consist of a pipe-in-pipe design, small diameter pipes, and are not piggable. Recent inspection data of the transfer lines have shown areas with corrosion on both interior of the encasements and exterior of the primary pipes, with nearly 50 percent wall loss on the primary pipes and nearly 25% wall loss on the encasement pipes due to pitting corrosion. The visual inspections of the transfer lines have shown presence of corrosion products near the pipeline risers and beyond. It has been hypothesized that the corrosion is predominantly due to the high humidity conditions and in some cases is driven by the presence of residual hydrotest water in the encasement and the associated contact with the safety significant primary pipe. Therefore, drying of the transfer lines could lead to corrosion mitigation. Experimental studies are being conducted to understand the effect of environmental conditions, especially, relative humidity and temperature, on transfer line grade carbon steel corrosion and on mitigating corrosion. The experimental conditions are selected based on the seasonal temperature changes, and relative humidity conditions ranging from 30 to 100 percent. The experimental data will be used as guidance for maintaining a dry environment that will help mitigate the transfer-line corrosion caused by the high humidity conditions.

Shukla, Pavan K.↗

NASA NTRS1991

Evaluation of cloudiness parameterizations using a cumulus ensemble model

Diagnostic cloudiness parameterizations in large-scale models are evaluated by using a two-dimensional numerical cumulus ensemble model. The model covers a large horizontal domain (512 km) but resolves individual clouds. This study explores the dependence of diagnostic relations (between cloud amount and a large-scale variable) on cloud regime, horizontal averaging distance, and cloud type for tropical convective cloud regimes. Large-scale variables, including relative humidity, cumulus mass flux, large-scale vertical velocity and surface precipitation rate, are examined. It is shown that the total cloud amount can be better estimated as the sum of separate estimates of stratiform and convective cloud amounts using different large-scale variables than by an estimate of the total cloud amount using any single large-scale variable. The stratiform cloud amount can best be estimated by using relative humidity. The convective cloud amount can be diagnosed by using cumulus mass flux. Neither set of diagnostic relations depends significantly on the stimulated cloud regime or horizontal averaging distance, but other diagnostic relations do show some such dependence. These results are interpreted and their implications for cloudiness parameterization are discussed.

Xu, Kuan-Man↗

NASA NTRS1977

Absorption of sound in air - High-frequency measurements

The absorption of sound in air at frequencies from 4 to 100 kHz in 1/12 octave intervals, for temperatures from 255.4 K (0 F) to 310.9 K (100 F) in 5.5 K (10 F) intervals, and at 10% relative-humidity increments between 0% and saturation has been measured. The values of free-field absorption have been analyzed to determine the relaxation frequency of oxygen for each of the 92 combinations of temperature and relative humidity studied and the results are compared to an empirical expression. The relaxation frequencies of oxygen have been analyzed to determine the microscopic energy-transfer rates.

Bass, H. E.↗

NASA NTRSDate not supplied

Airborne High Spectral Resolution Lidar-2 Measurements of Enhanced Depolarization in Marine Aerosols

Airborne NASA Langley Research Center (LaRC) High Spectral Resolution Lidar-2 (HSRL-2) measurements acquired during the recent NASA EVS-3 Aerosol Cloud Meteorology Interactions over the Western Atlantic Experiment (ACTIVATE) revealed enhanced particulate linear depolarization associated with aerosols within the marine boundary layer. These HSRL-2 observations were acquired off the east coast of the United States in February and March 2020 when this lidar was deployed on the NASA LaRC UC-12 aircraft. HSRL-2 measured profiles of aerosol backscattering, extinction,and depolarization at 355 and 532nm and aerosol backscattering and depolarization at 1064nm. Typically HSRL-2 measures low (<5%) linear particulate depolarization associated with marine sea salt aerosols. However, during several ACTIVATE flights, particularly those that occurred with outbreaks of cold, dry air, linear particulate depolarization exceeded 15-20% (532nm) for aerosols within a few hundred meters above the surface. These high values indicated that these particles were nonspherical. Elevated depolarization values were also observed at 355 and 1064 nm. HSRL-2 measured aerosol extinction/backscatter ratio (“lidar ratio”) values around 20-25 sr (355 and 532 nm) that are typically associated with sea salt particles. Coincident measurements of relative humidity from dropsondes released from the UC-12and in situ Diode Laser Hygrometer (DLH) measurements flown on the NASA HU-25 aircraft showed that highest depolarization values of these nonspherical particles were found when the relative humidity (RH)was below 50-60%.These lidar observations of elevated depolarization associated with sea salt aerosol are consistent with previous lidar measurements of sea salt aerosols in dry conditions. We discuss these HSRL-2 measurements also in the context of coincident airborne in situ measurements of particle size and composition acquired on the HU-25 aircraft. We also found that CALIOP satellite measurements observed elevated depolarization during some similar cold air outbreaks. In such cases, the operational CALIOP algorithms attributed the elevated depolarization to nonspherical dust particles rather than the more likely scenario of nonspherical sea salt particles associated with low RH.

aerosols↗

DOE OSTI2021

Impact of solar geoengineering on temperatures over the Indonesian Maritime Continent

Climate change has been projected to increase the intensity and magnitude of extreme temperature in Indonesia. Solar radiation management (SRM) has been proposed as a strategy to temporarily combat global warming, buying time for negative emissions. Though the global impacts of SRM have been extensively studied in recent years, regional impacts, especially in the tropics, have received much less attention. This paper investigates the potential stratospheric sulfate aerosol geoengineering to modify mean and extreme temperature, as well as the relative humidity and wet bulb temperature (WBT) change over Indonesian Maritime Continent (IMC) based on simulations from three different earth system models. We applied statistical downscaling and corrected the bias of model output to reproduce historical temperatures and relative humidity over IMC. We compared SRM as specified by the Geoengineering Model Intercomparison Project (GeoMIP) G4 experiment – 5 Tg of SO 2 into the lower stratosphere between 2020 and 2069 – concurrent with the RCP4.5 emissions scenario. SRM is able to significantly reduce the temperature means and extremes, and although differences in magnitude of response and spatial pattern occur, there is a generally consistent response. Additionally, the spatial response of changes forced by RCP4.5 scenario and SRM impact is notably heterogeneous in the archipelago, highlighting uncertainties that would be critical in assessing socio-economic consequences of both doing, and not doing SRM. In general, SRM has bigger impacts in reducing temperatures over land than oceans, and the southern monsoon region shows more variability. SRM is also effective at reducing the likelihood of WBT > 27OC events compared to RCP4.5 after some years of SRM deployment as well as during the post-termination period of SRM. Regional downscaling may be an effective tool in obtaining policy-relevant information about local effects of different future scenarios involving SRM.

54 ENVIRONMENTAL SCIENCES↗

NASA NTRS1980

The washout of combustion-generated hydrogen chloride

The coefficient for the washout from a rocket exhaust cloud of HCl generated by the combustion of an ammonium perchlorate-based solid rocket propellant such as that to be used for the Space Shuttle Booster is determined. A mathematical model of HCl scavenging by rain is developed taking into account rain droplet size, fall velocity and concentration under various rain conditions, partitioning of exhaust HCl between liquid and gaseous phases, the tendency of HCl to promote water vapor condensation and the concentration and size of droplets within the exhaust cloud. The washout coefficient is calculated as a function of total cloud water content, total HCl content at 100% relative humidity, condensation nuclei concentration and rain intensity. The model predictions are compared with experimental results obtained in scavenging tests with solid rocket exhaust and raindrops of different sizes, and the large reduction in washout coefficient at high relative humidities predicted by the model is not observed. A washout coefficient equal to 0.0000512 times the -0.176 power of the mass concentration of HCl times the 0.773 power of the rainfall intensity is obtained from the experimental data.

Fenton, D. L.↗

NASA NTRS1994

Observation of hydration of single, modified carbon aerosols

We have compared the hydration behavior of single carbon particles that have been treated by exposure to gaseous H2SO4 with that of untreated particles. Untreated carbon particles did not hydrate as the relative humidity varied from 0 to 80% at 23 C. In contrast, treated particles hydrated under subsaturation conditions; mass increases of up to 30% were observed. The mass increase is consistent with sulfuric acid equilibration with the ambient relative humidity in the presence of inert carbon. For the samples studied, the average amount of absorbed acid was 14% +/- 6% by weight, which corresponds to a surface coverage of approximately 0.1 monolayer. The mass fraction of surface-absorbed acid is comparable to the soluble mass fraction observed by Whitefield et al. (1993) in jet aircraft engine aerosols. Estimates indicate this mass fraction corresponds to 0.1% of the available SO2 exiting an aircraft engine ending up as H2SO4 on the carbon aerosol. If this heterogeneous process occurs early enough in the exhaust plume, it may compete with homogeneous nucleation as a mechanism for producing sulfuric acid rich aerosols.

Wyslouzil, B. E.↗

DOE OSTI2021

Effect of Humidity on the Reactive Uptake of Ammonia and Dimethylamine by Nitrogen-Containing Secondary Organic Aerosol

This study investigated the uptake of ammonia (NH3) by secondary organic aerosol (SOA) particles generated via limonene photooxidation or ozonolysis as well as the uptake of dimethylamine (DMA) by limonene ozonolysis, α-cedrene photooxidation, or toluene photooxidation SOA in an environmental chamber between 0–50% relative humidity. In addition to the acid-base equilibrium uptake, NH3 and DMA can react with SOA carbonyl compounds converting them into nitrogen-containing organic compounds (NOCs). The effective reactive uptake coefficients for the formation of NOCs from ammonia were measured on the order of 10−5. The observed DMA reactive uptake coefficients ranged from 10−5 to 10−4. Typically, the reactive uptake coefficient decreased with increasing relative humidity. This is consistent with NOC formation by a condensation reaction between NH3 or DMA with SOA, which produces water as a product. Ammonia is more abundant in the atmosphere than amines. However, the larger observed reactive uptake coefficient suggests that amine uptake may also be a potential source of organic nitrogen in particulate matter.

54 ENVIRONMENTAL SCIENCES↗

NASA NTRS2019

Utilization of Airborne Observations to Assess Model Parametrizations of Critical RH Profiles in the Arctic Ocean

Observational paucity is a reality in the Arctic Ocean. This is especially true for near-surface variables such as temperature, moisture, heat fluxes and BL clouds. As a result, modeling has become one of the major avenues for understanding current and future Arctic trends. Reanalyses are frequently used to force global ocean circulation and sea-ice models. But in northern high latitudes, model integrations and reanalyses are known to have large uncertainties in temperature and humidity profiles, and in boundary layer cloudiness. These are common sources of error in the surface radiative budget terms.An important way to diagnose these biases spatially and temporally is by using satellite remote sensing data. However, remotely-sensed observations also have large uncertainties, especially in near-surface temperature and relative humidity profiles.In situ observational studies are important in bridging our knowledge gap in regions such as the Arctic Ocean. Here, we utilize airborne and ship observations from the ARISE, ACME-IV, and ASCOS campaigns to construct critical relative humidity (RH) profiles over the Beaufort Sea. Such profiles are used as parameterization inputs in the NASA GOES global model to derive the total water condensate in a model grid-box, which determines the cloud fraction. Currently, the critical RH profiles are derived by global AIRS data, relaying mostly on mid-latitude regions, which are not necessarily relevant to the Arctic.We derive campaign-wide mean, standard deviation, and critical RH values, for grid size of 50x50 km and altitude bins between 50 to 400 m, covering both open-ocean and sea-ice covered regions. We compare profiles over open ocean and sea-ice, and look at correlations between the observed critical RH values and water condensate (by cloud number concentration) from observations versus the modeled ones. We then input our calculated values of minimal critical RH values into a set of GEOS single column model (SCM) simulations over the ARISE and ASCOS regions and compare the differences between the predicted values of cloud liquid water path (LWP), ice water path (IWP) and surface fluxes with the observed ones under the range of input parameterizations. Finally, we discuss the implications on surface radiative budget predictions in this region.

Segal-Rozenhaimer, Michal↗

DOE OSTI2023

Membrane Adsorbents Comprising Self-Assembled Inorganic Nanocages (SINCs) for Super-fast Direct Air Capture Enabled by Passive Cooling

The objectives of the proposed project were to develop highly porous membrane adsorbents comprising CO 2 -philic polymers and self-assembled inorganic nanocages (SINCs) for rapid temperature swing adsorption using electricity-free solar heating and radiative cooling, enabling an economically viable approach for direct air capture (DAC). Our core technical activities combine three key innovations. (1) Highly porous flat-sheet membrane adsorbents contain CO 2 -philic amines that can be easily produced using a phase inversion method. (2) CO 2 -philic SINCs can be easily dispersed in the polymers with great stability (compared with the metal-organic frameworks or MOFs). (3) The adsorption and desorption are integrated with solar heating and radiative cooling for rapid continuous operation, in contrast to traditional long-cycle separate operation. The membrane adsorbents containing amines, polymers, and SINCs were produced using a one-step industrial process. The porous membranes coupled with porous SINCs offer low resistance for gas flow and fast CO 2 sorption/desorption cycles, while the incorporation of the additional amine groups provides high CO 2 sorption capacity. The key achievements are summarized below. (1) Membrane adsorbents with high PEI loading (>40%), high porosity of >80%, and low gasflow resistance were prepared in one step using commercially available, low-cost materials. (2) Membrane adsorbents based on Solupor and PEI show CO 2 sorption capacity of >1.5 mmol/g using air containing 400 ppm at a relative humidity of 15%. (3) Effect of the adsorbent compositions (such as PEI type, PEI content, SINC content, porosity) on the CO 2 sorption was systematically investigated. (4) Effect of the processing conditions (such as CO 2 content, temperature, and relative humidity) on the CO 2 sorption was systematically investigated; (5) The stability of the membrane adsorption against many cycles of sorption and desorption was studied. The higher molecular weight of PEI (PEI25k) shows better stability than PEI800. (6) Advanced materials with radiative cooling were developed, which can decrease the temperature by 5-7 °C compared to the ambient temperature. (7) Preliminary techno-economic analysis shows that our process may achieve a capture cost of $1,343/tonne CO 2 with a total OPEX cost of $1,112/tonne CO 2 . The adsorbent replacement cost accounted for 52% of the total OPEX cost. Membrane adsorbents with lower costs and longer operation life can significantly decrease the cost. The proposed project directly addresses the requirement of DE-FOA-0002188, i.e., novel materials with CO 2 adsorption capacity for direct air capture with integrated solar heating and radiative cooling to reduce the cost of the DAC. Our future work will focus on the development of low-cost adsorbents that can be stable at the sorption and desorption conditions for long term.

14 SOLAR ENERGY↗