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At least 361 records · Page 20

Comparative Study of Aerosol and Cloud Detected by CALIPSO and OMI

The Ozone Monitoring Instrument (OMI) on the Aura Satellite detects the presence of desert dust and smoke particles (also known as aerosols) in terms of a parameter known as the UV Aerosol Index (UV AI). The Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observations (CALIPSO) mission measures the vertical distribution of aerosols and clouds. Aerosols and clouds play important roles in the atmosphere and climate system. Accurately detecting their presence, altitude, and properties using satellite radiance measurements is a very important task. This paper presents a comparative analysis of the CALIPSO Version 2 Vertical Feature Mask (VFM) product with the (OMI) UV Aerosol Index (UV AI) and reflectivity datasets for a full year of 2007. The comparison is done at regional and global scales. Based on CALIPSO arid OMI observations, the vertical and horizontal extent of clouds and aerosols are determined and the effects of aerosol type selection, load, cloud fraction on aerosol identification are discussed. It was found that the spatial-temporal correlation found between CALIPSO and OMI observations, is strongly dependent on aerosol types and cloud contamination. CALIPSO is more sensitivity to cloud and often misidentifies desert dust aerosols as cloud, while some small scale aerosol layers as well as some pollution aerosols are unidentified by OMI UV AI. Large differences in aerosol distribution patterns between CALIPSO and OMI are observed, especially for the smoke and pollution aerosol dominated areas. In addition, the results found a significant correlation between CALIPSO lidar 1064 nm backscatter and the OMI UV AI over the study regions.

Chen, Zhong↗

Retrieval of Aerosol Optical Depth Above Clouds from OMI Observations: Sensitivity Analysis, Case Studies

A large fraction of the atmospheric aerosol load reaching the free troposphere is frequently located above low clouds. Most commonly observed aerosols above clouds are carbonaceous particles generally associated with biomass burning and boreal forest fires, and mineral aerosols originated in arid and semi-arid regions and transported across large distances, often above clouds. Because these aerosols absorb solar radiation, their role in the radiative transfer balance of the earth atmosphere system is especially important. The generally negative (cooling) top of the atmosphere direct effect of absorbing aerosols, may turn into warming when the light-absorbing particles are located above clouds. The actual effect depends on the aerosol load and the single scattering albedo, and on the geometric cloud fraction. In spite of its potential significance, the role of aerosols above clouds is not adequately accounted for in the assessment of aerosol radiative forcing effects due to the lack of measurements. In this paper we discuss the basis of a simple technique that uses near-UV observations to simultaneously derive the optical depth of both the aerosol layer and the underlying cloud for overcast conditions. The two-parameter retrieval method described here makes use of the UV aerosol index and reflectance measurements at 388 nm. A detailed sensitivity analysis indicates that the measured radiances depend mainly on the aerosol absorption exponent and aerosol-cloud separation. The technique was applied to above-cloud aerosol events over the Southern Atlantic Ocean yielding realistic results as indicated by indirect evaluation methods. An error analysis indicates that for typical overcast cloudy conditions and aerosol loads, the aerosol optical depth can be retrieved with an accuracy of approximately 54% whereas the cloud optical depth can be derived within 17% of the true value.

Torres, O.↗

Evaluation of the Global Aerosol Microphysical ModelE2-TOMAS Model Against Satellite and Ground-Based Observations

The TwO-Moment Aerosol Sectional (TOMAS) microphysics model has been integrated into the state-of-the- art general circulation model, GISS ModelE2. This paper provides a detailed description of the ModelE2-TOMAS model and evaluates the model against various observations including aerosol precursor gas concentrations, aerosol mass and number concentrations, and aerosol optical depths. Additionally, global budgets in ModelE2-TOMAS are compared with those of other global aerosol models, and the ModelE2-TOMAS model is compared to the default aerosol model in ModelE2, which is a one-moment aerosol (OMA) model (i.e. no aerosol microphysics). Overall, the ModelE2- TOMAS predictions are within the range of other global aerosol model predictions, and the model has a reasonable agreement (mostly within a factor of 2) with observations of sulfur species and other aerosol components as well as aerosol optical depth. However, ModelE2-TOMAS (as well as ModelE2-OMA) cannot capture the observed vertical distribution of sulfur dioxide over the Pacific Ocean, possibly due to overly strong convective transport and over-predicted precipitation. The ModelE2-TOMAS model simulates observed aerosol number concentrations and cloud condensation nuclei concentrations roughly within a factor of 2. Anthropogenic aerosol burdens in ModelE2-OMA differ from ModelE2-TOMAS by a few percent to a factor of 2 regionally, mainly due to differences in aerosol processes including deposition, cloud processing, and emission parameterizations. We observed larger differences for naturally emitted aerosols such as sea salt and mineral dust, as those emission rates are quite different due to different upper size cutoff assumptions.

Lee, Y. H.↗

A13H-2546: Intercomparison of biomass burning aerosol properties from in-situ and remote-sensing instruments in ORACLES-2016

The magnitude of the cumulative effects of aerosols, both directly and on cloud properties, remains the biggest source of uncertainty in our understanding of anthropogenic radiative forcing on the climate. The magnitude of aerosol effects in any given region will depend on not just the aerosol concentration, but also on the characteristics of the aerosol under consideration. The NASA ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) campaign was conducted in 2016-2018 over three deployments in the Southeast Atlantic Ocean (SEA), with the goal of making observations of seasonal biomass burning (BB) smoke plumes overlying persistent stratocumulus cloud decks. During the first ORACLES deployment (September 2016), two NASA aircraft (a P-3 and an ER-2) were flown with a suite of aerosol, cloud, radiation, and meteorological instruments for remote-sensing and in-situ observations. In ORACLES, data collected by eight different instrument teams are used to derive aerosol properties over this region by independent methods. Here we present a comparison of results from the different instrument retrievals with a focus on the measures of aerosol absorption. We focus on specific cases with near-coincident measurements from in-situ (PSAP or PTI for aerosol absorption combined with a nephelometer for aerosol scattering) and remote sensing (4STAR, AirMSPI, RSP, and SSFR) instruments from coordinated flights between the two aircraft. We use the single scattering albedo (SSA), a measure of the relative absorption versus total extinction by aerosols, as the main comparable property between the various remote sensing and in-situ methods. For the remote sensing instruments, we see general good agreement in the total aerosol loading (aerosol optical depth, AOD), though see some differences in the absorbing component (AAOD). We report values for the retrieved aerosol parameters measured in the ORACLES flights and comment upon the observed variability between different instruments. Finally, we discuss these ORACLES results in the context of previous measurements of BB aerosol over the SEA.

Kristina Pistone↗

Uncertainty in Observational Estimates of the Aerosol Direct Radiative Effect and Forcing

Aerosols continue to be responsible for the largest uncertainty in determining the anthropogenic radiative forcing of the climate. To both reconcile the large range in satellite-based estimates of the aerosol direct radiative effect (DRE, the direct interaction with solar radiation by all aerosols) and to optimize the design of future observing systems, we build a framework for assessing uncertainty in aerosol DRE and the aerosol direct radiative forcing (DRF, the radiative effect of just anthropogenic aerosols, RF_ari). Shortwave aerosol radiative kernels (Jacobians) were derived using the MERRA-2 reanalysis data. These radiative kernels are used to compute a lower-bound on the systematic uncertainty in observational estimates of the aerosol DRE/DRF by making the optimistic assumption that global aerosol observations can be made with the accuracy found in the Aerosol Robotic Network (AERONET) sun photometer retrievals. The total uncertainty is shown to be dominated by contributions from the aerosol single scattering albedo uncertainty. These uncertainty estimates were compared to a literature survey of mostly satellite-based aerosol DRE/DRF values. Comparisons to previous studies reveal that most have significantly underestimated the aerosol DRE uncertainty. Past estimates of the aerosol DRF uncertainty are smaller (on average) than our optimistic observational estimates, including the aerosol DRF uncertainty given in the Intergovernmental Panel on Climate Change (IPCC) fifth assessment report (AR5).

Tyler James Thorsen↗

Uncertainty in Observational Estimates of the Aerosol Direct Radiative Effect and Forcing

Aerosols continue to be responsible for the largest uncertainty in determining the anthropogenic radiative forcing of the climate. To both reconcile the large range in satellite-based estimates of the aerosol direct radiative effect (DRE, the direct interaction with solar radiation by all aerosols) and to optimize the design of future observing systems, we build a framework for assessing uncertainty in aerosol DRE and the aerosol direct radiative forcing (DRF, the radiative effect of just anthropogenic aerosols, RF_ari). Shortwave aerosol radiative kernels (Jacobians) were derived using the MERRA-2 reanalysis data. These radiative kernels are used to compute a lower-bound on the systematic uncertainty in observational estimates of the aerosol DRE/DRF by making the optimistic assumption that global aerosol observations can be made with the accuracy found in the Aerosol Robotic Network (AERONET) sun photometer retrievals. The total uncertainty is shown to be dominated by contributions from the aerosol single scattering albedo uncertainty. These uncertainty estimates were compared to a literature survey of mostly satellite-based aerosol DRE/DRF values. Comparisons to previous studies reveal that most have significantly underestimated the aerosol DRE uncertainty. Past estimates of the aerosol DRF uncertainty are smaller (on average) than our optimistic observational estimates, including the aerosol DRF uncertainty given in the Intergovernmental Panel on Climate Change (IPCC) fifth assessment report (AR5).

Tyler James Thorsen↗

Characterization of the aerosol vertical distributions and their impacts on warm clouds based on multi-year ARM observations

Aerosol vertical distribution plays a crucial role in cloud development and thus precipitation since both aerosol indirect and semi-direct effects significantly depend on the relative position of aerosol layer in reference to cloud, but its precise influence on cloud remains unclear. In this study, we integrated multi-year Raman Lidar measurements of aerosol vertical profiles from the U.S. Department of Energy Atmospheric Radiation Measurement (ARM) facility with available Value-Added Products of cloud features to characterize aerosol vertical distributions and their impacts on warm clouds over the continental and marine ARM atmospheric observatories, i.e., Southern Great Plains (SGP) and Eastern North Atlantic (ENA). A unimodal seasonal distribution of aerosol optical depths (AODs) with a peak in summer is found at upper boundary layer over SGP, while a bimodal distribution is observed at ENA for the AODs at lower levels with a major winter-spring maximum. The diurnal mean of upper-level AOD at SGP shows a maximum in the early evening. According to the relative positions of aerosol layers to clouds we further identify three primary types of aerosol vertical distribution, including Random, Decreasing, and Bottom. It is found that the impacts of aerosols on cloud may or may not vary with aerosol vertical distribution depending on environmental conditions, as reflected by the wide variations of the relations between AOD and cloud properties. For example, as AOD increases, the liquid water paths (LWPs) tend to be reduced at SGP but enhanced at ENA. The relations of cloud droplet effective radius with AOD largely depend on aerosol vertical distributions, particularly showing positive values in the Random type under low-LWP condition (<50gm -2 ). In conclusion, the distinct features of aerosol-cloud interactions in relation to aerosol vertical distribution are likely attributed to the continental-marine contrast in thermodynamic environments and aerosol conditions between SGP and ENA.

54 ENVIRONMENTAL SCIENCES↗

Radiative Forcing of Nitrate Aerosols From 1975 to 2010 as Simulated by MOSAIC Module in CESM2-MAM4

In this work, we incorporate the Model for Simulating Aerosol Interactions and Chemistry (MOSAIC) module in the Community Earth System Model version 2 (CESM2) Community Atmosphere Model Version 6 with interactive chemistry (CAM6-chem), and couple it with the four mode version of the Modal Aerosol Module (MAM4). The MOSAIC module is used to simulate the thermodynamics of the gas-aerosol mass exchange, with a special focus on simulating nitrate aerosol. By comparing against ground and satellite observations, we found that the MOSAIC/MAM4 scheme performs reasonably well in simulating spatiotemporal distributions of aerosols, including nitrate aerosol. We conducted a series of model experiments with and without nitrate aerosols, and examined the radiative effect (RE) associated with nitrate aerosols in 1975, 2000, and 2010, and accessed the radiative forcing (RF) of nitrate aerosols between the present day and pre-industrial periods. Comparing with the nitrate aerosol RE, we predicted relatively small RF of anthropogenic nitrate aerosol from aerosol-radiation interactions (RF ari : -0.014 W m -2 ) and large RF from aerosol-cloud interactions (RF aci : -0.219 W m -2 ). Regional signatures of nitrate RE/RF are noticeable and important: for instance, very small changes in RE ari in Europe and USA, but 2.8–3 times increases in RE ari in India and China from 1975 to 2010, while RE aci /RF aci in China is a warming effect due to the competing effect between sulfate and nitrate aerosols as cloud condensation nuclei.

54 ENVIRONMENTAL SCIENCES↗

Aerosols Optical and Radiative Properties in Indonesia Based on AERONET Version 3

Heterogeneity in seasonal aerosol types due to different sources, local characteristics, and meteorology lead to different optical and radiative properties from one place to another. This study analyzes the long-term averages of aerosol optical and radiative properties obtained by the Aerosol Robotic Network (AERONET) version 3 at four sites in Indonesia representing fire prone areas (Palangka Raya, Pontianak, Jambi: 2012–2020), and urban-industrial (Bandung: 2009–2018). We examined the seasonal variation of aerosol optical depth (AOD), Angstrom Exponent (AE), Precipitable Water Vapor (PWV), and Single Scattering Albedo (SSA) combined with meteorological parameters at these Indonesian sites. Multiple clustering techniques from different relationships among various aerosol optical and radiative parameters was employed to further study the aerosol type in respect to different seasonality. The results exhibited a distinct seasonal pattern at all sites except Bandung, whereas AOD increased owing to forest and peat fire outbreaks during the dry season. The trend in AOD annual depicts an increase in Bandung as emission from urban/industrial increases episodically, while it depicts a decrease at the three biomass burning sites. As AOD increased, Palangka Raya, Pontianak, and Jambi exhibited wider ranges of observed AE (1.2–1.8) and high FMF (>0.8) in the dry burning period (June to October). On the other hand, Bandung has more aerosol distribution in the range of FMF values 0.6–1 and AE 1–1.6, compared with other sites, suggesting contribution of complex aerosol emission from different sources and likely due to the formation of secondary aerosol production from trace gases. Palangka Raya, Pontianak, and Jambi exhibited non-absorbing characteristics, as indicated by high SSA (>0.95), high FMF, and high EAE values (1.2–1.7) with no discrepancy in seasonal patterns, implying that biomass burning aerosols in Indonesia tend to cool the atmosphere with strong scattering rather than absorbing. At Bandung, aerosols mixed with slightly absorbing and non-absorbing aerosols owing to urban and industrial emissions. This study lays a foundation for further research on the contribution of aerosol radiative forcing to climate within the complex aerosol and cloud environments in Indonesia.

Aerosol optical depth↗

The Turning Point of the Aerosol Era

Over the CMIP6 historical period (1850–2014), aerosols provided the largest negative forcing compared to all other climate forcings via their ability to absorb or scatter solar radiation and alter clouds. Aerosols played an important role in counterbalancing warming by greenhouse gases (GHGs). Here we study aerosol forcing trends in the CMIP6 simulations of the NASA Goddard Institute for Space Studies (GISS) ocean-atmosphere ModelE version 2.1 (GISS-E2.1-G) using a fully coupled atmospheric composition configuration, including interactive gas-phase chemistry, and either an aerosol microphysical (MATRIX) or a mass-based aerosol (OMA) module. Simulations of the CMIP6 historical period are analyzed as well as four Shared Socioeconomic Pathway (SSP) future scenarios for 2015–2100: SSP1-2.6, SSP2-4.5, SSP3-7.0, and SSP5-8.5. The main conclusion of this study is that aerosol forcing in the GISS model has reached its turning point, switching from globally increasing to a decreasing trend in the first decade of the 21st century. This result is robust, independent of which aerosol module or SSP scenario is used. Non-linear aerosol-cloud interactions dominate as a forcing agent over aerosol-radiation interactions. Aerosols' ability to counterbalance GHG forcing on the global scale is today at a level comparable to that at the beginning of the last century. In the 1980s, the decade of largest global aerosol loads, aerosols balanced up to 80% of GHG forcing. As a consequence, global warming of the last decades, which is primarily driven by greenhouse gases, has been augmented by the effect of decreasing aerosol cooling in our model. By the end of this century, following the SSP scenarios, aerosols will only counterbalance 0%–20% of GHG forcing, depending on model and on scenario.

Aerosol forcing↗

Marine Aerosol to Refinery Emissions: Transport and Evolution of CCN in the Houston Metropolitan Area and Their Impact on Cloud Formation

The Experiment of Sea Breeze Convection, Aerosols, Precipitation and Environment (ESCAPE) campaign aimed to untangle the impacts of contrasting aerosol sources on cloud microphysical properties within deep convective cells using airborne observations with the National Research Council Canada (NRC) Convair CV‐580 research aircraft. Horizontal and vertical gradients of aerosol number size distributions, total aerosol concentrations and cloud condensation nuclei (CCN) spectra were measured in the lower troposphere to quantify the impact of different aerosol sources on aerosol‐cloud interactions. This study focuses on a research flight dedicated to characterizing the aerosol and CCN properties in the Houston Metropolitan region and identifies five main categories of aerosols based on characteristics of aerosol number size distributions, their CCN properties and meteorological conditions. These categories encompassed more than two orders of magnitude differences in aerosol and CCN concentrations, yet their hygroscopic properties remained similar. Aerosol number size distributions and effective hygroscopicity parameters are used to generate continuous CCN spectra to represent the major aerosol types. The different CCN spectra are then incorporated into a 1‐D aerosol‐cloud parcel model using a large range of updrafts selected in the range of those observed during the ESCAPE campaign to assess the impact of the major aerosol sources in Houston on deep convective cloud microphysical properties.

aerosol-cloud interactions↗

Indications of a Decrease in the Depth of Deep Convective Cores with Increasing Aerosol Concentration during the CACTI Campaign

Abstract An aerosol indirect effect on deep convective cores (DCCs), by which increasing aerosol concentration increases cloud-top height via enhanced latent heating and updraft velocity, has been proposed in many studies. However, the magnitude of this effect remains uncertain due to aerosol measurement limitations, modulation of the effect by meteorological conditions, and difficulties untangling meteorological and aerosol effects on DCCs. The Cloud, Aerosol, and Complex Terrain Interactions (CACTI) campaign in 2018–19 produced concentrated aerosol and cloud observations in a location with frequent DCCs, providing an opportunity to examine the proposed aerosol indirect effect on DCC depth in a rigorous and robust manner. For periods throughout the campaign with well-mixed boundary layers, we analyze relationships that exist between aerosol variables (condensation nuclei concentration > 10 nm, 0.4% cloud condensation nuclei concentration, 55–1000-nm aerosol concentration, and aerosol optical depth) and meteorological variables [level of neutral buoyancy (LNB), convective available potential energy, midlevel relative humidity, and deep-layer vertical wind shear] with the maximum radar-echo-top height and cloud-top temperature (CTT) of DCCs. Meteorological variables such as LNB and deep-layer shear are strongly correlated with DCC depth. LNB is also highly correlated with three of the aerosol variables. After accounting for meteorological correlations, increasing values of the aerosol variables [with the exception of one formulation of aerosol optical depth (AOD)] are generally correlated at a statistically significant level with a warmer CTT of DCCs. Therefore, for the study region and period considered, increasing aerosol concentration is mostly associated with a decrease in DCC depth.

54 ENVIRONMENTAL SCIENCES↗

Absorption Properties of Mediterranean Aerosols Obtained from Multi-year Ground-based and Satellite Remote Sensing Observations

Aerosol absorption properties are of high importance to assess aerosol impact on regional climate. This study presents an analysis of aerosol absorption products obtained over the Mediterranean Basin or land stations in the region from multi-year ground-based AERONET and satellite observations with a focus on the Absorbing Aerosol Optical Depth (AAOD), Single Scattering Albedo (SSA) and their spectral dependence. The AAOD and Absorption Angstrom Exponent (AAE) data set is composed of daily averaged AERONET level 2 data from a total of 22 Mediterranean stations having long time series, mainly under the influence of urban-industrial aerosols and/or soil dust. This data set covers the 17 yr period 1996-2012 with most data being from 2003-2011 (approximately 89 percent of level-2 AAOD data). Since AERONET level-2 absorption products require a high aerosol load (AOD at 440 nm greater than 0.4), which is most often related to the presence of desert dust, we also consider level-1.5 SSA data, despite their higher uncertainty, and filter out data with an Angstrom exponent less than 1.0 in order to study absorption by carbonaceous aerosols. The SSA data set includes both AERONET level-2 and satellite level-3 products. Satellite-derived SSA data considered are monthly level 3 products mapped at the regional scale for the spring and summer seasons that exhibit the largest aerosol loads. The satellite SSA dataset includes the following products: (i) Multi-angle Imaging SpectroRadiometer (MISR) over 2000-2011, (ii) Ozone Monitoring Instrument (OMI) near-UV algorithm over 2004-2010, and (iii) MODerate resolution Imaging Spectroradiometer (MODIS) Deep-Blue algorithm over 2005-2011, derived only over land in dusty conditions. Sun-photometer observations show that values of AAOD at 440 nm vary between 0.024 +/- 0.01 (resp. 0.040 +/- 0.01) and 0.050 +/- 0.01 (0.055 +/- 0.01) for urban (dusty) sites. Analysis shows that the Mediterranean urban-industrial aerosols appear "moderately" absorbing with values of SSA close to approximately 0.94-0.95 +/- 0.04 (at 440 nm) in most cases except over the large cities of Rome and Athens, where aerosol appears more absorbing (SSA approximately 0.89-0.90 +/- 0.04). The aerosol Absorption Angstrom Exponent (AAE, estimated using 440 and 870 nm) is found to be larger than 1 for most sites over the Mediterranean, a manifestation of mineral dust (iron) and/or brown carbon producing the observed absorption. AERONET level-2 sun-photometer data indicate the existence of a moderate East-West gradient, with higher values over the eastern basin (AAEEast. = 1.39/AAEWest. = 1.33) due to the influence of desert dust. The North-South AAE gradient is more pronounced, especially over the western basin. Our additional analysis of AERONET level-1.5 data also shows that organic absorbing aerosols significantly affect some Mediterranean sites. These results indicate that current climate models treating organics as nonabsorbing over the Mediterranean certainly underestimate the warming effect due to carbonaceous aerosols. A~comparative analysis of the regional SSA variability has been attempted using satellite data. OMI and MODIS data show an absorbing zone (SSA approximately 0.90 at 470-500 nm) over Northeastern Africa that does not appear in the MISR retrievals. In contrast, MISR seems able to observe the East-West SSA gradient during summer, as also detected by AERONET. Also, the analysis of SSA provided by satellites indicates that the aerosol over the Mediterranean Sea appears less absorbing during spring (MAM) than summer (JJA).

satellite remote sensing observations↗

Utilization of O4 Slant Column Density to Derive Aerosol Layer Height from a Space-Borne UV-Visible Hyperspectral Sensor: Sensitivity and Case Study

The sensitivities of oxygen-dimer (O4) slant column densities (SCDs) to changes in aerosol layer height are investigated using the simulated radiances by a radiative transfer model, the linearized pseudo-spherical vector discrete ordinate radiative transfer (VLIDORT), and the differential optical absorption spectroscopy (DOAS) technique. The sensitivities of the O4 index (O4I), which is defined as dividing O4 SCD by 10(sup 40) molecules (sup 2) per centimeters(sup -5), to aerosol types and optical properties are also evaluated and compared. Among the O4 absorption bands at 340, 360, 380, and 477 nanometers, the O4 absorption band at 477 nanometers is found to be the most suitable to retrieve the aerosol effective height. However, the O4I at 477 nanometers is significantly influenced not only by the aerosol layer effective height but also by aerosol vertical profiles, optical properties including single scattering albedo (SSA), aerosol optical depth (AOD), particle size, and surface albedo. Overall, the error of the retrieved aerosol effective height is estimated to be 1276, 846, and 739 meters for dust, non-absorbing, and absorbing aerosol, respectively, assuming knowledge on the aerosol vertical distribution shape. Using radiance data from the Ozone Monitoring Instrument (OMI), a new algorithm is developed to derive the aerosol effective height over East Asia after the determination of the aerosol type and AOD from the MODerate resolution Imaging Spectroradiometer (MODIS). About 80 percent of retrieved aerosol effective heights are within the error range of 1 kilometer compared to those obtained from the Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) measurements on thick aerosol layer cases.

Air Pollution↗

A51F-0123: Model Analysis of Tropospheric Aerosol Variability and Sources over the North Atlantic During NAAMES 2015-2016

The North Atlantic Aerosols and Marine Ecosystems Study (NAAMES) is a five-year Earth-Venture Suborbital-2 Mission to characterize the plankton ecosystems and their influences on remote marine aerosols, boundary layer clouds, and their implications for climate in the North Atlantic. While marine-sourced aerosols have been shown to make important contributions to surface aerosol loading, cloud condensation nuclei and ice nuclei concentrations over remote marine and coastal regions, it is still a challenge to differentiate the marine biogenic aerosol signal from the strong influence of continental pollution outflow. We examine here the spatiotemporal variability and quantify the sources of tropospheric aerosols over the North Atlantic during the first two phases (November 2015 and May-June 2016) of NAAMES using a state-of-the-art chemical transport model (GEOS-Chem). The model is driven by the Modern-Era Retrospective analysis for Research and Applications, Version 2 (MERRA-2) from the NASA Global Modeling and Assimilation Office (GMAO). It includes sulfate-nitrate-ammonium aerosol thermodynamics coupled to ozone-NOx-hydrocarbon-aerosol chemistry, mineral dust, sea salt, elemental and organic carbon aerosols, and especially a recently implemented parameterization for the marine primary organic aerosol emission. The simulated aerosols over the North Atlantic are evaluated with available satellite (e.g., MODIS) observations of aerosol optical depths (AOD), and aircraft and ship aerosol measurements. We diagnose transport pathways for continental pollution outflow over the North Atlantic using carbon monoxide, an excellent tracer for anthropogenic pollution transport. We also conduct model perturbation experiments to quantify the relative contributions of terrestrial and oceanic sources to the aerosol loading, AOD, and their variability over the North Atlantic.

aerosols↗

Distribution and Sources of Tropospheric Aerosols Over the Western North Atlantic During ACTIVATE (February-March 2020)

The Aerosol Cloud meTeorology Interactions oVer the western ATlantic Experiment (ACTIVATE) is a five-year (2019-2023) NASA Earth-Venture Suborbital-3 (EVS-3) mission to robustly characterize aerosol-cloud-meteorology interactions during February-June, with a focus on marine boundary layer clouds. This characterization requires understanding of aerosol composition, distribution, transport pathways, and sources. Here we use the GEOS-Chem chemical transport model driven by the MERRA-2 reanalysis to simulate tropospheric carbon monoxide (CO) and aerosols over the western North Atlantic Ocean (WNAO) during the first field deployment of ACTIVATE (February-March 2020). CO is used as a tracer to diagnose transport pathways for continental pollution outflow to the WNAO. The aerosol simulation represents all major aerosols including sulfate-nitrate-ammonium (SNA), mineral dust, sea salt, black and organic carbon aerosols. Model-simulated mixing ratios of SNA and organic carbon are compared with aircraft observations. We show that intensive aerosol mass measurements in the lower troposphere over the North American outflow region during ACTIVATE provide strong constraints on model aerosol wet scavenging. Comparisons of model aerosol extinctions with the airborne High Spectral Resolution Lidar-2 (HSRL-2) measurements indicate that the model generally captures continental outflow of aerosols and enhanced extinctions associated with sea salt. Simulated aerosol optical depths (AODs) and extinction vertical profiles are also compared with satellite retrievals from MODIS/Aqua and CALIOP/CALIPSO, respectively. CALIOP sometimes observes enhanced aerosol extinction at altitudes between ~1.5km and ~2.0km south of 32°N. The model reproduces this enhancement and attributes it to coarse-mode sea salt associated with high relative humidity. The relative contributions of continental and oceanic sources to the aerosol loading, AOD, and their distributions over the study domain will also be discussed.

aerosols↗

Subtask 2.6 – Optimization of Aerosol Mitigation Technology for Postcombustion CO 2 Capture

Growing concerns over the impact of CO 2 emissions from combustion sources on global climate change have prompted numerous research and development projects aimed at developing cost-effective technologies for CO 2 capture. One family of technologies being demonstrated at pilot and full scale globally is postcombustion CO 2 capture (PCCC) systems that employ amine-based solvents. The captured CO 2 can be compressed and permanently stored underground or used for enhanced oil recovery (EOR). The proximity of North Dakota’s lignite-fired fleet of power plants to potential CO 2 storage options creates a unique atmosphere for PCCC within the state. However, the aerosols present in lignite flue gas present a challenge for large-scale PCCC at North Dakota power plants. Aerosols can negatively impact the long-term performance of amine-based solvents for CO 2 capture. Amine-based solvents are volatile, and aerosols provide nucleation sites where amine vapors can condense. Because aerosols cannot be easily captured at the column outlet using conventional technologies, the amine-laden aerosols escape the system and lead to accelerated solvent losses. Moreover, aerosol components can chemically react with amines to form degradation products that can permanently deactivate the amine, cause fouling, and lead to hazardous emissions. Many of the elements that have been shown to catalyze solvent degradation are present in lignite coals and can exacerbate solvent replacement economics. Understanding this issue is critical to the implementation of solvent-based CO 2 capture systems as applied to lignite-fired generation systems. The Energy & Environmental Research Center (EERC) designed and carried out this project to optimize aerosol mitigation technology for PCCC at a lignite-fired power plant. To meet the goal of this project, the following objectives were identified: Determine the effectiveness of a wet electrostatic precipitator (WESP) on collection of aerosols at a low-rank coal-fired power station. Determine the impact of aerosols on the efficiency and degradation products of amine-based carbon capture systems fired with low-rank fuels. Work was conducted at Minnkota Power Cooperative’s (MPC’s) Milton R. Young (MRY) Station Unit 2 using a slipstream of flue gas from the outlet of the plant’s flue gas desulfurization (FGD) unit. To gather initial data for sizing and specifying a WESP for this system, a temporary pilot-scale WESP was rented and installed on-site. Several different conditions were tested to examine the impact of flow rate, voltage, and current on WESP performance. The WESP was effective at removing large particulate (>200 nm) but caused an increase in fine particulate (<75 nm). Fine particulate material at the inlet and outlet of the WESP was collected, analyzed, and showed that crystalline sulfates carried over from the plant’s FGD unit were being converted to fine aerosols and SO 2 was being converted to SO 3 through the WESP. Additionally, the high moisture content of the flue gas stream at this sample location also contributed to an overall increase in aerosol mass under some of the test conditions. Using the results from the rented WESP, the project team installed a smaller-scale WESP upstream of the EERC’s slipstream CO 2 capture system. Flue gas was routed through a pilot-scale FGD unit to remove SO 2 to very low levels (~1 ppm) and then through a direct contact cooler (DCC) to further cool the gas and to remove moisture. The gas exiting the DCC was then routed through the new WESP before passing to the CO 2 absorber columns. Fluor’s amine-based solvent was used to scrub CO 2 from the slipstream through a set of two absorber columns. The rich solvent was regenerated in a stripper column by heating to drive off captured CO 2 . The system operated using a catch-and-release method where the CO 2 was separated to provide data on the process, but the captured CO 2 was released back into the host site stack. Aerosols and sulfur species were measured at multiple locations throughout the pilot-scale system. The inlet FGD and DCC removed much of the particulate matter and gaseous sulfur upstream of the WESP. With this configuration, the WESP achieved >95% particulate capture. The new WESP did not show any of the increases in SO 3 or other aerosol species that had been consistently observed with the larger-scale WESP installed immediately downstream of the plant’s full-scale FGD unit. Particulate samples captured and analyzed from the WESP inlet did not show any presence of crystalline sulfate materials, indicating that the pilot-scale FGD and DCC were efficient at reducing carryover from the plant’s full-scale FGD unit. A set of parametric tests were conducted on the new WESP to assess the impacts of flow rate, voltage, number of online WESP fields, and gas-phase sulfur content on aerosol and sulfur transformations. The results showed that the WESP performed similarly well at all sets of conditions. Sulfur and particulate matter exiting the WESP were further reduced through the absorber column as the amine-based solvent captured some of the residual contaminants. Solvent analysis showed that these species were slowly concentrating in the solvent over the duration of the test. When the WESP was taken offline and the sulfur slip through the FGD allowed to rise, the sulfate content in the solvent rose sharply, showing that the extra FGD and WESP were effective at reducing sulfate and cation uptake. This would be expected to extend amine-based solvent life by slowing the formation of heat-stable salts and other degradation products. This subtask was cofunded through the EERC–U.S. Department of Energy Joint Program on Research and Development for Fossil Energy-Related Resources Cooperative Agreement No. DE-FE0024233. Nonfederal funding was provided by the North Dakota Industrial Commission and MPC.

01 COAL, LIGNITE, AND PEAT↗

Final Report on Aerosol Pretreatment Technology Performance and Benchmarking

Solvent-based post-combustion CO 2 capture (PCC) technology remains one of the leading methods to combat global CO 2 emissions produced from large-scale coal-fired power production. Advanced solventbased PCC technology has made significant improvements in design and performance that reduce capital and operating costs to enable its commercial use. Key to low cost, manageable logistics, and environmentally safe operation of solvent-based PCC technology are minimal solvent losses from the process through the treated gas stream exiting PCC plant absorbers. High flue gas aerosol particle concentrations (>10 5 particles/cm 3 ) for particles in the range of 70-200 nm have been shown to cause significant amine solvent losses for solvent-based PCC processes through several mechanisms including absorption of solvent and water into growing aerosol particles. Flue gas aerosol pretreatment technology is the only realistic and economically attractive method to reduce very high aerosol particle concentrations (>10 7 particles/cm 3 ) to enable solvent-based PCC for existing power plants lacking sufficient particle removal systems, such as baghouses. The overall goal of this project was to design, construct, independently test, and evaluate three flue gas aerosol pretreatment technologies identified to significantly reduce high aerosol particle concentrations (>10 7 particles/cm 3 ) in the 70-200 nm particle size range: (1) a novel, high-velocity water injection spray concept developed by RWE and tested by Linde, (2) an innovative electrostatic precipitator (ESP) device with optimized operating conditions developed by Washington University in St. Louis (WUSTL), and (3) a non-regenerative sorbent-based filter technology developed by InnoSepra for SO x and NO x removal from coal-fired power plant flue gas. Each technology has been validated with tests on 500-1000 scfm of actual coal-fired flue gas and evaluated in terms of particle removal efficiency (%), cost competitiveness, and environmental impact. Aerosol measurements were performed upstream and downstream of each aerosol reduction unit during independent testing of each technology using advanced instrumentation and analytical methods provided by WUSTL. To perform aerosol measurements, isokinetic probes were inserted into flanged pipes attached to the flue gas piping, and a small suction pump was used to sample gas containing aerosol particles. Aerosol particle number concentrations (# particles/cm 3 ) and size distributions were then measured using a scanning mobility particle sizer (SMPS, TSI Inc.) for very fine particles (<1,000 nm) and a particle counter manufactured by GRIMM for particles larger than 1,000 nm. This report summarizes the aerosol removal performance results from pilot scale testing of each technology. Performance results have been benchmarked against pre-defined targets and other flue gas aerosol pretreatment technologies with documented performance. Linde Gas North America LLC has been the prime contractor to DOE responsible for overall project management and provided the design for the high-velocity water spray-based aerosol removal technology based on a design concept developed by the German utility company RWE.

20 FOSSIL-FUELED POWER PLANTS↗