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At least 235 records · Page 13
All sourcesNASA NTRSDOE OSTI
NASA NTRS2022

Volcanic Climate Warming through Radiative and Dynamical Feedbacks of SO2 Emissions

Volcanic flood basalt eruptions have been linked to or are contemporaneous with major climate disruptions, ocean anoxic events, and mass extinctions throughout at least the last 400M years of Earth’s history. Previous studies and recent history have shown that volcanically-driven climate cooling can occur through reflection of sunlight by H2SO4 aerosols, while longer-term climate warming can occur via CO2 emissions. We use the Goddard Earth Observing System Chemistry-Climate Model to simulate a four-year duration volcanic SO2 emission of the scale of the Wapshilla Ridge member of the Columbia River Basalt eruption. Brief cooling from H2SO4 aerosols is outweighed by dynamically and radiatively driven warming of the climate through a three orders of magnitude increase in stratospheric H2O vapor.

Scott D Guzewich↗
NASA NTRS2012

Aquarius Main Structure Configuration

The Aquarius/SAC-D Observatory is a joint US-Argentine mission to map the salinity at the ocean surface. This information is critical to improving our understanding of two major components of Earth's climate system - the water cycle and ocean circulation. By measuring ocean salinity from space, the Aquarius/SAC-D Mission will provide new insights into how the massive natural exchange of freshwater between the ocean, atmosphere and sea ice influences ocean circulation, weather and climate. Aquarius is the primary instrument on the SAC-D spacecraft. It consists of a Passive Microwave Radiometer to detect the surface emission that is used to obtain salinity and an Active Scatterometer to measure the ocean waves that affect the precision of the salinity measurement. The Aquarius Primary Structure houses instrument electronics, feed assemblies, and supports a deployable boom with a 2.5 m Reflector, and provides the structural interface to the SAC-D Spacecraft. The key challenge for the Aquarius main structure configuration is to satisfy the needs of component accommodations, ensuring that the instrument can meet all operational, pointing, environmental, and launch vehicle requirements. This paper describes the evolution of the Aquarius main structure configuration, the challenges of balancing the conflicting requirements, and the major configuration driving decisions and compromises.

Eremenko, Alexander↗
NASA NTRS2016

Ice Melt, Sea Level Rise and Superstorms: Evidence from Paleoclimate Data, Climate Modeling, and Modern Observations that 2C Global Warming Could Be Dangerous

We use numerical climate simulations, paleoclimate data, and modern observations to study the effect of growing ice melt from Antarctica and Greenland. Meltwater tends to stabilize the ocean column, inducing amplifying feedbacks that increase subsurface ocean warming and ice shelf melting. Cold meltwater and induced dynamical effects cause ocean surface cooling in the Southern Ocean and North Atlantic, thus increasing Earth's energy imbalance and heat flux into most of the global ocean's surface. Southern Ocean surface cooling, while lower latitudes are warming, increases precipitation on the Southern Ocean, increasing ocean stratification, slowing deepwater formation, and increasing ice sheet mass loss. These feedbacks make ice sheets in contact with the ocean vulnerable to accelerating disintegration. We hypothesize that ice mass loss from the most vulnerable ice, sufficient to raise sea level several meters, is better approximated as exponential than by a more linear response. Doubling times of 10, 20 or 40 years yield multi-meter sea level rise in about 50, 100 or 200 years. Recent ice melt doubling times are near the lower end of the 10-40-year range, but the record is too short to confirm the nature of the response. The feedbacks, including subsurface ocean warming, help explain paleoclimate data and point to a dominant Southern Ocean role in controlling atmospheric CO2, which in turn exercised tight control on global temperature and sea level. The millennial (500-2000-year) timescale of deep-ocean ventilation affects the timescale for natural CO2 change and thus the timescale for paleo-global climate, ice sheet, and sea level changes, but this paleo-millennial timescale should not be misinterpreted as the timescale for ice sheet response to a rapid, large, human-made climate forcing. These climate feedbacks aid interpretation of events late in the prior interglacial, when sea level rose to C6-9m with evidence of extreme storms while Earth was less than 1 C warmer than today. Ice melt cooling of the North Atlantic and Southern oceans increases atmospheric temperature gradients, eddy kinetic energy and baroclinicity, thus driving more powerful storms. The modeling, paleoclimate evidence, and ongoing observations together imply that 2 C global warming above the preindustrial level could be dangerous. Continued high fossil fuel emissions this century are predicted to yield (1) cooling of the Southern Ocean, especially in the Western Hemisphere; (2) slowing of the Southern Ocean overturning circulation, warming of the ice shelves, and growing ice sheet mass loss; (3) slowdown and eventual shutdown of the Atlantic overturning circulation with cooling of the North Atlantic region; (4) increasingly powerful storms; and (5) nonlinearly growing sea level rise, reaching several meters over a timescale of 50-150 years. These predictions, especially the cooling in the Southern Ocean and North Atlantic with markedly reduced warming or even cooling in Europe, differ fundamentally from existing climate change assessments. We discuss observations and modeling studies needed to refute or clarify these assertions.

Computer simulation↗
DOE OSTI2024

Impacts of Sea‐Level Rise on Coastal Groundwater Table Simulated by an Earth System Model With a Land‐Ocean Coupling Scheme

Abstract Sea‐level rise (SLR) poses a severe threat to the coastal environment through seawater intrusion into freshwater aquifers. The rising groundwater table also exacerbates the risk of pluvial, fluvial, and groundwater flooding in coastal regions. However, current Earth system models (ESMs) commonly ignore the exchanges of water at the land‐ocean interface. To address this gap, we developed a novel land‐ocean hydrologic coupling scheme in a state‐of‐the‐science ESM, the Energy Exascale Earth System Model version 2 (E3SMv2). The new scheme includes the lateral exchange between seawater and groundwater and the vertical infiltration of seawater driven by the SLR‐induced inundation. Simulations were performed with the updated E3SMv2 for the global land‐ocean interface to assess the impacts of SLR on coastal groundwater under a high CO 2 emission scenario. By the middle of this century, seawater infiltration on the inundated areas will be the dominant component in the land‐ocean coupling process, while the lateral subsurface flow exchange will be much smaller. The SLR‐induced seawater infiltration will raise the groundwater levels, enhance evapotranspiration, and increase runoff with distinct spatial patterns globally in the future. Although the coupling process is induced by SLR, we found topography and warming temperature have more control on the coupling impacts, probably due to the relatively modest magnitude of SLR during the selected future period. Overall, our study suggests significant groundwater and seawater exchange at the land‐ocean interface, which needs to be considered in ESMs.

54 ENVIRONMENTAL SCIENCES↗
NASA NTRS2023

The Hazard Components of Representative Key Risks. The Physical Climate Perspective

The framework of Representative Key Risks (RKRs) has been adopted by the Intergovernmental Panel on Climate Change Working Group II (WGII) to categorize, assess and communicate a wide range of regional and sectoral key risks from climate change. These are risks expected to become severe due to the potentially detrimental convergence of changing climate conditions with the exposure and vulnerability of human and natural systems. Other papers in this special issue treat each of eight RKRs holistically by assessing their current status and future evolution as a result of this convergence. However, in these papers, such assessment cannot always be organized according to a systematic gradation of climatic changes. Often the big-picture evolution of risk has to be extrapolated from either qualitative effects of “low”, “medium” and “high” warming, or limited/focused analysis of the consequences of particular mitigation choices (e.g., benefits of limiting warming to 1.5 or 2C), together with consideration of the socio-economic context and possible adaptation choices. In this study we offer a representation – as systematic as possible given current literature and assessments – of the future evolution of the hazard components of RKRs. We identify the relevant hazards for each RKR, based upon the WGII authors’ assessment, and we report on their current state and expected future changes in magnitude, intensity and/or frequency, linking these changes to Global Warming Levels (GWLs) to the extent possible. We draw on the assessment of changes in climatic impact-drivers relevant to RKRs described in the 6th Assessment Report by Working Group I supplemented when needed by more recent literature. For some of these quantities - like regional trends in oceanic and atmospheric temperature and precipitation, some heat and precipitation extremes, permafrost thaw and Northern Hemisphere snow cover - a strong and quantitative relationship with increasing GWLs has been identified. For others - like frequency and intensity of tropical cyclones and extra-tropical storms, and fire weather - that link can only be described qualitatively. For some processes - like the behavior of ice sheets, or changes in circulation dynamics - large uncertainties about the effects of different GWLs remain, and for a few others - like ocean pH and air pollution - the composition of the scenario of anthropogenic emissions is most relevant, rather than the warming reached. In almost all cases, however, the basic message remains that every small increment in CO2 concentration in the atmosphere and associated warming will bring changes in climate phenomena that will contribute to increasing risk of impacts on human and natural systems, in the absence of compensating changes in these systems’ exposure and vulnerability, and in the absence of effective adaptation. Our picture of the evolution of RKR-relevant climatic impact-drivers complements and enriches the treatment of RKRs in the other papers in at least two ways: by filling in their often only cursory or limited representation of the physical climate aspects driving impacts, and by providing a fuller representation of their future potential evolution, an important component – if never the only one – of the future evolution of risk severity.

Representative Key Risks↗
DOE OSTI2020

Acidification in the U.S. Southeast: Causes, Potential Consequences and the Role of the Southeast Ocean and Coastal Acidification Network

Coastal acidification in southeastern U.S. estuaries and coastal waters is influenced by biological activity, run-off from the land, and increasing carbon dioxide in the atmosphere. Acidification can negatively impact coastal resources such as shellfish, finfish, and coral reefs, and the communities that rely on them. Organismal responses for species located in the U.S. Southeast document large negative impacts of acidification, especially in larval stages. For example, the toxicity of pesticides increases under acidified conditions and the combination of acidification and low oxygen has profoundly negative influences on genes regulating oxygen consumption. In corals, the rate of calcification decreases with acidification and processes such as wound recovery, reproduction, and recruitment are negatively impacted. Minimizing the changes in global ocean chemistry will ultimately depend on the reduction of carbon dioxide emissions, but adaptation to these changes and mitigation of the local stressors that exacerbate global acidification can be addressed locally. The evolution of our knowledge of acidification, from basic understanding of the problem to the emergence of applied research and monitoring, has been facilitated by the development of regional Coastal Acidification Networks (CANs) across the United States. This synthesis is a product of the Southeast Coastal and Ocean Acidification Network (SOCAN). SOCAN was established to better understand acidification in the coastal waters of the U.S. Southeast and to foster communication among scientists, resource managers, businesses, and governments in the region. Here we review acidification issues in the U.S. Southeast, including the regional mechanisms of acidification and their potential impacts on biological resources and coastal communities. We recommend research and monitoring priorities and discuss the role SOCAN has in advancing acidification research and mitigation of and adaptation to these changes.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2026

Linking international technical specifications for acoustic characterization of marine energy converter sounds with environmental compliance criteria

As new ocean energy technologies emerge and are deployed for testing and operations, sound emissions are a potential concern for environmental effects to marine life. Consistent acoustic measurement and data analysis methods can help promote comparisons of technologies and transferability between project sites. In 2022, acoustic emissions from a prototype scale wave energy converter (WEC) were characterized for a range of environmental conditions and power generation states in the coastal waters off southern California using a set of international technical specifications. Results from the international technical specification analyses were applied to United States regulatory threshold criteria for acoustic impacts to marine mammals and examined in the context of European underwater noise monitoring guidelines. Weighted 24 hour cumulative sound exposure levels SEL24h calculated from the highest power generation state WEC sound pressure levels were often more than 20 dB below threshold criteria for temporary threshold shifts in five relevant marine mammal hearing groups. Following European Union recommendations for analyses and reporting, WEC sound characterization in third octave bands centered at 63 Hz and 125 Hz show clear spatial decay of WEC-generated noise, with more pronounced attenuation at 63 Hz, and a less marked but still detectable gradient at 125 Hz, collectively suggesting a relatively confined acoustic footprint under the observed conditions. The value of the international technical specification approach is highlighted by the isolation of WEC sounds from the surrounding soundscape. This allows for a robust characterization of acoustic emissions through a range of device power generation and sea states. Furthermore, in threshold-based regulatory contexts like the U.S., this facilitates direct evaluation of source contributions, while in broader monitoring frameworks used in the E.U. it provides a reproducible foundation for assessing the contribution of emerging ocean energy technologies to the underwater acoustic environment.

Haxel, Joseph H. (ORCID:0000000273864761)↗
NASA NTRS2016

Health and Climate Impacts of Ocean-Going Vessels in East Asia

East Asia has the most rapidly growing shipping emissions of both CO2 and traditional air pollutants, but the least in-depth analysis. Full evaluation of all pollutants is needed to assess the impacts of shipping emissions. Here, using an advanced method based on detailed dynamic ship activity data, we show that shipping emissions in East Asia accounted for 16% of global shipping CO2 in 2013, compared to only 4-7% in 2002-2005. Increased emissions lead to large adverse health impacts, with 14,500-37,500 premature deaths per year. Global mean radiative forcing from East Asian shipping is initially negative, but would become positive after approximately eight years for constant current emissions. As a large fraction of vessels are registered elsewhere, joint efforts are necessary to reduce emissions and mitigate the climate and health impacts of shipping in the region.

climate change impacts↗
DOE OSTI2024

Modification of CO2/H2O Selectivity of Polymer Through Graphene Coating for Carbon Capture Materials

A harmful issue that needs attention and solution is the rising carbon dioxide (CO2) in our atmosphere. Carbon dioxide in our atmosphere is at an all time high and has continuously increased since the industrial revolution. It has increased tremendously going from 315 parts per million (ppm) in the 1960s up to 419.3 ppm in 2023 as shown in Figure 1. Moreover, CO2 emissions have increased from 11 billion tons/year in the 1960s to 38.6 billion tons/year in 2023. The increase in CO2 found in our atmosphere has a number of detrimental effects such as increase in global temperatures and an increase in the ocean’s acidity. Human activities are greatly involved in the cause of CO2 emissions. At Lawrence Livermore National Lab (LLNL) the Microencapsulated CO2 sorbents (MECS) division has been doing research and investigating formulations for their microcapsules. MECS are core-shell microcapsules consisted of a highly permeable polymer shell and a fluid (sodium carbonate solution) that reacts and absorbs carbon dioxide. An example of the microcapsules are shown in Figure 2. Equation 1 shows the chemical reaction of the fluid (sodium carbonate) contained in the polymer shell that acts as the carbon dioxide sorbent and becomes sodium bicarbonate. The LLNL MECS team is in the process of scaling up their microcapsules for potential applications in “carbon capture from flue gas streams generated by fossil fuel combustion in industrial plants and operations, carbon capture in breweries and soft drink manufacture, carbon capture directly from indoor air to improve its quality”. The microcapsule’s possibility for commercial applications was discovered in 2017.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Biological enhancement of cloud droplet concentrations observed off East Antarctica

Abstract The impact that biogenic emissions have on aerosol-cloud interactions across the Southern Ocean is poorly quantified. Here we use satellite and ship observations during austral summer to study these interactions. We present observational evidence that biogenic aerosols increase cloud condensation nuclei and cloud droplet number concentrations over the Southern Ocean off East Antarctica, coinciding with very low concentrations of ice-nucleating particles and higher occurrences of supercooled liquid-containing low-level clouds.

Mallet, Marc D.↗
DOE OSTI2025

Infrared Thermometer Instrument Handbook

The infrared thermometer (IRT) is a ground-based radiation pyrometer that provides measurements of the brightness temperature of the scene in its field of view. The ground IRT (sometimes referred to as the upwelling instrument) lens has a wide field of view for measuring the radiating temperature of the ground surface. It measures in a narrow range of the infrared band, details of which can be found in Table 2. It provides data to the user averaged to 1-minute resolution. The infrared thermometer for sea-surface temperature (IRTSST) is a ship-based radiation pyrometer that provides measurements of the temperature of the sea surface. The upwelling infrared emission is determined with two different IRTs for over-ocean field campaigns and the data is at 1-second temporal resolution. The IRTs are mounted at heights varying between 2 and 42 m above the ground, oriented so the mounting platform and other human made objects are not in the field of view, and also to ensure that the ground and vegetation cover are representative of the local area. The Heitronics IRT is generally mounted inside a small enclosure, and the Apogee IRT is shielded by a cylindrical enclosure that is part of the design from the manufacturer.

47 OTHER INSTRUMENTATION↗
NASA NTRS1990

Are there interactions of iodine and sulfur species in marine air photochemistry?

The effects of dimethyl sulfide (DMS) and methyl iodide (MI) emissions are analyzed using a two-dimensional photochemical model of a marine tropical tropospheric synoptic system. The model traces the atmospheric transformation cycles of the emissions to aerosols. The study is focused on remote tropical ocean regions and includes simulations of the spatial and diurnal variations of various iodine and sulfur species, and the species OH, HO2, and H2O2. One line of analysis leads to the conclusion that the reaction IO + DMS yields DMSO + I may play a significant role in destroying DMS if it proceeds at the published fast rate. Alternative lines of analyses are presented.

Chatfield, Robert B.↗
NASA NTRS2011

A Proposed Extension to the Soil Moisture and Ocean Salinity Level 2 Algorithm for Mixed Forest and Moderate Vegetation Pixels

The Soil Moisture and Ocean Salinity (SMOS)mission, launched in November 2009, provides global maps of soil moisture and ocean salinity by measuring the L-band (1.4 GHz) emission of the Earth's surface with a spatial resolution of 40-50 km.Uncertainty in the retrieval of soilmoisture over large heterogeneous areas such as SMOS pixels is expected, due to the non-linearity of the relationship between soil moisture and the microwave emission. The current baseline soilmoisture retrieval algorithm adopted by SMOS and implemented in the SMOS Level 2 (SMOS L2) processor partially accounts for the sub-pixel heterogeneity of the land surface, by modelling the individual contributions of different pixel fractions to the overall pixel emission. This retrieval approach is tested in this study using airborne L-band data over an area the size of a SMOS pixel characterised by a mix Eucalypt forest and moderate vegetation types (grassland and crops),with the objective of assessing its ability to correct for the soil moisture retrieval error induced by the land surface heterogeneity. A preliminary analysis using a traditional uniform pixel retrieval approach shows that the sub-pixel heterogeneity of land cover type causes significant errors in soil moisture retrieval (7.7%v/v RMSE, 2%v/v bias) in pixels characterised by a significant amount of forest (40-60%). Although the retrieval approach adopted by SMOS partially reduces this error, it is affected by errors beyond the SMOS target accuracy, presenting in particular a strong dry bias when a fraction of the pixel is occupied by forest (4.1%v/v RMSE,-3.1%v/v bias). An extension to the SMOS approach is proposed that accounts for the heterogeneity of vegetation optical depth within the SMOS pixel. The proposed approach is shown to significantly reduce the error in retrieved soil moisture (2.8%v/v RMSE, -0.3%v/v bias) in pixels characterised by a critical amount of forest (40-60%), at the limited cost of only a crude estimate of the optical depth of the forested area (better than 35% uncertainty). This study makes use of an unprecedented data set of airborne L-band observations and ground supporting data from the National Airborne Field Experiment 2005 (NAFE'05), which allowed accurate characterisation of the land surface heterogeneity over an area equivalent in size to a SMOS pixel.

Panciera, Rocco↗
NASA NTRS2019

Five Decades of Northern Land Carbon Uptake Revealed by the Interhemispheric CO2 Gradient

The global land and ocean carbon sinks have increased proportionally with increasing carbon dioxide emissions during the past decades. It is thought that Northern Hemisphere lands make a dominant contribution to the global land carbon sink; however, the long-term trend of the northern land sink remains uncertain. Here, using measurements of the interhemispheric gradient of atmospheric carbon dioxide from 1958 to 2016, we show that the northern land sink remained stable between the 1960s and the late 1980s, then increased by 0.5 ± 0.4 petagrams of carbon per year during the 1990s and by 0.6 ± 0.5 petagrams of carbon per year during the 2000s. The increase of the northern land sink in the 1990s accounts for 65% of the increase in the global land carbon flux during that period. The subsequent increase in the 2000s is larger than the increase in the global land carbon flux, suggesting a coincident decrease of carbon uptake in the Southern Hemisphere. Comparison of our findings with the simulations of an ensemble of terrestrial carbon models over the same period suggests that the decadal change in the northern land sink between the 1960s and the 1990s can be explained by a combination of increasing concentrations of atmospheric carbon dioxide, climate variability and changes in land cover. However, the increase during the 2000s is underestimated by all models, which suggests the need for improved consideration of changes in drivers such as nitrogen deposition, diffuse light and land-use change. Overall, our findings underscore the importance of Northern Hemispheric land as a carbon sink.

Carbon cycle↗
DOE OSTI2022

Multi-century dynamics of the climate and carbon cycle under both high and net negative emissions scenarios

Abstract. Future climate projections from Earth system models (ESMs) typically focus on the timescale of this century. We use a set of five ESMs and one Earth system model of intermediate complexity (EMIC) to explore the dynamics of the Earth's climate and carbon cycles under contrasting emissions trajectories beyond this century to the year 2300. The trajectories include a very-high-emissions, unmitigated fossil-fuel-driven scenario, as well as a mitigation scenario that diverges from the first scenario after 2040 and features an “overshoot”, followed by a decrease in atmospheric CO2 concentrations by means of large net negative CO2 emissions. In both scenarios and for all models considered here, the terrestrial system switches from being a net sink to either a neutral state or a net source of carbon, though for different reasons and centered in different geographic regions, depending on both the model and the scenario. The ocean carbon system remains a sink, albeit weakened by carbon cycle feedbacks, in all models under the high-emissions scenario and switches from sink to source in the overshoot scenario. The global mean temperature anomaly is generally proportional to cumulative carbon emissions, with a deviation from proportionality in the overshoot scenario that is governed by the zero emissions commitment. Additionally, 23rd century warming continues after the cessation of carbon emissions in several models in the high-emissions scenario and in one model in the overshoot scenario. While ocean carbon cycle responses qualitatively agree in both globally integrated and zonal mean dynamics in both scenarios, the land models qualitatively disagree in zonal mean dynamics, in the relative roles of vegetation and soil in driving C fluxes, in the response of the sink to CO2, and in the timing of the sink–source transition, particularly in the high-emissions scenario. The lack of agreement among land models on the mechanisms and geographic patterns of carbon cycle feedbacks, alongside the potential for lagged physical climate dynamics to cause warming long after CO2 concentrations have stabilized, points to the possibility of surprises in the climate system beyond the 21st century time horizon, even under relatively mitigated global warming scenarios, which should be taken into consideration when setting global climate policy.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2022

A numerical framework for simulating the atmospheric variability of supermicron marine biogenic ice nucleating particles

Abstract. We present a framework for estimating concentrations of episodically elevated high-temperature marine ice nucleating particles (INPs) in the sea surface microlayer and their subsequent emission into the atmospheric boundary layer. These episodic INPs have been observed in multiple ship-based and coastal field campaigns, but the processes controlling their ocean concentrations and transfer to the atmosphere are not yet fully understood. We use a combination of empirical constraints and simulation outputs from an Earth system model to explore different hypotheses for explaining the variability of INP concentrations, and the occurrence of episodic INPs, in the marine atmosphere. In our calculations, we examine the following two proposed oceanic sources of high-temperature INPs: heterotrophic bacteria and marine biopolymer aggregates (MBPAs). Furthermore, we assume that the emission of these INPs is determined by the production of supermicron sea spray aerosol formed from jet drops, with an entrainment probability that is described by Poisson statistics. The concentration of jet drops is derived from the number concentration of supermicron sea spray aerosol calculated from model runs. We then derive the resulting number concentrations of marine high-temperature INPs (at 253 K) in the atmospheric boundary layer and compare their variability to atmospheric observations of INP variability. Specifically, we compare against concentrations of episodically occurring high-temperature INPs observed during field campaigns in the Southern Ocean, the Equatorial Pacific, and the North Atlantic. In this case study, we evaluate our framework at 253 K because reliable observational data at this temperature are available across three different ocean regions, but suitable data are sparse at higher temperatures. We find that heterotrophic bacteria and MBPAs acting as INPs provide only a partial explanation for the observed high INP concentrations. We note, however, that there are still substantial knowledge gaps, particularly concerning the identity of the oceanic INPs contributing most frequently to episodic high-temperature INPs, their specific ice nucleation activity, and the enrichment of their concentrations during the sea–air transfer process. Therefore, targeted measurements investigating the composition of these marine INPs and drivers for their emissions are needed, ideally in combination with modeling studies focused on the potential cloud impacts of these high-temperature INPs.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2020

Investigating Secondary Aerosol Processes in the Amazon through Molecular-level Characterization of Semi-Volatile Organics

In areas where biogenic emissions are oxidized in the presence of anthropogenic pollutants, it has become increasingly apparent that secondary organic aerosol (SOA) formation from biogenic volatile organic compounds (BVOCs) is substantially enhanced. The Amazon forest is the dominant source of BVOCs globally, and the forest is rapidly being converted to urban and agricultural uses. We participated in a collaborative field study located in the Amazon region around Manaus, Brazil, in 2014 (Green Ocean Amazon; GoAmazon). This study was designed to comprehensively examine how BVOC emissions (specifically, the most highly emitted non-methane hydrocarbon, isoprene, and lesser studied sesquiterpenes) and their interaction with anthropogenic pollution (i.e., nitrogen oxides, sulfur dioxide, and black carbon) alter the atmosphere’s oxidative capacity, influence secondary aerosol formation, atmospheric composition and, ultimately, affect the earth’s radiation balance and climate. We provide the first hourly, in-situ measurement of 30 sesquiterpenes and 4 diterpenes, roughly estimating that sesquiterpene oxidation contributes to 10-14% of ozone reactive loss by terpenes and at least 0.4–5% (median 1 %) of total submicron OA mass. However, this is likely a low-end estimate, as evidence for additional unaccounted sesquiterpenes and their oxidation products clearly exists. We also provide new perspectives on sulfate, NO x , and particle acidity influencing isoprene-derived SOA, comparing the central Amazon environment with Southeastern U.S.A. summer, representing clean to polluted conditions, respectively. We find that summed concentrations of isoprene-derived SOA tracers correlated with particulate sulfate spanning three orders of magnitude, suggesting that 1 μg m -3 reduction in sulfate corresponds with at least ~0.5 μg m -3 reduction in isoprene-derived SOA. We also find that SOA mass derived from isoprene oxidation in the presence of NO x is primarily comprised of aerosol sulfate bound with isoprene oxidation products (i.e. organosulfates), ~97% in the Amazon and ~55% in the Southeastern U.S. We infer under natural conditions in high isoprene emission regions, preindustrial aerosol sulfate was almost exclusively isoprene-derived organosulfates, which are traditionally thought as representative of anthropogenic influence. We further report the first field observations showing that particle acidity impacts the distribution of isoprene oxidation tracers in the gas and particle phases, providing physicochemical insight into isoprene SOA formation chemistry. Coupled with other co-located measurements by the DOE Atmospheric Radiation Measurement (ARM) team and collaborating PIs at our measurement site (called T3), on the G1 aircraft, and at additional field sites (T0, T1, T2) this data set has been used to understand emission, oxidation, and particle formation pathways at the molecular level, to elucidate how these pathways change when influenced by anthropogenic sources, and to evaluate their importance for the atmospheric budget of aerosols and the earth’s radiation balance on regional scales. Recommendations: Further constraint of the role of sesquiterpenes on ozone (O 3 ) reactivity and SOA formation is limited by the availability of authentic standards and synthesized compounds of sesquiterpenes and their oxidation products. Future research efforts should focus on making such standards available via custom synthesis to allow for accurate quantification and focused oxidation experiments that will fully elucidate the chemistry of these compounds in the atmosphere. Further, reductions in aerosol sulfate (via SO 2 emissions control) continues to be one of the most effective methods to reduce SOA formation from isoprene, but the concerted role of ammonia (NH 3 ) gas emissions from (agricultural) industry and other sources requires more investigation to better understand the role of aerosol acidity in SOA formation and potential controls. As GoAmazon particles can be more acidic compared to areas with greater anthropogenic NH 3 emissions, this promotes relatively greater organosulfate (OS) formation from isoprene even in the presence of NO x . Because OS and inorganic sulfate differ in water uptake properties, this implies preindustrial aerosol sulfate (albeit less abundant) may have been less reflective than current earth system models assume. Further research should investigate the radiative impacts of organic vs inorganic sulfate in aerosols to improve model representation. Finally, future work (currently underway) should include constraint of the contributions of monoterpene (C 10 H 16 ) BVOCs and biomass burning VOCs as precursors to SOA formation in the region as well as their impacts on radiative forcing in the climate system.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2021

Powering Negative-Emissions Technologies with Marine Renewable Energy

The majority of modeled emissions scenarios that meet the climate change goals outlined in the 2015 Paris Agreement require not only significant reductions in anthropogenic carbon dioxide emissions, but also removal of carbon dioxide from the atmosphere ("negative emissions"). To date, research and development efforts have largely focused on land-based negative emissions technologies, such as bioenergy with carbon capture and storage. However, ocean-based technologies also have significant potential, and avoid competition for land use and fresh water with agriculture and human development. Marine carbon dioxide removal approaches include biological solutions that seek to increase carbon fixation through photosynthesis and chemical solutions that aim to increase the absorption of carbon dioxide in seawater. Most of these approaches have significant power requirements, especially when implemented at the scale necessary to meet negative-emissions goals. Marine renewable energy is uniquely poised to power marine carbon dioxide removal given its ability to provide carbon-free power at sea. In this work, the power requirements of marine carbon dioxide removal systems and the potential of marine renewable energy to power them are investigated, culminating in recommendations for future research and development to enable such developments.

marine renewable energy, carbon dioxide, climate c↗