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At least 19 records

Global Impacts of Marine Methanethiol Emissions and Chemistry in the Atmosphere

Oceanic emissions of dimethyl sulfide (DMS) have long been known to influence aerosol particle composition, cloud condensation nuclei (CCN) concentration, and Earth’s radiative budget. However, the impact of oceanic emissions of methanethiol (MeSH), a sulfur compound produced by the same oceanic precursor as DMS, has been relatively less explored. The gas-phase oxidation of MeSH has a higher effective yield of SO 2 and a shorter oxidative lifetime compared to DMS, highlighting the relevance of this pathway for the modeled representation of particle formation, growth, and CCN abundance in the marine atmosphere. Here, we use the global chemical transport model GEOS-Chem to explore possible scenarios representative of specific environmental conditions and MeSH emission schemes based on previous experimental studies. We further implement and test previously reported chemical mechanisms for MeSH oxidation, along with additional improvements, highlighting key uncertainties and sensitivities for regional and global sulfur budgets. We place our results in the context of recent modeling updates to DMS chemistry and cloud processing, which further impact SO 2 production in the marine atmosphere in parallel with MeSH oxidation. Within the overall marine sulfur budget, our findings highlight that MeSH plays a significant role in SO 2 production in the marine atmosphere, contributing to regional surface layer concentration increases of up to 40–60%. These results point to the importance of MeSH for efforts aimed at improving the modeled representation of sulfur spatiotemporal patterns relevant to air quality predictions and climate impact assessments.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Characterizing Ocean Acidification and Atmospheric Emission caused by Methane Released from Gas Hydrate Systems along the US Atlantic Margin (Final Report)

To assess the environmental impact of decomposing gas hydrates, this project characterized the atmospheric emission and ocean acidification associated with seafloor-released methane along the U.S. Atlantic Margin. This project leveraged the newly discovered seafloor seeps in this region, many of which are located near the landward limit of gas hydrate stability, to investigate the fate and environmental impact of methane once released from the seafloor. Several research directions were pursued during these investigations. First, high-spatial resolution surface surveys were conducted to characterize the degree to which sea-to-air emission of methane is correlated with acoustically detected seafloor bubble emissions. Second, the natural isotopic signatures of both radiocarbon and δ 13 C were measured throughout the water column to observe if seafloor-released methane was detected in surface waters or if it was replaced by a different source. Third, the extent of methane oxidation in the water column was constrained to assess the ability of this process to mitigate atmospheric methane emissions. Fourth, since aerobic methane oxidation ultimately converts methane to carbon dioxide, the extent of ocean acidification relating to this process was assessed. Ultimately, this project was conducted in four stages. Stage one involved preparations for the research expedition along the U.S. Atlantic Margin. This involved calibrating, modifying, and validating equipment needed for sample and data collection in this unique environment. Stage two involved executing the at-sea science. This research was conducted from 25 August to 5 September 2017 on the R/V Hugh R. Sharp. This expedition left from Lewes, Delaware and investigated the continental slope from approximately this latitude down to Cape Hatteras, North Carolina. Third, any samples unanalyzed on the research vessel were returned to the laboratory and measured. Fourth, the data were interpreted, and publications and presentations were prepared.

03 NATURAL GAS↗

Benchmark estimate of the effect of anthropogenic emissions on the ocean surface

Abstract Investigations into the role of anthropogenic emissions in the occurrence of extreme weather often use a method that compares simulations of atmospheric climate models run under a factual scenario of historical boundary conditions observed during the period of the event against simulations run under a counterfactual scenario of what those boundary conditions might naturally have been over that same period in the absence of anthropogenic emissions. A particular requirement for this experiment design is an accurate estimation of ocean surface boundary conditions for use by the counterfactual natural simulations. Here we use output from the CMIP5 multi‐climate‐model archive to develop a robust estimate of sea surface temperatures and sea ice conditions for use in counterfactual natural simulations, intended as a benchmark estimate to facilitate comparison across climate models and across studies. This development includes tests to ensure that the final estimate is stable from year‐to‐year and stable against other perturbations to the methodology, as well as consideration of the strengths and weaknesses in comparison to other available attributable warming estimates. While this estimate is tailored specifically for the International CLIVAR C20C+ Detection and Attribution Project, it can be used by related projects as well.

Stone, Dáithí A.↗

Are Terrestrial Biosphere Models Fit for Simulating the Global Land Carbon Sink?

The Global Carbon Project estimates that the terrestrial biosphere has absorbed about one-third of anthropogenic CO 2 emissions during the 1959–2019 period. This sink-estimate is produced by an ensemble of terrestrial biosphere models and is consistent with the land uptake inferred from the residual of emissions and ocean uptake. The purpose of our study is to understand how well terrestrial biosphere models reproduce the processes that drive the terrestrial carbon sink. One challenge is to decide what level of agreement between model output and observation-based reference data is adequate considering that reference data are prone to uncertainties. To define such a level of agreement, we compute benchmark scores that quantify the similarity between independently derived reference data sets using multiple statistical metrics. Models are considered to perform well if their model scores reach benchmark scores. Our results show that reference data can differ considerably, causing benchmark scores to be low. Model scores are often of similar magnitude as benchmark scores, implying that model performance is reasonable given how different reference data are. While model performance is encouraging, ample potential for improvements remains, including a reduction in a positive leaf area index bias, improved representations of processes that govern soil organic carbon in high latitudes, and an assessment of causes that drive the inter-model spread of gross primary productivity in boreal regions and humid tropics. The success of future model development will increasingly depend on our capacity to reduce and account for observational uncertainties.

58 GEOSCIENCES↗

Electrochemical carbon dioxide capture to close the carbon cycle

Electrochemical CO 2 capture technologies are gaining attention due to their flexibility, their ability to address decentralized emissions (e.g., ocean and atmosphere) and their fit in an electrified industry. In the present work, recent progress made in electrochemical CO 2 capture is reviewed. The majority of these methods rely on the concept of “pH-swing” and the effect it has on the CO 2 hydration/dehydration equilibrium. Through a pH-swing, CO 2 can be captured and recovered by shifting the pH of a working fluid between acidic and basic pH. Such swing can be applied electrochemically through electrolysis, bipolar membrane electrodialysis, reversible redox reactions and capacitive deionization. In this review, we summarize main parameters governing these electrochemical pH-swing processes and put the concept in the framework of available worldwide capture technologies. We analyse the energy efficiency and consumption of such systems, and provide recommendations for further improvements. Although electrochemical CO 2 capture technologies are rather costly compared to the amine based capture, they can be particularly interesting if more affordable renewable electricity and materials (e.g., electrode and membranes) become widely available. Furthermore, electrochemical methods have the ability to (directly) convert the captured CO 2 to value added chemicals and fuels, and hence prepare for a fully electrified circular carbon economy.

54 ENVIRONMENTAL SCIENCES↗

Long-range transported continental aerosol in the eastern North Atlantic: three multiday event regimes influence cloud condensation nuclei

Abstract. The eastern North Atlantic (ENA) is a region dominated by pristine marine environment and subtropical marine boundary layer clouds. Under unperturbed atmospheric conditions, the regional aerosol regime in the ENA varies seasonally due to different seasonal surface-ocean biogenic emissions, removal processes, and meteorological regimes. However, during periods when the marine boundary layer aerosol in the ENA is impacted by particles transported from continental sources, aerosol properties within the marine boundary layer change significantly, affecting the concentration of cloud condensation nuclei (CCN). Here, we investigate the impact of long-range transported continental aerosol on the regional aerosol regime in the ENA using data collected at the U.S. Department of Energy's (DOE) Atmospheric Radiation Measurement (ARM) user facility on Graciosa Island in 2017 during the Aerosol and Cloud Experiments in the Eastern North Atlantic (ACE-ENA) campaign. We develop an algorithm that integrates number concentrations of particles with optical particle dry diameter (Dp) between 100 and 1000 nm, single scattering albedo, and black carbon concentration to identify multiday events (with duration >24 consecutive hours) of long-range continental aerosol transport in the ENA. In 2017, we detected nine multiday events of long-range transported particles that correspond to ∼ 7.5 % of the year. For each event, we perform HYSPLIT 10 d backward trajectories analysis, and we evaluate CALIPSO aerosol products to assess, respectively, the origins and compositions of aerosol particles arriving at the ENA site. Subsequently, we group the events into three categories, (1) mixture of dust and marine aerosols, (2) mixture of marine and polluted continental aerosols from industrialized areas, and (3) biomass burning aerosol from North America and Canada, and we evaluate their influence on aerosol population and cloud condensation nuclei in terms of potential activation fraction and concentrations at supersaturation of 0.1 % and 0.2 %. The arrival of plumes dominated by the mixture of dust and marine aerosol in the ENA in the winter caused significant increases in baseline Ntot. Simultaneously, the baseline particle size modes and CCN potential activation fraction remained almost unvaried, while cloud condensation nuclei concentrations increased proportionally to Ntot. Events dominated by a mixture of marine and polluted continental aerosols in spring, fall, and winter led to a statistically significant increase in baseline Ntot, a shift towards larger particular sizes, a higher CCN potential activation fractions, and cloud condensation nuclei concentrations of >170 % and up to 240 % higher than during baseline regime. Finally, the transported aerosol plumes characterized by elevated concentration of biomass burning aerosol from continental wildfires detected in the summertime did not statistically contribute to increase baseline aerosol particle concentrations in the ENA. However, particle diameters were larger than under baseline conditions, and CCN potential activation fractions were >75 % higher. Consequentially, cloud concentration nuclei concentrations increased by ∼ 115 % during the period affected by the biomass burning events. Our results suggest that, through the year, multiday events of long-range continental aerosol transport periodically affect the ENA and represent a significant source of CCN in the marine boundary layer. Based on our analysis, in 2017, the multiday aerosol plume transport dominated by a mixture of dust and marine aerosol, a mixture of marine and polluted continental aerosols, and biomass burning aerosols caused increases in the NCCN baseline regime of, respectively, 6.6 %, 8 %, and 7.4 % at SS 0.1 % (and, respectively, 6.5 %, 8.2 %, and 7.3 % at SS 0.2 %) in the ENA.

54 ENVIRONMENTAL SCIENCES↗

Light Absorption by Brown Carbon over the South-East Atlantic Ocean

Biomass burning emissions often contain brown carbon (BrC), which represents a large family of light-absorbing organics that is chemically complex and therefore difficult to estimate their absorption of incoming solar radiation, resulting in large uncertainties in the estimation of the global direct radiative effect of aerosols. Here we investigate the contribution of BrC to the total light absorption of biomass burning aerosols over the South-East Atlantic Ocean with different optical models utilizing a suite of airborne measurements from the ORACLES 2018 campaign by introducing an effective refractive index of black carbon (BC), m eBC = n eBC +ik eBC , that accounts for all possible absorbing components at 660 nm wavelength to facilitate the attribution of absorption at shorter wavelengths. Most values of the imaginary part of the refractive index, k eBC , were larger than those commonly used for BC from biomass burning emissions, suggesting contributions from absorbers beyond BC at 660 nm. The TEM-EDX single particle analysis further suggests that these long-wavelength absorbers might include iron oxides, as iron is found to be present only when large values of k eBC are derived. Using this effective BC refractive index, we find that the contribution of BrC to the total absorption at 470 nm (R BrC,470 ) ranges from ~5–15 %, with the organic aerosol mass absorption coefficient (MAC OA,470 ) at this wavelength ranging from 0.25 ± 0.34 m 2 g -1 to 0.43 ± 0.12 m 2 g -1 . The core-shell model yielded much higher estimates of MAC OA,470 and R BrC,470 than homogeneous mixing models, underscoring the importance of model treatment. Another key finding was that estimates of the BrC contribution at 470 nm from the commonly used AAE (absorption Ångström exponent) attribution method (< 5 %) are much lower than the BrC contribution estimates (R BrC,470 ) using our new methodology that accounts for contributions from both BrC and non-carbonaceous, long-wavelength absorbers, such as magnetite. Thus, it is recommended that application of any optical properties-based attribution method use absorption coefficients at the longest possible wavelength to minimize the influence of BrC at the long wavelength and to account for potential contributions from other absorbing materials.

54 ENVIRONMENTAL SCIENCES↗

Skillful Multi‐Month Predictions of Ecosystem Stressors in the Surface and Subsurface Ocean

Abstract Anthropogenic carbon emissions and associated climate change are driving rapid warming, acidification, and deoxygenation in the ocean, which increasingly stress marine ecosystems. On top of long‐term trends, short term variability of marine stressors can have major implications for marine ecosystems and their management. As such, there is a growing need for predictions of marine ecosystem stressors on monthly, seasonal, and multi‐month timescales. Previous studies have demonstrated the ability to make reliable predictions of the surface ocean physical and biogeochemical state months to years in advance, but few studies have investigated forecast skill of multiple stressors simultaneously or assessed the forecast skill below the surface. Here, we use the Community Earth System Model (CESM) Seasonal to Multiyear Large Ensemble (SMYLE) along with novel observation‐based biogeochemical and physical products to quantify the predictive skill of dissolved inorganic carbon (DIC), dissolved oxygen, and temperature in the surface and subsurface ocean. CESM SMYLE demonstrates high physical and biogeochemical predictive skill multiple months in advance in key oceanic regions and frequently outperforms persistence forecasts. We find up to 10 months of skillful forecasts, with particularly high skill in the Northeast Pacific (Gulf of Alaska and California Current Large Marine Ecosystems) for temperature, surface DIC, and subsurface oxygen. Our findings suggest that dynamical marine ecosystem prediction could support actionable advice for decision making.

Environmental Sciences & Ecology↗

Observations Indicate That Clouds Amplify Mechanisms of Southern Ocean Heat Uptake

Abstract The Southern Ocean has absorbed most of the excess heat associated with anthropogenic greenhouse gas emissions. Since Southern Ocean observations are sparse in certain regions and seasons, much of our knowledge of ocean heat uptake is based on climate model simulations. However, climate models still inadequately represent some properties of Southern Ocean clouds, and they have not identified the mechanisms by which clouds may affect Southern Ocean heat uptake (SOHU). Here, we use the ERA5 and JRA‐55 reanalyses to assess the influence of clouds and other atmospheric processes on SOHU from 1979 to 2020. We find that years with the highest SOHU between 45° and 65°S are dominated by ocean heat uptake anomalies during winter and spring, but not during summer or fall. Winter and spring cloud cover are up to 7% higher when SOHU is up to 5.5 W/m 2 higher than the climatological seasonal mean, with the largest increases in the South Pacific Ocean. Clouds also contain more liquid water. These changes in cloud properties increase downwelling longwave radiation, amplifying ocean heat uptake. Cloud changes are also concomitant with a more stable lower atmosphere, which suppresses turbulent heat fluxes out of the surface. Overall, we find that SOHU is likely not mediated by enhanced surface shortwave absorption over the observational time period. A better understanding of how atmospheric processes impact ocean heat uptake may help improve our understanding of ocean heat uptake mechanisms in the current generation of climate models.

54 ENVIRONMENTAL SCIENCES↗

Assessing the sequestration time scales of some ocean-based carbon dioxide reduction strategies

Abstract Ocean-based carbon dioxide (CO 2 ) removal (CDR) strategies are an important part of the portfolio of approaches needed to achieve negative greenhouse gas emissions. Many ocean-based CDR strategies rely on injecting CO 2 or organic carbon (that will eventually become CO 2 ) into the ocean interior, or enhancing the ocean’s biological pump. These approaches will not result in permanent sequestration, because ocean currents will eventually return the injected CO 2 back to the surface, where it will be brought into equilibrium with the atmosphere. Here, a model of steady state global ocean circulation and mixing is used to assess the time scales over which CO 2 injected in the ocean interior remains sequestered from the atmosphere. There will be a distribution of sequestration times for any single discharge location due to the infinite number of pathways connecting a location at depth with the sea surface. The resulting probability distribution is highly skewed with a long tail of very long transit times, making mean sequestration times much longer than typical time scales. Deeper discharge locations will sequester purposefully injected CO 2 much longer than shallower ones and median sequestration times are typically decades to centuries, and approach 1000 years in the deep North Pacific. Large differences in sequestration times occur both within and between the major ocean basins, with the Pacific and Indian basins generally having longer sequestration times than the Atlantic and Southern Oceans. Assessments made over a 50 year time horizon illustrates that most of the injected carbon will be retained for injection depths greater than 1000 m, with several geographic exceptions such as the Western North Atlantic. Ocean CDR strategies that increase upper ocean ecosystem productivity with the goal of exporting more carbon to depth will have mainly a short-term influence on atmospheric CO 2 levels because ∼70% will be transported back to the surface ocean within 50 years. The results presented here will help plan appropriate ocean CDR strategies that can help limit climate damage caused by fossil fuel CO 2 emissions.

54 ENVIRONMENTAL SCIENCES↗

Riverine Plastic Pollution: Sampling and Analysis Methods

Riverine plastic pollution has been found in all major U.S. rivers, but the exact amount of plastic being released to the oceans has not been quantified. Field studies conducted in U.S. rivers have used a range of sampling and analysis techniques and rarely measured the mass of the plastic collected. Measurements of riverine plastic pollution are needed to calibrate and validate models used to estimate the U.S. riverine plastic emissions to the oceans. This report surveys measurement methods used to quantify riverine pollution and current estimates of U.S. riverine plastic pollution from measurements and models. Measurement methods include field sampling and laboratory analysis. Field sampling methods are described for large (macro) and small (micro) plastic particles. Laboratory analysis methods are described for macro and microplastic with an emphasis on the detailed characterization processes of microplastics. Waterborne leachate analysis is also briefly described. Three models are described that estimate plastic pollution based on mismanaged plastic waste in the river catchment basins. The models were validated and calibrated with global data sources. The data sources were predominantly outside of the U.S., where the magnitude and composition of plastic pollution is different than what is found in U.S. rivers. Comprehensive measurements of riverine plastics are needed not only to characterize the riverine plastic pollution, but also parameterize and validate models of plastic fate and transport. This report also describes five key U.S. rivers that span a range of sizes and environmental conditions that could be sampled to obtain data to support characterization and model development of plastic pollution from rivers to oceans. Sampling and analysis protocol recommendations are made to ensure the highest quality of data are collected in the five rivers.

54 ENVIRONMENTAL SCIENCES↗

Atmospheric Radiative and Oceanic Biological Productivity Responses to Increasing Anthropogenic Combustion‐Iron Emission in the 1850–2010 Period

Abstract Anthropogenic emission is an important component of the present‐day iron cycle yet its long‐term impacts on climate are poorly understood. Iron mineralogy strongly affects its radiative and oceanic interactions and was unrepresented in previous studies. We perform simulations using a mineralogy‐based inventory and an atmospheric transport model and estimate the 1850–2010 global mean direct radiative forcing (DRF) to be +0.02 to +0.10 W/m 2 . We estimate that the CO 2 sequestration of 0.2–13 ppmv over the last 150 years due to enhanced phytoplankton productivity by anthropogenic iron deposition causes an avoided CO 2 forcing of −0.002 to −0.16 W/m 2 . While globally small, these impacts can be higher in specific regions; the anthropogenic DRF is +0.5 W/m 2 over areas with more coal combustion and metal smelting, and anthropogenic soluble iron sustains >10% of marine net primary productivity in the high‐latitude North Pacific Ocean, a region vulnerable to stratification due to climate change.

54 ENVIRONMENTAL SCIENCES↗

Surface Methane Concentrations Along the Mid-Atlantic Bight Driven by Aerobic Subsurface Production Rather Than Seafloor Gas Seeps

Relatively minor amounts of methane, a potent greenhouse gas, are currently emitted from the oceans to the atmosphere, but such methane emissions have been hypothesized to increase as oceans warm. Here, we investigate the source, distribution, and fate of methane released from the upper continental slope of the U.S. Mid-Atlantic Bight, where hundreds of gas seeps have been discovered between the shelf break and ~1,600 m water depth. Using physical, chemical, and isotopic analyses, we identify two main sources of methane in the water column: seafloor gas seeps and in situ aerobic methanogenesis which primarily occurs at 100–200 m depth in the water column. Stable isotopic analyses reveal that water samples collected at all depths were significantly impacted by aerobic methane oxidation, the dominant methane sink in this region, with the average fraction of methane oxidized being 50%. Due to methane oxidation in the deeper water column, below 200 m depth, surface concentrations of methane are influenced more by methane sources found near the surface (0–10 m depth) and in the subsurface (10–200 m depth), rather than seafloor emissions at greater depths.

54 ENVIRONMENTAL SCIENCES↗

Ocean-Powered Oyster Tumbling: A Review of Techniques and Opportunities for Emission Reductions

Oysters perform critical roles in shoreline ecosystems by improving water quality, providing habitat for species, and preventing erosion. These ecosystem functions are present even when oysters are farmed. Because of this, and the lack of need for nutrient inputs, oyster farming is often viewed as environmentally friendly. However, fossil fuels play a large part in oyster farming practices. Fossil fuels are used to power boats, tools, and farming equipment. Oyster tumbling machines, which are used to control biofouling and produce a desirable shape and size, use a significant amount of energy and are often powered by diesel generators. As the oyster farming industry grows and practices such as integrated multi-trophic aquaculture expand, decarbonization of the industry becomes more important. One solution may be “ocean-powered” tumbling, whereby oyster grow-out gear is designed to use a range of ocean movements to tumble oysters gradually as they grow. This solution eliminates the need for fossil fuel-powered tumblers and tends to be less labor intensive. A wide range of ocean-powered gear is used by farms across the United States. New approaches and designs are being explored, making ocean-powered oyster tumbling accessible in different environments. Water movements at oyster farms are primarily driven by tidal exchange, currents, wind waves, or a combination. This paper compares methods of ocean-powered tumbling, explores the transition from standard fossil fuel-powered tumbling techniques to ocean-powered tumbling, and estimates the emission reductions of decarbonizing oyster tumbling practices.

16 TIDAL AND WAVE POWER↗

Maritime Fuel Cell Generator Project [FY2018]

Fuel costs and emissions in maritime ports are an opportunity for transportation energy efficiency improvement and emissions reduction efforts. Ocean-going vessels, harbor craft, and cargo handling equipment are still major contributors to air pollution in and around ports. Diesel engine costs continually increase as tighter criteria pollutant regulations come into effect and will continue to do so with expected introduction of carbon emission regulations. Diesel fuel costs will also continue to rise as requirements for cleaner fuels are imposed. Both aspects will increase the cost of diesel-based power generation on the vessel and on shore. Although fuel cells have been used in many successful applications, they have not been technically or commercially validated in the port environment. One opportunity to do so was identified in Honolulu Harbor at the Young Brothers Ltd. wharf. At this facility, barges sail regularly to and from neighboring islands and containerized diesel generators provide power for the reefers while on the dock and on the barge during transport, nearly always at part load. Due to inherent efficiency characteristics of fuel cells and diesel generators, switching to a hydrogen fuel cell power generator was found to have potential emissions and cost savings. Deployment in Hawaii showed the unit needed greater reliability in the start-up sequence, as well as an improved interface to the end-user, thereby presenting opportunities for repairing/upgrading the unit for deployment in another locale. In FY2018, the unit was repaired and upgraded based on the Hawaii experience, and another deployment site was identified for another 6-month deployment of the 100 kW MarFC.

08 HYDROGEN↗

A New Framework for the Attribution of Air‐Sea CO 2 Exchange

Abstract The air‐sea transfer of carbon dioxide can be viewed as a dynamic system through which atmospheric and oceanic processes push surface waters away from thermodynamic equilibrium, while diffusive gas transfer pulls them back toward local equilibrium. These push/pull processes drive significant sub‐seasonal, seasonal, and interannual variability in air‐sea carbon fluxes, the quantification of which is critical both for diagnosing the ocean response to fossil fuel emissions and for attempts to mitigate anthropogenic climate disruption through intentional modification of surface ocean biogeochemistry. In this study, we present a new approach for attributing air‐sea carbon fluxes to specific mechanisms. The new framework is first applied to a two‐box ocean nutrient and carbon cycle model as an illustrative example. Next, outputs from a regional eddy‐resolving model of the Southern Ocean are analyzed. The roles of multiple physical and biogeochemical processes are identified. The decomposition of the seasonal air‐sea carbon flux shows the dominant role of biological carbon pumps that are partially compensated by the transport convergence. Finally, the framework is used to diagnose the response to mesoscale iron and alkalinity release, explicitly quantifying transport feedback and eventual impacts on net air‐sea carbon flux. Ocean carbon transport has divergent influences between iron and alkalinity release, due to opposing near‐surface gradients of dissolved inorganic carbon. We suggest that our attribution framework may be a useful analytical technique for monitoring natural ocean carbon fluxes and quantifying the impacts of human intervention on the ocean carbon cycle.

Ito, Takamitsu [School of Earth and Atmospheric Sc↗

Observationally constrained analysis of sulfur cycle in the marine atmosphere with NASA ATom measurements and AeroCom model simulations

The atmospheric sulfur cycle plays a key role in air quality, climate, and ecosystems, such as pollution, radiative forcing, new particle formation, and acid rain. In this study, we compare the spatially and temporally resolved measurements from the NASA Atmospheric Tomography (ATom) mission with simulations from five AeroCom III models for four sulfur species (dimethyl sulfide (DMS), sulfur dioxide (SO 2 ), particulate methanesulfonate (MSA), and particulate sulfate (SO 4 )). We focus on remote regions over the Pacific, Atlantic, and Southern oceans from near the surface to ~12 km altitude range covering all four seasons. In general, the differences among model results can be greater than 1 order of magnitude. Comparing with observations, model-simulated SO 2 is generally low, whereas SO 4 is generally high. Simulated DMS concentrations near the sea surface exceed observed levels by a factor of 5 in most cases, suggesting potential overestimation of DMS emissions in all models. With GEOS model simulations of tagging emission from anthropogenic, biomass burning, volcanic, and oceanic sources, we find that anthropogenic emissions are the dominant source of sulfate aerosol (40 %–60 % of the total amount) in the ATom measurements at almost all altitudes, followed by volcanic emissions (18 %–32 %) and oceanic sources (16 %–32 %). Similar source contributions can also be derived at broad ocean basins and on monthly scales, indicating the representativeness of ATom measurements for global ocean. Our work presents the first assessment of AeroCom sulfur study using ATom measurements, providing directions for improving sulfate simulations, which remain the largest uncertainty in radiative forcing estimates in aerosol climate models.

54 ENVIRONMENTAL SCIENCES↗

Optimizing biological carbon uptake by regulating carbonate-bicarbonate equilibrium

Balancing the global carbon budget is a grand challenge and a critical research mission for sustaining life on Earth. Oceans absorb ca. 30% of global anthropogenic CO 2 emissions and dissolved CO 2 in the oceans forms carbonic acid that dissociates to generate H + , bicarbonate, and carbonate. By regulating the carbonate-bicarbonate equilibrium, rates of marine photosynthesis can be substantially enhanced, thereby capturing and condensing CO 2 into a readily utilizable form. The specific goal of this project was to demonstrate enhanced marine biomass production at the bench-scale towards advancing sustainable marine CO 2 removal. Our proof-of-concept experimental results are highly promising and we have filed a PNNL invention disclosure. In consideration of which, no further details are included in this document.

54 ENVIRONMENTAL SCIENCES↗