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DOE OSTI2022

Increased Variability of Biomass Burning Emissions in CMIP6 Amplifies Hydrologic Cycle in the CESM2 Large Ensemble

Abstract Historical simulations performed for the Coupled Model Intercomparison Project Phase 6 used biomass burning emissions between 1997 and 2014 containing higher spatial and temporal variability compared to emission inventories specified for earlier years, and compared to emissions used in previous (e.g., CMIP5) simulation intercomparisons. Using the Community Earth System Model version 2 Large Ensemble, we show this increased biomass burning emissions variability leads to amplification of the hydrologic cycle poleward of 40°N. Notably, the high variability of biomass burning emissions leads to increased latent heat fluxes, column‐integrated precipitable water, and precipitation. Greater ocean heat uptake, weaker meridional energy transport from the tropics, greater atmospheric shortwave and longwave absorption, and lower relative humidity act to moderate this hydrologic cycle amplification. Our results suggest it is not only the secular changes (on multidecadal timescales) in biomass burning emissions that impact the hydrologic cycle, but also the shorter timescale variability in emissions.

Heyblom, Kyle B.↗
DOE OSTI2020

Modeling suggests fossil fuel emissions have been driving increased land carbon uptake since the turn of the 20th Century

Terrestrial vegetation removes CO 2 from the atmosphere; an important climate regulation service that slows global warming. This 119 Pg C per annum transfer of CO 2 into plants—gross primary productivity (GPP)—is the largest land carbon flux globally. While understanding past and anticipated future GPP changes is necessary to support carbon management, the factors driving long-term changes in GPP are largely unknown. In this study, we show that 1901 to 2010 changes in GPP have been dominated by anthropogenic activity. Our dual constraint attribution approach provides three insights into the spatiotemporal patterns of GPP change. First, anthropogenic controls on GPP change have increased from 57% (1901 decade) to 94% (2001 decade) of the vegetated land surface. Second, CO 2 fertilization and nitrogen deposition are the most important drivers of change, 19.8 and 11.1 Pg C per annum (2001 decade) respectively, especially in the tropics and industrialized areas since the 1970’s. Third, changes in climate have functioned as fertilization to enhance GPP (1.4 Pg C per annum in the 2001 decade). These findings suggest that, from a land carbon balance perspective, the Anthropocene began over 100 years ago and that global change drivers have allowed GPP uptake to keep pace with anthropogenic emissions.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2022

Pan-Arctic seasonal cycles and long-term trends of aerosol properties from 10 observatories

Even though the Arctic is remote, aerosol properties observed there are strongly influenced by anthropogenic emissions from outside the Arctic. This is particularly true for the so-called Arctic haze season (January through April). In summer (June through September), when atmospheric transport patterns change, and precipitation is more frequent, local Arctic sources, i.e., natural sources of aerosols and precursors, play an important role. Over the last few decades, significant reductions in anthropogenic emissions have taken place. At the same time a large body of literature shows evidence that the Arctic is undergoing fundamental environmental changes due to climate forcing, leading to enhanced emissions by natural processes that may impact aerosol properties. In this study, we analyze 9 aerosol chemical species and 4 particle optical properties from 10 Arctic observatories (Alert, Kevo, Pallas, Summit, Thule, Tiksi, Barrow/Utgiavik, Villum, and Gruvebadet and Zeppelin Observatory – both at Ny-Ålesund Research Station) to understand changes in anthropogenic and natural aerosol contributions. Variables include equivalent black carbon, particulate sulfate, nitrate, ammonium, methanesulfonic acid, sodium, iron, calcium and potassium, as well as scattering and absorption coefficients, single scattering albedo and scattering Ångström exponent. First, annual cycles are investigated, which despite anthropogenic emission reductions still show the Arctic haze phenomenon. Second, long-term trends are studied using the Mann–Kendall Theil–Sen slope method. We find in total 41 significant trends over full station records, i.e., spanning more than a decade, compared to 26 significant decadal trends. The majority of significantly declining trends is from anthropogenic tracers and occurred during the haze period, driven by emission changes between 1990 and 2000. For the summer period, no uniform picture of trends has emerged. Twenty-six percent of trends, i.e., 19 out of 73, are significant, and of those 5 are positive and 14 are negative. Negative trends include not only anthropogenic tracers such as equivalent black carbon at Kevo, but also natural indicators such as methanesulfonic acid and non-sea-salt calcium at Alert. Positive trends are observed for sulfate at Gruvebadet. No clear evidence of a significant change in the natural aerosol contribution can be observed yet. However, testing the sensitivity of the Mann–Kendall Theil–Sen method, we find that monotonic changes of around 5 % yr –1 in an aerosol property are needed to detect a significant trend within one decade. This highlights that long-term efforts well beyond a decade are needed to capture smaller changes. It is particularly important to understand the ongoing natural changes in the Arctic, where interannual variability can be high, such as with forest fire emissions and their influence on the aerosol population. To investigate the climate-change-induced influence on the aerosol population and the resulting climate feedback, long-term observations of tracers more specific to natural sources are needed, as well as of particle microphysical properties such as size distributions, which can be used to identify changes in particle populations which are not well captured by mass-oriented methods such as bulk chemical composition.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2020

Impact of Dust-Cloud-Radiation-Precipitation Dynamical Feedback on Subseasonal-to-Seasonal Variability of the Asian Summer Monsoon in Global Variable-Resolution Simulations With MPAS-CAM5

In this study, we investigate the effects of increased dust emission from the Middle East deserts on subseasonal-to-seasonal (S₂S) variability of the Asian summer monsoon (ASM). Numerical experiments are performed using the Model for Prediction Across Scales (MPAS) coupled with the Community Atmosphere Model (CAM5) physics, with regional refinement at 30 km grid resolution over South Asia and the surrounding regions. Result shows that increased dust emission and transport from the Middle East/West Asia region induces a strong dust-cloud-radiation-precipitation-circulation feedback, resulting in a colder surface over the desert regions and the western Tibetan Plateau, but warmer and moister troposphere with enhanced cloudiness and precipitation over the Pakistan/Northwest India (PNWI) region. The latter changes are amplified by the dust aerosol induced Elevated Heat Pump (EHP) mechanism along the West Himalayas/Iranian Plateau foothill regions, most pronounced during May-June. During July-August, cloud radiation feedback further enhances the warming of the upper troposphere, and cooling of the land surface over the PNWI and adjacent regions over West Asia. The upper tropospheric heating and increased precipitation over PNWI spur a large-scale anomalous Rossby wavetrain and a northward displacement of the subtropical jetstream, manifesting in a contraction of the South Asian High and westward shift of the Western Pacific Subtropical High. As a result, the entire ASM precipitation-cloud system is displaced westward. Precipitation and cloudiness are intensified over northwest and western India and west Asia, but suppressed over southern and central East Asia. Analyses of the S₂S variability of the upper level vorticity balance suggests that heating by Middle East dust plays an important role in exciting, and anchoring a teleconnection pattern through interactions among dust-cloud radiation, precipitation heating over the PNWI, the development of an upper level Rossby wavetrain, and the northward shift of the boreal summer jetstream over Eurasia.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2025

Measurement report: Extreme heat and wildfire emissions enhance volatile organic compounds in a temperate forest

Climate extremes are projected to cause unprecedented deviations in the emission and transformation of volatile organic compounds (VOCs), which trigger feedback mechanisms that will impact the atmospheric oxidation and formation of aerosols and clouds. However, the response of VOCs to future conditions such as extreme heat and wildfire events is still uncertain. This study explored the modification of the mixing ratio and distribution of several anthropogenic and biogenic VOCs in a temperate oak–hickory–juniper forest as a response to increased temperature and transported biomass burning plumes. A chemical ionization mass spectrometer was deployed on a tower at a height of 32 m in rural central Missouri, United States, for the continuous and in situ measurement of VOCs from June to August of 2023. The maximum observed temperature in the region was 38 °C, and during multiple episodes the temperature remained above 32 °C for several hours. Biogenic VOCs such as isoprene and monoterpene followed closely the temperature daily profile but at varying rates, whereas anthropogenic VOCs were insensitive to elevated temperature. During the measurement period, wildfire emissions were transported to the site and substantially increased the mixing ratios of acetonitrile and benzene, which are produced from burning of biomass. An in-depth analysis of the mass spectra revealed more than 250 minor compounds, such as formamide and methylglyoxal. Extreme heat and presence of wildfire plumes modified the overall volatility, reactivity, O : C, and H : C ratios of the extended list of VOCs. The calculated OH reactivities during extreme temperature condition and transport of biomass burning plumes were 106.37±4.27 and 106.22±5.15 s −1 , respectively, which are substantially higher than background level of 98.78±1.16 s −1 . Multivariate analysis also clustered the compounds into five factors, which highlighted the sources of the unaccounted-for VOCs. Ultimately, results here underscore the effect of extreme heat and wildfire emissions on the overall chemical properties VOC in a temperate forest.

Salvador, Christian Mark [Oak Ridge National Labor↗
DOE OSTI2023

Biologically Cooling the Planet: A BRISK Approach that Directly Connects the Ground to Deep Space

Climate change is a grave threat to our ability to thrive and prosper on Earth. Accumulation of greenhouse gases in the atmosphere stifle the Earth’s ability to cool itself, which leads to a rise of the average temperature – Global warming. The planetary cooling is exclusively radiative – thermal radiation escapes into cold outer space via a flux of photons at the low-infrared range. The penetration of these photons through Earth’s atmosphere is dictated by atmospheric transparency, which, serendipitously possesses a window centered around the peak of the Plank spectrum for a black body at about room temperature – the average temperature of Earth. This window spanning about 8 --13 μm wavelengths allows most of the photons in this range to escape into the Cosmos carrying our planet’s heat away. The efficiency of this outer heat flux – and thus planet’s cooling ability – can be controlled via emissivity – a function of wavelength which multiplies the fundamental Plank spectrum of a black body at a given temperature. In the presence of non-trivial atmospheric transparency it can be shown that radiative cooling can be enhanced with properly “designed” emissivity function. For the last 100 years, or so, people have been looking into ways to engineer materials to take advantage of such enhancement for various cooling applications, from making ice to cool clothes, and substantial progress has been achieved, including cooling in direct sunlight. The beauty if this approach is that it is entirely passive – no energy input is required. The objective of this project was to investigate whether biological systems possess such advanced cooling capacity, developed via millennia of evolution, to enhance plant’s adaptation to a hot environment, to increase cooling capability, and possibly modulate spectral emissivities on short or long time scales. We wanted to know if BRISK (Biological Radiative Sky Cooling) occurs and to what extent. It is unknown whether biological systems can perform this "spectral redistribution." It is reasonable to expect, however, that they might: in particular, desert plants under high heat stress and arid conditions might evolve this mechanism in order to maintain a tolerable internal temperature. Our intended approach was twofold: extensive literature search and supporting experimental investigations on select plants. We obtained the answers from the former, while the latter proved to be more complicated to perform with required accuracy in the timespan/budget of a small seedling project. After one year of research, we concluded that among the plant species studied there seem to be no evidence of BRISK, but it’s not the end of the story. Our planet’s biosphere is immense, and the evolution is continuing. With our preliminary results and a better understanding of what to look for further discoveries await, considering the accelerated pace of infrared imaging and spectroscopy technology development, from microscopic to satellite-based studies of plants and canopies. In the end, Earth’s energy balance is ultimately tied to radiative cooling so that further investigation into this problem is directly tied to solving the Climate Change challenge.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2022

Economic and biophysical limits to seaweed farming for climate change mitigation

Net-zero greenhouse gas (GHG) emissions targets are driving interest in opportunities for biomass-based negative emissions and bioenergy, including from marine sources such as seaweed. Yet the biophysical and economic limits to farming seaweed at scales relevant to the global carbon budget have not been assessed in detail. We use coupled seaweed growth and technoeconomic models to estimate the costs of global seaweed production and related climate benefits, systematically testing the relative importance of model parameters. Under our most optimistic assumptions, sinking farmed seaweed to the deep sea to sequester a gigaton of CO 2 per year costs as little as US$\$$480 per tCO 2 on average, while using farmed seaweed for products that avoid a gigaton of CO 2 -equivalent GHG emissions annually could return a profit of $\$$50 per tCO 2 -eq. However, these costs depend on low farming costs, high seaweed yields, and assumptions that almost all carbon in seaweed is removed from the atmosphere (that is, competition between phytoplankton and seaweed is negligible) and that seaweed products can displace products with substantial embodied non-CO 2 GHG emissions. Moreover, the gigaton-scale climate benefits we model would require farming very large areas (>90,000 km 2 )—a >30-fold increase in the area currently farmed. Our results therefore suggest that seaweed-based climate benefits may be feasible, but targeted research and demonstrations are needed to further reduce economic and biophysical uncertainties.

60 APPLIED LIFE SCIENCES↗
DOE OSTI2026

Polar primary aerosols across the ocean-sea ice-snow-atmosphere interface: From sources to impacts

Primary aerosols play a critical role in polar climate systems, influencing cloud formation, precipitation, radiative balance, and surface energy budgets. This paper provides a comprehensive synthesis of primary aerosol sources, transformation and removal processes, and broader atmospheric impacts in polar regions, emphasizing their links to ocean and sea ice biogeochemistry. These aerosols (including sea salt, primary organic aerosol, and primary biological aerosol particles) originate from marine and cryospheric environments and are emitted through physical processes, such as wave breaking, bubble bursting, and blowing snow. Emission sources include seawater, sea ice, snow, and freshwater from river discharge and glacial runoff. Once airborne, these particles can serve as a chemical reservoir, influencing atmospheric composition and reactivity, and as seeds for cloud droplet and ice crystal formation, influencing cloud microphysics and polar climate. Despite their importance, many of the processes governing primary aerosol emissions and transformations remain poorly constrained. The most pressing knowledge gaps pertain to emission processes, limited spatiotemporal observational coverage, instrumentation constraints, parameterization development, and the integration of interdisciplinary expertise. To improve our understanding of primary aerosol drivers and their response to climate, future research efforts should prioritize strategically coordinated and cross-disciplinary process studies, advancements in measurement technologies and coverage, and close collaboration between modelers and observational scientists to inform and refine model parameterizations. As polar regions continue to undergo profound changes marked by increased precipitation, reduced sea and land ice, freshening oceans, and shifting ecosystem dynamics, characterizing present-day primary aerosol populations is vital. Improved understanding will be essential for anticipating future changes in aerosol-radiation and aerosol-cloud interactions and their implications for polar and global climate systems.

Aerosol-cloud↗
DOE OSTI2020

Optical properties and composition of viscous organic particles found in the Southern Great Plains

Abstract. Atmospheric high-viscosity organic particles (HVOPs) were observed in samples of ambient aerosols collected in April and May 2016 in the Southern Great Plains of the United States. These particles were apportioned as either airborne soil organic particles (ASOPs) or tar balls (TBs) from biomass burning based on spetro-microscopic imaging and assessments of meteorological records of smoke and precipitation data. Regardless of their apportionment, the number fractions of HVOPs were positively correlated (R2=0.85) with increased values of absorption Ångström exponent (AAE) measured in situ for ambient aerosol at the site. Extending this correlation to 100 % HVOPs yields an AAE of 2.6, similar to previous literature reports of the class of light-absorbing organic particles known as brown carbon (BrC). One out of the three samples investigated had a significant number of ASOPs, while the other two samples contained TBs. Although there are chemical similarities between ASOPs and TBs, they can be distinguished based on composition inferred from near-edge absorption X-ray fine structure (NEXAFS) spectroscopy. ASOPs were distinguished from TBs based on their average -COOH/C=C and -COOH/COH peak ratios, with ASOPs having lower ratios. NEXAFS spectra of filtered soil organic brine particles nebulized from field samples of standing water deposited after rain were consistent with ASOPs when laboratory particles were generated by bubble bursting at the air–organic brine interface. However, particles generated by nebulizing the bulk volume of soil organic brine had a particle composition different from ASOPs. These observations are consistent with the raindrop generation mechanism responsible for ASOP emissions in the area of study. In contrast, nebulized samples carry with them higher fractions of soil inorganics dissolved in the bulk volume of soil brine, which are not aerosolized by the raindrop mechanism. Our results support the bubble bursting mechanism of particle generation during rainfall resulting in the ejection of soil organics into the atmosphere. In addition, our results show that ASOPs may only be atmospherically relevant during times when suitable emission conditions are met.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2020

Constraining the Twomey effect from satellite observations: issues and perspectives

Abstract. The Twomey effect describes the radiative forcing associated with a change in cloud albedo due to an increase in anthropogenic aerosol emissions. It is driven by the perturbation in cloud droplet number concentration (ΔNd, ant) in liquid-water clouds and is currently understood to exert a cooling effect on climate. The Twomey effect is the key driver in the effective radiative forcing due to aerosol–cloud interactions, but rapid adjustments also contribute. These adjustments are essentially the responses of cloud fraction and liquid water path to ΔNd, ant and thus scale approximately with it. While the fundamental physics of the influence of added aerosol particles on the droplet concentration (Nd) is well described by established theory at the particle scale (micrometres), how this relationship is expressed at the large-scale (hundreds of kilometres) perturbation, ΔNd, ant, remains uncertain. The discrepancy between process understanding at particle scale and insufficient quantification at the climate-relevant large scale is caused by co-variability of aerosol particles and updraught velocity and by droplet sink processes. These operate at scales on the order of tens of metres at which only localised observations are available and at which no approach yet exists to quantify the anthropogenic perturbation. Different atmospheric models suggest diverse magnitudes of the Twomey effect even when applying the same anthropogenic aerosol emission perturbation. Thus, observational data are needed to quantify and constrain the Twomey effect. At the global scale, this means satellite data. There are four key uncertainties in determining ΔNd, ant, namely the quantification of (i) the cloud-active aerosol – the cloud condensation nuclei (CCN) concentrations at or above cloud base, (ii) Nd, (iii) the statistical approach for inferring the sensitivity of Nd to aerosol particles from the satellite data and (iv) uncertainty in the anthropogenic perturbation to CCN concentrations, which is not easily accessible from observational data. This review discusses deficiencies of current approaches for the different aspects of the problem and proposes several ways forward: in terms of CCN, retrievals of optical quantities such as aerosol optical depth suffer from a lack of vertical resolution, size and hygroscopicity information, non-direct relation to the concentration of aerosols, difficulty to quantify it within or below clouds, and the problem of insufficient sensitivity at low concentrations, in addition to retrieval errors. A future path forward can include utilising co-located polarimeter and lidar instruments, ideally including high-spectral-resolution lidar capability at two wavelengths to maximise vertically resolved size distribution information content. In terms of Nd, a key problem is the lack of operational retrievals of this quantity and the inaccuracy of the retrieval especially in broken-cloud regimes. As for the Nd-to-CCN sensitivity, key issues are the updraught distributions and the role of Nd sink processes, for which empirical assessments for specific cloud regimes are currently the best solutions. These considerations point to the conclusion that past studies using existing approaches have likely underestimated the true sensitivity and, thus, the radiative forcing due to the Twomey effect.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2020

Corrosion of AISI 310 and 316 in Molten Hydroxide Under Steam Electrolysis Conditions

Steam electrolyzers, utilizing molten hydroxide electrolyte, offers potential for improvement in electrochemical efficiency, cost reduction, use of conventional materials of construction and process scale up for large scale hydrogen production. Stainless steels, used for the fabrication of cell components (current collector, gas separator, wet seals, and manifolds) experience accelerated corrosion in the presence of molten hydroxide electrolyte in both oxidizing (anodic) and reducing (cathodic) atmospheres. In this study, the corrosion behavior of AISI 310 and 316 in hydroxide melt has been studied at 600°C for 50 h. Melt immersion tests revealed formation of the porous lithium iron oxide at the melt-oxide interface for both AISI 310 and 316. Inductively coupled plasma optical emission spectrometry (ICP-OES) analysis showed the presence of Cr in the electrolyte melt obtained from samples exposed to oxidizing atmosphere. Thermochemical analysis was performed to validate the experimental results.

corrosion↗
DOE OSTI2021

Evaluation of regional transport of PM2.5 during severe atmospheric pollution episodes in the western Yangtze River Delta, China

During winter 2018, the 16 prefecture-level cities in Anhui Province, Western Yangtze River Delta region, China had very high PM2.5 concentrations and prolonged pollution days. The impact of regional transport in the formation, accumulation, as well as dispersion of fine particulate matter (PM2.5) in Anhui Province was very significant. This study quantified and analyzed the vertical transport of PM2.5 in three major cities (Hefei, Fuyang, and Suzhou) of Anhui Province in January and July 2018 using the Weather Research and Forecasting (WRF) model coupled with the Community Multiscale Air Quality (CMAQ) model. The results of the inter-regional transport of PM2.5 revealed the dominant transport pathways for the three cities. The flux mainly flowed into Fuyang from Henan (2.23 and 1.42 kt/day in January and July, respectively) and Bozhou (1.96 and 1.21 kt/day in January and July, respectively), while the main flux from Fuyang flowed into Henan (-2.15 kt/day) and Lu'an (-1.91 kt/day) in January and Henan (-0.34 kt/day) and Bozhou (-0.29 kt/day) in July. In addition, the dominant transport pathways and the heights at which they occurred were identified: the northwest-southeast and northeast-south pathways in both winter and summer at both lower (?300 m) and higher (=300 m) levels for Fuyang; the northwest-south and northeast-southwest pathways in winter (at both lower and upper levels) and northwest-east and northeast-southwest pathways in summer at lower and upper levels for Hefei; and the northwest-southeast and northeast-south pathways in both winter (from 50 m up to the top level) and summer (between 100 and 300 m) for Suzhou. Furthermore, the intensities of daily PM2.5 transport fluxes in Fuyang during the atmospheric pollution episode (APE1) were stronger than the monthly average. These results show that joint emission controls across multiple cities along the identified pathways are urgently needed to reduce winter episodes.

Sulaymon, Ishaq D.↗
DOE OSTI2020

Hybrid Absorption–Crystallization Strategies for the Direct Air Capture of CO2 Using Phase-Changing Guanidium Bases: Insights from in Operando X-ray Scattering and Infrared Spectroscopy Measurements

Efforts to limit rising concentrations of CO 2 have motivated the development of negative emission technologies. Direct air capture (DAC) of CO 2 is one of the negative emissions technologies that has been proposed for the direct removal of CO 2 from the atmosphere. Phase-changing bis(iminonoguanidine) (BIG) sorbents have been developed for the direct air capture of CO 2 . These phase changing sorbents, specifically glyoxal-bis(iminoguanidine) (GBIG), involve (1) CO 2 absorption with aqueous amino acid salts, such as K- or Na-glycinate to yield bicarbonate-rich solutions, (2) crystallization of the bicarbonate anions with a BIG solid, which regenerates the amino acid, and (3) solid-state CO 2 release from the carbonate crystals and BIG regeneration. Despite the promising potential of these materials, their structural evolution during the thermal regeneration of the BIG solids, chemical regeneration of the sodium or potassium glycinate solvents, and the crystallization behavior of CO 2 -loaded BIG bicarbonate remain to be evaluated and understood in detail. The aim of this study is to probe these knowledge gaps. In situ wide-angle X-ray Scattering (WAXS) results show that CO 2 and water molecules in GBIG bicarbonate are simultaneously released in a single step during the thermal regeneration of the sorbent at 97 – 134 °C. In situ ATR-FTIR measurements showed that sodium glycinate and GBIG bicarbonate are simultaneously generated when GBIG, glycine, and sodium bicarbonate are reacted. The crystallization of GBIG bicarbonate from GBIG and CO 2 -loaded monoethanolamine (MEA) occurs rapidly in the first 10 min of the reaction, as determined using in situ GI-SAXS measurements. Overall, the insights from these studies are essential for the scalable implementation of CO 2 capture technologies using these phase-changing sorbents.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

Kicking the can down the road: understanding the effects of delaying the deployment of stratospheric aerosol injection

Abstract Climate change is a prevalent threat, and it is unlikely that current mitigation efforts will be enough to avoid unwanted impacts. One potential option to reduce climate change impacts is the use of stratospheric aerosol injection (SAI). Even if SAI is ultimately deployed, it might be initiated only after some temperature target is exceeded. The consequences of such a delay are assessed herein. This study compares two cases, with the same target global mean temperature of ∼1.5° C above preindustrial, but start dates of 2035 or a ‘delayed’ start in 2045. We make use of simulations in the Community Earth System Model version 2 with the Whole Atmosphere Coupled Chemistry Model version 6 (CESM2-WACCM6), using SAI under the SSP2-4.5 emissions pathway. We find that delaying the start of deployment (relative to the target temperature) necessitates lower net radiative forcing (−30%) and thus larger sulfur dioxide injection rates (+20%), even after surface temperatures converge, to compensate for the extra energy absorbed by the Earth system. Southern hemisphere ozone is higher from 2035 to 2050 in the delayed start scenario, but converges to the same value later in the century. However, many of the surface climate differences between the 2035 and 2045 start simulations appear to be small during the 10–25 years following the delayed SAI start, although longer simulations would be needed to assess any longer-term impacts in this model. In addition, irreversibilities and tipping points that might be triggered during the period of increased warming may not be adequately represented in the model but could change this conclusion in the real world.

Brody, Ezra (ORCID:000900030008681X)↗
DOE OSTI2023

Inorganic Hydrogeochemistry in the 21st Century

Abstract Chemical and isotopic processes occur in every segment of the hydrological cycle. Hydrogeochemistry—the subdiscipline that studies these processes—has seen a transformation from “witch's brew” to credible science since 2000. Going forward, hydrogeochemical research and applications are critical to meeting urgent societal needs of climate change mitigation and clean energy, such as (1) removing CO 2 from the atmosphere and storing gigatons of CO 2 in soils and aquifers to achieve net‐zero emissions, (2) securing critical minerals in support of the transition from fossil fuels to renewable energies, and (3) protecting water resources by adapting to a warming climate. In the last two decades, we have seen extensive activity and progress in four research areas of hydrogeochemistry related to water‐rock interactions: arsenic contamination of groundwater; the use of isotopic and chemical tracers to quantify groundwater recharge and submarine groundwater discharge; the kinetics of chemical reactions and the mineral‐water interface's control of contaminant fate and transport; and the transformation of geochemical modeling from an expert‐only exercise to a widely accessible tool. In the future, embracing technological advances in machine learning, cyberinfrastructure, and isotope analytical tools will allow breakthrough research and expand the role of hydrogeochemistry in meeting society's needs for climate change mitigation and the transition from fossil fuels to renewable energies.

Zhu, Chen (ORCID:0000000153746787)↗
DOE OSTI2021

Novel Algae Technology for CO2 Utilization

The United States, the world’s largest energy user and second largest CO2 emitter, is heavily dependent on fossil energy. In 2014, U.S. coal burning utilities emitted ~1562 million (MM) tons/year (TPY) of CO2 into the atmosphere, accounting for 76% of the total US power sector emissions1. Hence, reducing the CO2 emission footprint from coal plants is widely viewed as a key element in mitigating global warming. Despite significant interest, implementation of CO2 capture technologies has been constrained by the high capture cost which significantly increases the total cost of electricity. Not only is capturing CO2 with traditional technologies expensive, but generally the CO2 has little value and additional expense must be incurred for sequestration. This project funded by a SBIR grant from the U.S. D.O.E. to Helios-NRG in collaboration with the State University of New York at Buffalo (UB) and Membrane Technology and Research Inc. (MTR) aimed to develop a novel, algae based technology to capture CO2 from the effluent of coal-based power plants and convert it to renewable bio-fuels and higher value co-products such as animal feed and nutraceuticals with the potential to enable a substantial reduction in the net cost of carbon capture. The Phase 2 project was aimed at further demonstrating the technical feasibility of the proposed multi-stage continuous (MSC) flow CO2 capture system and the generation of high-value co-products to offset the CO2 capture cost. The project was completed and the project objectives were met and exceeded. A first-of-a-kind integrated, laboratory scale MSC process unit was fabricated and tested in a greenhouse. The tests were conducted with the preferred algae species identified in Phase I and simulated flue gas containing contaminants at levels typically present in the post flue gas desulfurization (FGD) stream, including ~12% CO2, acid gas (SOX, NOX), and a large number of heavy metals. The tests were successful and demonstrated a 25g/m2/day seasonal average algae productivity and an 80% CO2 capture efficiency. Two new algae species were identified for high-value nutraceutical production. Studies to improve growth rate and nutraceutical content of these algae species were performed and a pathway for further improvements was identified. A new dewatering technology called DeAqua was further advanced. Significant improvement in the performance index was achieved. The anti-fouling membrane was developed and fabricated into a module. The fabricated membrane module was tested with algae slurry and demonstrated improved fouling resistant properties, that can potentially reduce the cost and energy of the critical dewatering step. Test data were used to simulate operation of the overall process. The preliminary economic analysis was updated and modelled based on a 5000-acre algae farm. To the extent possible, the financial and operating assumptions used were the same as those used in the DOE’s 2022 projections for algae technology for CO2 capture and utilization. The results showed the proposed technology’s potential to significantly reduce the cost of CO2 capture compared to current options and that the high value products generated from the CO2 captured can make a step change in the cost of carbon capture. Plans to advance the technology to Phase 2B were developed and potential end-user partners were identified.

Maloney, James↗
DOE OSTI2022

Importance of different parameterization changes for the updated dust cycle modeling in the Community Atmosphere Model (version 6.1)

Abstract. The Community Atmosphere Model (CAM6.1), the atmospheric component of the Community Earth System Model (CESM; version 2.1), simulates the life cycle (emission, transport, and deposition) of mineral dust and its interactions with physio-chemical components to quantify the impacts of dust on climate and the Earth system. The accuracy of such quantifications relies on how well dust-related processes are represented in the model. Here we update the parameterizations for the dust module, including those on the dust emission scheme, the aerosol dry deposition scheme, the size distribution of transported dust, and the treatment of dust particle shape. Multiple simulations were undertaken to evaluate the model performance against diverse observations, and to understand how each update alters the modeled dust cycle and the simulated dust direct radiative effect. The model–observation comparisons suggest that substantially improved model representations of the dust cycle are achieved primarily through the new more physically-based dust emission scheme. In comparison, the other modifications induced small changes to the modeled dust cycle and model–observation comparisons, except the size distribution of dust in the coarse mode, which can be even more influential than that of replacing the dust emission scheme. We highlight which changes introduced here are important for which regions, shedding light on further dust model developments required for more accurately estimating interactions between dust and climate.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2024

Increased Asian Sulfate Aerosol Emissions Remarkably Enhance Sahel Summer Precipitation

Observational evidence shows that Sahel summer precipitation has experienced a considerable increase since the 1980s, coinciding with significant diverging trends of increased sulfate emissions in Asia and decreased emissions in Europe (dipole pattern of aerosols between Asia and Europe). The decrease in European sulfate aerosols has substantial effects on the Sahel summer precipitation increase, but the corresponding effect of increased Asian sulfate is unknown. Multi-model simulations in the Precipitation Driver and Response Model Intercomparison Project (PDRMIP) show, compared to decreased European aerosols, that increased Asian aerosols similarly enhance the Sahel summer precipitation but with different large-scale atmospheric circulation changes. Further analysis of the Sixth Coupled Model Intercomparison Project (CMIP6) simulations under historical attribution and various emission scenarios reinforces the results about the climate impacts of anthropogenic aerosols and suggests that in future scenarios with strong international cooperation and rapid climate mitigations (SSP2-45), the Sahel drought will be intensified likely due to the decline in Asian aerosol emissions. Our results suggest that Asian anthropogenic aerosols are likely a non-negligible driver of the recent recovery in Sahel precipitation amounts

54 ENVIRONMENTAL SCIENCES↗