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At least 109 records · Page 6

Pilot testing of CO2 capture from a coal-fired power plant—Part 2: Results from 1-MWe pilot tests

Abstract Using a 1-MWe slipstream pilot plant, solid-sorbent-based post-combustion CO2 capture was tested at a coal-fired power plant. Results from pilot testing were used to develop a preliminary full-scale commercial design. The sorbent selected for pilot-scale evaluation during this project consisted of an ion-exchange resin that incorporated amines covalently bonded to the substrate. A unique temperature-swing-absorption (TSA) process was developed that incorporated a three-stage fluidized-bed adsorber integrated with a single-stage fluidized-bed regenerator. Overall, following start-up and commissioning challenges that are often associated with first-of-a-kind pilots, the pilot plant operated as designed and expected, with a few key exceptions. The two primary exceptions were associated with: (i) handling characteristics of the sorbent, which were sufficiently different at operating temperature than at ambient temperature when design specifications were established with lab-scale testing; and (ii) CO2 adsorption in the transport line between the regenerator and adsorber that preloaded the sorbent with CO2 prior to entering the adsorber. Results from the pilot programme demonstrate that solid-sorbent-based post-combustion capture can be utilized to achieve 90% CO2 capture from coal-fired power plants.

Sjostrom, Sharon↗

Metallic Phase-Free Zn-Al Mixed Oxide Dual Function Materials Enable High Co Selectivity in Reactive Carbon Capture From Dilute Streams

Scaling conventional carbon capture and utilization methods can be limited by cost and permitting issues associated with transportation of captured CO2. Reactive carbon capture (RCC), in which a single solid-phase dual function material (DFM) is used to both capture CO2 from dilute streams (e.g., flue gas) and catalytically convert the bound species to products in a single unit operation, has the potential to reduce energy and capital costs by over 50% relative to separate capture and conversion. To incentivize adoption, high-value products such as methanol and CO should be targeted. Appealingly, CO can be produced at atmospheric pressure, thereby lowering overall H2 demand; however, high reaction temperatures (> 600 degrees C) and the use of oxidizable transition metals, such as Ni, are often necessary to drive the reverse water-gas shift (RWGS) during reactive desorption of the bound CO2. The sensitivity of these transition metals to oxygen undercuts their utility in point source RCC. To further derisk RCC, it is essential to develop metallic-phase free DFMs that are insensitive to residual oxygen in flue gas and can achieve selective reactive desorption to CO at moderate pressures (< 400 degrees C). To this end, we have developed K-modified Zn-Al mixed oxides (K/ZnAlOx) to convert captured CO2 to CO with > 97% selectivity and yields up to 53% of captured CO2 at 400 degrees C. Complementary in situ spectroscopy studies revealed the role of K-modification in improving RCC performance of unmodified ZnAlOx. The top performing DFM was also subjected to extended RCC cycling with oxygen co-fed with CO2 during the capture test to assess durability under simulated flue gas.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Mapping Rice Production in China with AVHRR Imagery

The study of rice agriculture is necessary for both the importance of rice as a vital food source and because of the fact that cultivating it has an unfortunate byproduct, namely methane gas. As a food source, rice is a staple for a large majority of the world's population, especially in Asia. Because the populations of many Asian nations are increasing at rapid rates, the production of rice will need to similarly increase. In 1989, it was estimated that the demand for rice would increase by 65% by the year 2019. Rice crops are considered to be one of the primary anthropogenic sources of methane gas. A reason for concern is that this gas is a so-called "greenhouse" trace gas and given its increasing levels in the atmosphere, is thought to contribute to the suspected global warming phenomenon. Some estimate that methane may contribute up to 20% to the global warming effect. Trace gas emissions from anthropogenic sources is an issue that generates great worldwide interest because of the fact that mankind is very likely affecting the current and future climate in potentially negative ways. In an effort to better understand these effects, scientists and engineers are conducting research on all of the varied fronts which relate to climate change and biosphere/atmosphere interactions. The study of global warming through increasing concentrations of greenhouse gases is one area which has received much media and scientific attention. Research fueled by debates on this topic is being conducted on numerous, interrelated fronts in an effort to better understand the complex relationship between human activities and the earth's climate. The research ranges from attempting to verify if the observed data even supports the existence of an anthropogenically generated global-warming phenomenon, to identification of sources and sinks of the trace gases, to measuring the source strengths, to studies which focus on modeling the processes which generate the gases, and finally, to trying to project their impact on the global climatic system. Some of the more commonly known sources of greenhouse gases are related to industry and transportation. Carbon dioxide, CO2, from automobile emissions is one such example. Lesser known are sources from natural and cultivated vegetation, such as the methane, CH4, resulting from rice cropping. While the concentration of atmospheric methane is significantly less than that of carbon dioxide, CH4 has been estimated to have up to 32 times the insulating capability of carbon dioxide, making it an important gas to monitor. The remainder of this chapter will provide some additional background information on the effects of atmospheric methane, and the role that rice agriculture plays as a source in the methane budget. This will be followed by a brief description of efforts to model this source of atmospheric methane. Finally, this chapter will end with a statement of the hypotheses of this thesis, at which time a description of the information contained in the rest of this document will be provided.

Paliouras, Eleni J.↗

Habitable planets with high obliquities

Earth's obliquity would vary chaotically from 0 degrees to 85 degrees were it not for the presence of the Moon (J. Laskar, F. Joutel, and P. Robutel, 1993, Nature 361, 615-617). The Moon itself is thought to be an accident of accretion, formed by a glancing blow from a Mars-sized planetesimal. Hence, planets with similar moons and stable obliquities may be extremely rare. This has lead Laskar and colleagues to suggest that the number of Earth-like planets with high obliquities and temperate, life-supporting climates may be small. To test this proposition, we have used an energy-balance climate model to simulate Earth's climate at obliquities up to 90 degrees. We show that Earth's climate would become regionally severe in such circumstances, with large seasonal cycles and accompanying temperature extremes on middle- and high-latitude continents which might be damaging to many forms of life. The response of other, hypothetical, Earth-like planets to large obliquity fluctuations depends on their land-sea distribution and on their position within the habitable zone (HZ) around their star. Planets with several modest-sized continents or equatorial supercontinents are more climatically stable than those with polar supercontinents. Planets farther out in the HZ are less affected by high obliquities because their atmospheres should accumulate CO2 in response to the carbonate-silicate cycle. Dense, CO2-rich atmospheres transport heat very effectively and therefore limit the magnitude of both seasonal cycles and latitudinal temperature gradients. We conclude that a significant fraction of extrasolar Earth-like planets may still be habitable, even if they are subject to large obliquity fluctuations.

NASA Discipline Exobiology↗

Visualization of Radiation Environment on Mars: Assessment with MARIE Measurements

For a given GCR (Galactic Cosmic Ray) environment at Mars, particle flux of protons, alpha particles, and heavy ions, are also needed on the surface of Mars for future human exploration missions. For the past twelve months, the MARJE (Martian Radiation Environment Experiment) instrument onboard the 200J Mars Odyssey has been providing the radiation measurements from the Martian orbit. These measurements are well correlated with the HZETRN (High Z and Energy Transport) and QMSFRG (Quantum Multiple-Scattering theory of nuclear Fragmentation) model calculations. These model calculations during these specific GCR environment conditions are now extended and transported through the CO2 atmosphere onto the Martian surface. These calculated pa11icle flux distributions are presented as a function of the Martian topography making use of the MOLA (Mars Orbiter Laser Altimeter) data from the MGS (Mars Global Surveyor). Also, particle flux calculations are presented with visualization in the human body from skin depth to the internal organs including the blood-forming organs.

Saganti, P.↗

Spin-Up and Tuning of the Global Carbon Cycle Model Inside the GISS ModelE2 GCM

Planetary carbon cycle involves multiple phenomena, acting at variety of temporal and spacial scales. The typical times range from minutes for leaf stomata physiology to centuries for passive soil carbon pools and deep ocean layers. So, finding a satisfactory equilibrium state becomes a challenging and computationally expensive task. Here we present the spin-up processes for different configurations of the GISS Carbon Cycle model from the model forced with MODIS observed Leaf Area Index (LAI) and prescribed ocean to the prognostic LAI and to the model fully coupled to the dynamic ocean and ocean biology. We investigate the time it takes the model to reach the equilibrium and discuss the ways to speed up this process. NASA Goddard Institute for Space Studies General Circulation Model (GISS ModelE2) is currently equipped with all major algorithms necessary for the simulation of the Global Carbon Cycle. The terrestrial part is presented by Ent Terrestrial Biosphere Model (Ent TBM), which includes leaf biophysics, prognostic phenology and soil biogeochemistry module (based on Carnegie-Ames-Stanford model). The ocean part is based on the NASA Ocean Biogeochemistry Model (NOBM). The transport of atmospheric CO2 is performed by the atmospheric part of ModelE2, which employs quadratic upstream algorithm for this purpose.

Climate model↗

Hybrid Electric Aircraft Thermal Management: Now, New Visions and Future Concepts and Formulation

The global fuel consumption by commercial airlines has increased each year since 2009 and is predicted to reach an all-time high of 97 billion gallons in 2019. There is also an environmental impact from this: CO2 emissions from commercial passenger and freight operations totaled 918 Mt in 2018 (ICCT, 2019), or around 2.5% of global energy-related CO2 emissions. Passenger transport accounted for 81% of the total. Emissions from aviation have grown 32% over the past five years. Coupled with this aspect, there is a continuous and growing need to satisfy ever-growing electrical power needs on commercial and military aircraft. All the armed services (Army, Navy, and Air Force) are continuously trying to enhance UAV (unmanned aerial vehicle) endurance and range across a broad fleet of different aircraft. The commercial Boeing 787 requires about 1.2MWe and that is expected to grow. Current technologies used to supply increased on-board electrical power are generally: 1) “burn more fuel and convert through on-board generators” and 2) use additional heavy (i.e., weight-inefficient) and sometimes unsafe battery systems on-board the aircraft. The aircraft industry is seeking new, innovative ways to satisfy this increasing power demand. One as-yet-untapped power source is the enormous amount of “waste” thermal energy flowing out the jet engine exhaust; some estimates in smaller “by-pass” flow jet engines is several hundreds of kilowatts (e.g., Pratt & Whitney Canada PW545B turbofan). This quantity is much higher in large jet engines associated with commercial aircraft. This large waste thermal energy manifests itself in large temperature differences within the by-pass-flow engine exhaust system relative to outside ambient conditions, because of the actual by-pass engine design configuration. There is strong need to develop thermal technologies and systems that could harness and convert at least a portion of this thermal energy into useful electrical energy to satisfy growing on-board electrical needs. In addition, there is a strong desire within the aircraft and engine manufacturing community to reduce the “carbon footprint” of the industry though reduced fuel usage worldwide. NASA has a robust aircraft electrification program to meet these desires and support industry in its aircraft electrification objectives. This program is integrating thermoacoustic systems, advanced lightweight heat exchanger technology, and advanced heat pipe technology to capture and transport large amounts of engine waste thermal energy for on-board power conversion, advanced heat-pump cooling, and exergy enhancement (i.e., temperature lift). Advanced lightweight heat exchangers are envisioned to capture engine exhaust thermal energy at approximately 673 K and deliver it to efficient thermoacoustic power conversion systems operating at temperature ratios (Thot/Tcold) > 1.6. Advanced heat pipe systems are envisioned to transport thermal energy from low temperature sources, through thermoacoustic heat pumps, to high temperature needs such as wing anti-icing, fuel pre-heating, and combustion air pre-heating. The paper will discuss the current state-of-the-art, objectives, system design architecture, and remaining technical challenges in system formulation within the NASA aircraft electrification program.

Dyson, Rodger↗

Performance of a Natural Gas Solid Oxide Fuel Cell System With and Without Carbon Capture

The fuel cell program at the United States Department of Energy (DOE) National Energy Technology Laboratory (NETL) is focused on the development of low-cost, highly efficient, and reliable fossil-fuel-based solid oxide fuel cell (SOFC) power systems that can generate environmentally-friendly electric power with at least 90 percent carbon capture. NETL’s SOFC technology development roadmap is aligned with near-term market opportunities in the distributed generation sector to validate and advance the technology while paving the way for utility-scale natural gas (NG)- and coal-derived synthesis gas-fueled applications via progressively larger system demonstrations. The present study represents a part of a series of system evaluations being carried out at NETL to aid in prioritizing technological advances along research pathways to the realization of utility-scale SOFC systems, a transformational goal of the fuel cell program. In particular, the system performance of utility-scale NG fuel cell (NGFC) systems with and without carbon dioxide (CO2) capture is presented. The NGFC system analyzed features an external auto-thermal reformer (ATR) feeding the fuel to the SOFC system consisting of planar anode-supported SOFC with separated anode and cathode off-gas streams. In systems with CO2 capture, an air separation unit (ASU) is used to provide the oxygen for the ATR and for the combustion of unutilized fuel in the SOFC anode exhaust along with a CO2 purification unit to provide a nearly pure CO2 stream suitable for transport for usage in enhanced oil recovery operations or for storage in underground saline formations. Remaining thermal energy in the exhaust gases is recovered in a bottoming steam Rankine cycle while supplying any process heat requirements. A reduced order model (ROM) developed at the Pacific Northwest National Laboratory (PNNL) is used to predict the SOFC performance. The ROM, while being computationally effective for system studies, provides other detailed information about the state of the stack, such as the internal temperature gradient, generally not available from simple performance models often used to represent the SOFC. Such additional information can be important in system optimization studies to preclude operation under off-design conditions that can adversely impact overall system reliability. The NGFC system performance was analyzed by varying salient system parameters, including the percent of internal (to the SOFC module) NG reformation—ranging from 0 to 100 percent—fuel utilization, and current density. The impact of advances in underlying SOFC technology on electrical performance was also explored.

solid oxide fuel cell (SOFC), natural gas fuel cel↗

Transport Analysis & Optimization in a MW-Scale CO2 Electrolyzer (Final Report)

As Twelve continues to scale up their CO2 electrolyzers, both in the size of a single cell and in the number of cells used in a stack, thermal management becomes a growing concern, since excess heat can affect reaction yield and accelerate degradation. In this project, we aim to computationally explore how the anode flow fields used in Twelve’s CO2 electrolyzers function as heat exchangers. In particular, using a homogenized model of a CO2 electrolyzer, we first estimate the amount of heat generated in a cell. Then, we develop a computational fluid dynamics (CFD) model of the so-called “flow field”, i.e. a flow manifold, based on Twelve’s CAD drawings, to evaluate how these flow fields perform as a heat exchanger for the generated heat. We explore both a single cell and a 3-cell stack operating in parallel, where heat generated in one cell can now be transferred to another cell. We evaluate how performance is affected when environmental heat losses are taken into account. Finally, we leverage topology optimization to explore the types of design features a computational optimization algorithm would suggest to supplement our intuition. Overall, our work aims to provide design recommendations for CO2 electrolyzer flow fields and provides a foundation for future studies of flow field optimization.

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗

Modeling of Isotope Fractionation in Stratospheric CO2, N2O, CH4, and O3: Investigations of Stratospheric Chemistry and Transport, Stratosphere-Troposphere Exchange, and Their Influence on Global Isotope Budgets

Until recently, the stable isotopic composition of chemically and datively important stratospheric species, such as ozone (O3), carbon dioxide (CO2), nitrous oxide (N2O), and methane (CH4), was largely unexplored, despite indications from the few measurements available and theoretical studies that global-scale isotopic variations will provide a unique tool for quantifying rates of global-scale mass transport into, within, and out of the stratosphere and for understanding the mechanisms of chemical reactions involved in ozone production. The number and geographical extent of observations are beginning to increase rapidly, however, as access to the stratosphere, both directly and by remote-sensing, has increased over the last 10 years and as new analytical techniques have been developed that make global-scale isotope measurements by whole-air sampling more feasible. The objective of this study, begun in April 1999, is to incorporate into the Livermore 2D model the likely photochemical fractionation processes that determine the isotopic compositions of stratospheric CO2, N2O, CH4, and O3, and to use the model results and new observations from NASA field campaigns in 1996 and 1997 to investigate stratospheric chemistry and mass transport. Additionally, since isotopic signatures from the stratosphere are transferred to the troposphere by downward transport at middle and high latitudes, the isotopic compositions may also serve as sensitive tracers of stratosphere-totroposphere transport. Comparisons of model results with stratospheric and upper tropospheric observations from these campaigns, as well as with ground-based observations from new NOAA and NSF-sponsored studies, will help determine whether the magnitudes of the stratospheric fractionation processes are large enough to use as global-scale tracers of transport into the troposphere and, if so, will be used to help constrain the degree of coupling between the troposphere and the stratosphere.

Boering, Kristie A.↗

Transport Cost for Carbon Removal Projects With Biomass and CO2 Storage

Strategies to remove carbon from the atmosphere are needed to meet global climate goals. Promising strategies include the conversion of waste biomass to hydrogen, methane, liquid fuels, or electricity coupled with CO 2 capture and storage (CCS). A key challenge for these projects is the need to connect geographically dispersed biomass supplies with geologic storage sites by either transporting biomass or CO 2 . We assess the cost of transport for biomass conversion projects with CCS using publicly available cost data for trucking, rail, and CO 2 pipelines in the United States. We find that for large projects (order of 1 Mt/yr CO 2 or greater), CO 2 by pipeline is the lowest cost option. However, for projects that send most of the biomass carbon to storage, such as gasification to hydrogen or electricity production, biomass by rail is a competitive option. For smaller projects and lower fractions of carbon sent to storage, such as for pyrolysis to liquid fuels, CO 2 by rail is the lowest cost option. Assessing three plausible example projects in the United States, we estimate that total transport costs range from $24/t-CO 2 stored for a gasification to hydrogen project traversing 670 km to $\$ 36$/t for a gasification to renewable natural gas project traversing 530 km. In general, if developers have flexibility in choosing transport mode and project type, biomass sources and storage sites can be connected across hundreds of kilometers for transport costs in the range of $20-40/t-CO 2 stored. Truck and rail are often viable modes when pipelines cannot be constructed. Distances of 1,000 km or more can be connected in the same cost range when shared CO 2 pipelines are employed.

09 BIOMASS FUELS↗

Carbon Management Projects (CONNECT) Database and Explorer

Overview The Carbon Management Projects (CONNECT) Toolkit is an online exploratory visualization tool developed by the U.S. Department of Energy's (DOE) Office of Fossil Energy and Carbon Management (FECM) with support from other federal agencies such as the U.S. Environmental Protection Agency (EPA) and the U.S. Department of Transportation (DOT). It provides a single point of access to authoritative information on federal agency investment in a portfolio of research, development, and demonstration (RD&D) projects that have been publicly announced to advance technologies for point source carbon capture, carbon dioxide removal, transport, storage, and conversion, collectively referred to as carbon management. The RD&D programs covered in this tool are authorized by annual congressional appropriations ("Base Program") and the 2021 Infrastructure Investment and Jobs Act (IIJA). The tool also incorporates public information on other federal initiatives, such as the Regional Clean Hydrogen Hubs, and public information released by other government agencies, such as the Environmental Protection Agency's (EPA) and Primacy States’ Underground Injection Control Class VI permits and EPA’s facility level greenhouse gas (GHG) emissions. Developed in a geographic information system, the tool organizes carbon management projects into five groups based on the primary technology that a project aims to advance, each visually represented as a digital layer ("carbon management project layer"). Only federally funded projects are included, which can be awarded projects that are completed or ongoing, or projects that have been selected but are currently under negotiation. Project information can be viewed in the map or in the attribute table below it when turned on. In the map view, each project is displayed at either its host site (for field work), where available, or its performer site (project lead's location, further explained in the table below). Host sites and performer sites are represented in distinct icons. Several reference layers offer additional public information on infrastructural and natural resource environment for carbon management. These reference layers, combined with multiple geographical basemaps, enable users to visualize the carbon management project layers in context. Carbon management project information will be updated monthly based on feedback and information availability. Carbon management project layers Point Source Carbon Capture (PSC) This layer contains DOE-funded projects focused on capturing carbon dioxide (CO2) from power plants or industrial facilities. Carbon Dioxide Removal (CDR) This layer contains DOE-funded projects focused on capturing CO2 from the atmosphere, including direct air capture (DAC) and DAC hubs, direct ocean capture, enhanced mineralization, and biomass carbon removal and storage. For projects with multiple host sites, each of the sites are displayed individually with the project cost and cost sharing information representing the total for the entire project. Carbon Transport This layer contains DOE- and DOT-funded projects focused on CO2 transport. The Transport Research and Development sublayer contains projects that do not involve physical infrastructure; the Proposed Transport Corridor sublayer contains projects for which either a route for the transport infrastructure has been proposed or a general area for the transport infrastructure has been identified. Carbon Storage This layer contains DOE-funded key projects focused on CO2 storage. For projects with multiple field-work sites, each of the sites are displayed individually on the map with the project cost and cost sharing information representing the overall total for the entire project. Carbon Conversion This layer contains DOE-funded projects focused on converting CO2 into economically valuable products. Reference layers The following layers provide additional information in the geographic proximity of carbon management projects. Users should reference the original sources for more details (weblinks provided below and in pop-up windows on the map). Regional Clean Hydrogen Hub and Facility These layers illustrate the approximate areas of the Regional Clean Hydrogen Hubs announced by DOE's Office of Clean Energy Demonstrations (OCED) and the approximate locations of individual facilities that constitute the hubs (see "Where are the H2Hubs located?" on the webpage linked above). EPA Facility Level GHG Emissions (direct emitter) This layer shows direct CO2 emissions from stationary sources in 2022, using data extracted from EPA's Facility Level Information on GreenHouse gases Tool (FLIGHT). Captured and injected CO2 are not deducted from direct emitters’ total emissions. Contact EPA for additional details. Underground Injection Control Class VI permit/permit application This layer shows the locations of CO2 injection wells that are granted or in the process of applying for an Underground Injection Control Class VI permit by EPA or a Primacy State (currently Louisiana, North Dakota, and Wyoming). The URLs for the permits or permit applications are provided in the pop-up windows associated with the well locations. Contact EPA for additional details. Carbon Storage Resource This layer contains information on prospective CO2 storage resources in saline formations and oil and gas reservoirs provided by the National Carbon Sequestration Database and Geographic Information System (NATCARB) spatial database. Contact NETL for additional details. Existing CO2 pipeline This layer shows active CO2 pipelines based on information digitized from the map issued by the Pipeline and Hazardous Materials Safety Administration (PHMSA). Contact PHMSA for additional details.

Carbon Conversion↗

Accelerating CO2 Storage Site Characterization through a New Understanding of Favorable Formation Properties and the Impact of Core-Scale Heterogeneities

CO2 sequestration in deep geologic formations can permanently reduce atmospheric CO2 emissions and help to abate climate change. Target formations must undergo a time- and resource-intensive site evaluation process, assessing storage capacity, environmental safety, and suitability for CO2 trapping via reactive transport models based on data from a limited number of core samples. As such, simulations are often simplified and omit heterogeneities in formation properties that may be significant but are not well understood. To facilitate more rapid site assessment, this work first defines the aquifer properties of favorable storage formations through the analysis of promising and active storage sites. Data show quartz is the most prevalent formation mineral with carbonate minerals, highly reactive with injected CO2, present in over 75% of formations. Porosity and permeability data are highly clustered at 10–30% and 10–1000 mD. Field-scale reactive transport simulations are then constructed and used to analyze CO2 trapping efficiency. The models consider porosity and carbonate mineral heterogeneity as well as the impacts of typical temperature gradients. Simulated sequestration efficiencies are compared to results from a comparable homogenous model to understand the implications of aquifer non-uniformities. The results show a lower sequestration efficiency in the homogeneous model during the injection phase. During the post-injection phase, the homogenization of porosity and carbonate mineralogy results in a higher sequestration efficiency. Incorporating the temperature gradient also increases the sequestration efficiency. Importantly, the maximum deviation between the homogeneous and heterogeneous simulations at the end of the 50-year study period is only ~10%. Larger impacts may be incurred for properties outside the defined, promising ranges suggested here.

Environmental Sciences & Ecology↗

Monthly Representations of Mid-Tropospheric Carbon Dioxide from the Atmospheric Infrared Sounder

The Atmospheric Infrared Sounder (AIRS) on NASA's Earth Observing System Aqua spacecraft was launched in May of 2002 and acquires hyperspectral infrared spectra used to generate a wide range of atmospheric products including temperature, water vapor, and trace gas species including carbon dioxide. Here we present monthly representations of global concentrations of mid-tropospheric carbon dioxide produced from 8 years of data obtained by AIRS between the years of 2003 and 2010. We define them as "representations" rather than "climatologies" to reflect that the files are produced over a relatively short time period and represent summaries of the Level 3 data. Finally, they have not yet been independently validated. The representations have a horizontal resolution of 2.0 deg x 2.5 deg (Latitude x Longitude) and faithfully reproduce the original 8 years of monthly L3 CO2 concentrations with a standard deviation of 1.48 ppm and less than 2% outliers. The representations are intended for use in studies of the global general circulation of CO2 and identification of anomalies in CO2 typically associated with atmospheric transport. The seasonal variability and trend found in the AIRS CO2 data are discussed.

Carbon Dioxide↗

Vertical transport rates in the statosphere in 1993 from observations of CO2, N2O, and CH4

Measurements of CO2, N2O, and CH4 are analyzed to define hemispheric average vertical exchange rates in the lower stratosphere from November 1992 to October 1993. Effective vertical diffusion coefficients were small in summer, less than or equal to 1 sq m/s at altitudes below 25 km; values were similar near the tropopause in winter, but increased markedly with altitude. The analysis suggests possible longer residence times for exhaust from stratospheric aircraft, and more efficient transport from 20 km to the middle stratosphere, than predicted by many current models. Seasonally-resolved measurements of stratospheric CO2 and N2O provide significant new constraints on rates for global-scale vertical transport.

Wofsy, Steven C.↗

Vertical Transport Rates in the Stratosphere in 1993 from Observations of CO2, N2O and CH4

Measurements of CO2, N2O and CH4 are analyzed to define hemispheric average vertical exchange rates in the lower stratosphere from November 1992 to October 1993. Effective vertical diffusion coefficients were small in summer, less than or equal to 1 m(exp 2)/sec at altitudes below 25 km; values were similar near the tropopause in winter, but increased markedly with altitude. The analysis suggests possibly longer residence times for exhaust from stratospheric aircraft, and more efficient transport from 20 km to the middle stratosphere, than predicted by many current models. Seasonally-resolved measurements of stratospheric CO2 and N2O provide significant new constraints on rates for global-scale vertical transport.

Wofsy, Steven C.↗

Coherent infrared lidar mission and technology needs for measurements of transport and concentration of tropospheric trace species

The science justification and the feasibility of aircraft-based CO2 Doppler lidar measurements of transport between the free troposphere and the stratosphere (or planetary boundary layer) are discussed for a wide range of seasonal and geographic conditions. Ground-based coherent CO2 lidar aerosol scattering experiments using a stable ring resonator (about 50 mJ/pulse) CO2 laser with external injection locking are reported. Comparative studies of injection-locked CO2 laser unstable resonators and master oscillator power amplifiers are reported for future CO2 lidar missions with respect to requirements of pulse energy, duration/shape, frequency chirp, efficiency for heterodyne detection, and combined Doppler lidar and Differential Absorption Lidar missions.

Hess, R. V.↗

Reactive Transport Modeling of Anthropogenic Carbon Mineralization in Stacked Columbia River Basalt Reservoirs

Numerical simulation of CO2 storage in basalts and related reactive lithologies requires modeling complex, coupled hydrologic and chemical processes, including multi-phase flow and transport, partitioning of CO2 into the aqueous phase, and chemical interactions with aqueous fluids and rock minerals. We conducted reactive transport simulations of the Wallula pilot-scale CO2 injection into the flow tops of the Grande Ronde Basalt using our PNNL STOMP-CO2 simulator with the ECKEChem reactive module. Our mineralization simulation of the ~1,000 tons of injected CO2 into the interflow zones was based on the hydrologic transport model we previously developed. For this work, the simulations considered geochemical reactions involving the basalt components, precipitates, formation brine, and injected CO2. In our benchmark case, carbonate minerals precipitated, resulting in ~20% of the CO2 being mineralized in 10 years. Increasing the reaction rate of a single primary mineral phase (clinopyroxene) by an order of magnitude resulted in a carbon mineralization reaction extent of ~90% over the same time interval. Based on these initial sensitivity analysis results, it is clear that a thorough understanding of primary mineral dissolution rates is required for accurately predicting long-term fate and transport of injected CO2 into basalt formations. Our reactive transport numerical simulations will be key components of commercial-scale CO2 storage operation permitting, de-risking, and optimization in mafic and ultramafic reservoirs.

Cao, Ruoshi↗