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DOE OSTI2024

Crystal Engineering of Hydrogen Bonding for Direct Air Capture of CO2: A Quantum Crystallography Perspective

Rising atmospheric CO2 levels demand efficient and sustainable carbon capture solutions. Direct air capture (DAC) via crystallizing hydrogen-bonded frameworks such as carbonate salts has emerged as a promising approach. This review explores the potential of crystal engineering, in tandem with advanced quantum crystallography techniques and computational modeling, to unlock the full potential of DAC materials. We examine the critical role of hydrogen bonding and other noncovalent interactions within a family of bis-guanidines that governs the formation of carbonate salts with high CO2 capture capacity and low regeneration energies for utilization. Quantum crystallography and charge density analysis prove instrumental in elucidating these interactions. A case study of a highly insoluble carbonate salt of a 2,6-pyridine-bis-(iminoguanidine) exemplifies the effectiveness of these approaches. However, challenges remain in the systematic and precise determination of hydrogen atom positions and atomic displacement parameters within DAC materials using quantum crystallography, and limitations persist in the accuracy of current energy estimation models for hydrogen bonding interactions. Future directions lie in exploring diverse functional groups, designing advanced hydrogen-bonded frameworks, and seamlessly integrating experimental and computational modeling with machine learning. This synergistic approach promises to propel the design and optimization of DAC materials, paving the way for a more sustainable future.

36 MATERIALS SCIENCE↗

NASA NTRS2016

Mars Molniya Orbit Atmospheric Resource Mining

This NIAC (NASA Advanced Innovative Concepts) work will focus on Mars and will build on previous efforts at analyzing atmospheric mining at Earth and the outer solar system. Spacecraft systems concepts will be evaluated and traded, to assess feasibility. However the study will primarily examine the architecture and associated missions to explore the closure, constraints and critical parameters through sensitivity studies. The Mars atmosphere consists of 95.5 percent CO2 gas which can be converted to methane fuel (CH4) and Oxidizer (O2) for chemical rocket propulsion, if hydrogen is transported from electrolyzed water on the Mars surface or from Earth. By using a highly elliptical Mars Molniya style orbit, the CO2 atmosphere can be scooped, ram-compressed and stored while the spacecraft dips into the Mars atmosphere at periapsis. Successive orbits result in additional scooping of CO2 gas, which also serves to aerobrake the spacecraft, resulting in a decaying Molniya orbit.

mining↗

NASA NTRS1991

Nonlinear dynamics of global atmospheric and Earth-system processes

General Circulation Model (GCM) studies of the atmospheric response to change boundary conditions are discussed. Results are reported on an extensive series of numerical studies based on the National Center for Atmospheric Research (NCAR) Community Climate Model (CCM) general circulation model. In these studies the authors determined the response to systematic changes in atmospheric CO2 ranging from 100 to 1000 ppm; to changes in the prescribed sea surface temperature (SST) in the Gulf of Mexico, such as occurred during the deglaciation phase of the last ice age; to changes in soil moisture over North America; and to changes in sea ice extent in the Southern Hemisphere. Study results show that the response of surface temperature and other variables is nearly logarithmic, with lower levels of CO2 implying greater sensitivity of the atmospheric state to changes in CO2. It was found that the surface temperature of the Gulf of Mexico exerts considerable control over the storm track and behavior of storm systems over the North Atlantic through its influence on evaporation and the source of latent heat. It was found that reductions in soil moisture can play a significant role in amplifying and maintaining North American drought, particularly when a negative soil moisture anomaly prevails late in the spring.

Saltzman, Barry↗

NASA NTRS2002

Prebiotic Synthesis from CO Atmospheres: Implications for the origins of life

Most models of the primitive atmosphere around the time life originated suggest that the atmosphere was dominated by carbon dioxide, largely based on the notion that the atmosphere was derived via volcanic outgassing, and that those gases were similar to those found in modern volcanic effluent. These models tend to downplay the possibility of a strongly reducing atmosphere, which had been thought to be important for prebiotic synthesis and thus the origin of life. However, there is no definitive geologic evidence for the oxidation state of the early atmosphere and bioorganic compounds are not efficiently synthesized from CO2 atmospheres. In the present study, it was shown that a CO-CO2-N2-H2O atmosphere can give a variety of bioorganic compounds with yields comparable to those obtained from a strongly reducing atmosphere. Atmospheres containing carbon monoxide might therefore have been conducive to prebiotic synthesis and perhaps the origin of life. CO-dominant atmospheres could have existed if the production rate of CO from impacts of extraterrestrial materials were high or if the upper mantle had been more reduced than today.

Meyer, Michael↗

DOE OSTI2023

Duke Forest FACE (FACTS-I): Plant and Soil Response Data

This dataset describing the responses of plant and soil pools and fluxes to elevated atmospheric CO2 concentration and increased nitrogen supply was collected from Duke Forest Free Air CO2 Enrichment (FACE) – Forest-Atmosphere Carbon Transfer and Storage (FACTS-I) experiment from 1996 to 2012. The dataset includes data files for allometry (diameter at breast height, tree height, and height to live crown base), leaf area index, biomass (stem, branch, foliage, and root biomass, tree density, and basal area), net primary productivity (stem, branch, foliage, reproductive, and coarse root NPP), sap flux density, soil CO2 efflux, and stem temperature. Data files were formatted as .csv (Microsoft Excel or other spreadsheet programs can be used to read the format) and file descriptions, including variable name, unit, and data range, can be found in ‘FileDescription_[data_name].txt’ files. The Duke FACE experiment was in a loblolly pine (Pinus taeda L.) plantation established in 1983. Naturally regenerated broadleaved species including sweetgum (Liquidambar styraciflua L.) and tulip poplar (Liriodendron tulipifera L.), mostly in the overstory, and winged elm (Ulmus alata Michx.) and red maple (Acer rubrum L.) were common in the understory. The FACE experiment commenced with two plots (plots 7-8) in 1994 (Oren et al. 2001), with six additional plots (plots 1-6) coming online on 27 August 1996. CO2 enrichment was terminated on 31 October 2010 and post-enrichment data collection continued through 2012. Complete fertilization was applied annually to half of plots 7-8 from 1998 to 2004. The nutrient addition experiment expanded to half of plots 1-6 with a common protocol of N-fertilization in 2005 and continued until 2012. The levels of treatment in this dataset were expressed as ambient CO2 (AMB) or elevated CO2 (ELE) for CO2 treatment and control soil (CONT) or fertilized soil (FERT) for N treatment, respectively.

54 ENVIRONMENTAL SCIENCES↗

NASA NTRS2003

InGaAsSb Detectors' Characterization for 2-Micron CO2 Lidar/DIAL Applications

Recent interest in monitoring atmospheric CO2 focuses attention on infrared remote sensing using the 2-micron lidar/differential absorption lidar (DIAL) technique. Quantum detectors are critical components in this technique, and many research efforts concentrate on developing such devices for the 2-micron wavelength. Characterization results of InGaAsSb quantum detectors for the 2-micron wavelength range are presented, including experimental setup and procedure. Detectors are prototype devices manufactured by using separate absorption and multiplication (SAM) structures. Characterization experiments include V-I measurements, spectral response and its variation with bias voltage and temperature, noise measurements, noise-equivalent-power (NEP) and detectivity calculations, and signal-to-noise ratio (SNR) estimation. A slight increase in the output signal occurred with increased bias voltage and was associated with a noise level increase. Cooling down the detectors reduces noise and shifts the cutoff wavelength to shorter values. Further improvement in the design and manufacturing process, by increasing the device gain and lowering its noise level, is necessary to meet the required CO2 lidar/DIAL specifications.

Refaat, Tamer F.↗

NASA NTRS2003

InGaAsSb Detectors Characterization for 2-Micron CO2 Lidar/DIAL Applications

Refaat, Tamer F.↗

NASA NTRS1992

Regional climatic effects of atmospheric SO2 on Mars

The conditions under which the valley networks on Mars may have formed remains controversial. The magnitude of an atmospheric greenhouse effect by an early massive CO2 atmosphere has recently been questioned by Kasting. Recent calculations indicate that if solar luminosity were less than about 86 percent of its current value, formation of CO2 clouds in the Martian atmosphere would depress the atmospheric lapse rate and reduce the magnitude of surface warming. In light of recent revisions of magma generation on Mars during each Martian epoch, and the suggestions by Wanke et al. that the role of liquid SO2 should be more carefully explored, we have recalculated the potential greenhouse warming by atmospheric SO2 on Mars, with an emphasis on more localized effects. In the vicinity of an active eruption, the concentration of atmospheric SO2 will be higher than if it is assumed that the erupted SO2 is instantaneously globally distributed. The local steady-state concentration of SO2 is a function of the rate at which it is released, its atmospheric lifetime, and the rate at which local winds act to disperse the SO2. We have made estimates of eruption rates, length of eruption, and dispersion rates of volcanically released SO2, for a variety of atmospheric conditions and atmospheric lifetimes of SO2 to explore the maximum regional climatic effect of SO2.

Postawko, S. E.↗

DOE OSTI2019

Nonlinear Climate Responses to Increasing CO2 and Anthropogenic Aerosols Simulated by CESM1

Abstract Atmospheric CO2 and anthropogenic aerosols (AA) have increased simultaneously. Because of their opposite radiative effects, these increases may offset each other, which may lead to some nonlinear effects. Here the seasonal and regional characteristics of this nonlinear effect from the CO2 and AA forcings are investigated using the fully coupled Community Earth System Model. Results show that nonlinear effects are small in the global mean of the top-of-the-atmosphere radiative fluxes, surface air temperature, and precipitation. However, significant nonlinear effects exist over the Arctic and other extratropical regions during certain seasons. When both forcings are included, Arctic sea ice in September–November decreases less than the linear combination of the responses to the individual forcings due to a higher sea ice sensitivity to the CO2-induced warming than the sensitivity to the AA-induced cooling. This leads to less Arctic warming in the combined-forcing experiment due to reduced energy release from the Arctic Ocean to the atmosphere. Some nonlinear effects on precipitation in June–August are found over East Asia, with the northward-shifted East Asian summer rain belt to oppose the CO2 effect. In December–February, the aerosol loading over Europe in the combined-forcing experiment is higher than that due to the AA forcing, resulting from CO2-induced circulation changes. The changed aerosol loading results in regional thermal responses due to aerosol direct and indirect effects, weakening the combined changes of temperature and circulation. This study highlights the need to consider nonlinear effects from historical CO2 and AA forcings in seasonal and regional climate attribution analyses.

54 ENVIRONMENTAL SCIENCES↗

NASA NTRS1979

The effect of errors in the assignment of the transmission functions on the accuracy of the thermal sounding of the atmosphere

In order to test the error of calculation in assumed values of the transmission function for Soviet and American radiometers sounding the atmosphere thermally from orbiting satellites, the assumptions of the transmission calculation is varied with respect to atmospheric CO2 content, transmission frequency, and atmospheric absorption. The error arising from variations of the assumptions from the standard basic model is calculated.

Timofeyev, Y. M.↗

NASA NTRS1991

Particulate organic matter delta C-13 variations across the Drake Passage

Particulate organic matter (POM) was sampled during two cruise transects across the Drake Passage during March 1986 to investigate the unusual C-13 depletion in high-latitude Southern Ocean plankton. This POM delta C-13 transition from -23.2 o/oo at 53.3 deg S to values as low as -30.3 o/oo at above 62 deg S does not track previously reported abrupt changes in water chemistry and plankton species composition associated with the Polar Front Zone. The north-south isotopic trend is not accompanied by significant changes in POM carbon or nitrogen concentrations, or in POM C/N. Differences in plankton standing crop or biochemistry (e.g. lipid content) do not appear responsible for the isotopic trends observed. The latitudinal change in POM delta C-13 is highly correlated with water temperature and with the calculated concentration of CO2 (aq) at equilibrium with atmospheric CO2. These observations are consistent with the hypothesis that CO2 (aq) significantly influences POM delta C-13 in ocean surface waters.

Rau, G. H.↗

NASA NTRS2008

Solid-State 2-Micron Laser Transmitter Advancement for Wind and Carbon Dioxide Measurements From Ground, Airborne, and Space-Based Lidar Systems

NASA Langley Research Center has been developing 2-micron lidar technologies over a decade for wind measurements, utilizing coherent Doppler wind lidar technique and carbon dioxide measurements, utilizing Differential Absorption Lidar (DIAL) technique. Significant advancements have been made towards developing state-of-the-art technologies towards laser transmitters, detectors, and receiver systems. These efforts have led to the development of solid-state lasers with high pulse energy, tunablility, wavelength-stability, and double-pulsed operation. This paper will present a review of these technological developments along with examples of high resolution wind and high precision CO2 DIAL measurements in the atmosphere. Plans for the development of compact high power lasers for applications in airborne and future space platforms for wind and regional to global scale measurement of atmospheric CO2 will also be discussed.

Singh, Upendra N.↗

NASA NTRS2015

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↗

NASA NTRS2006

Using SCIAMACHY and Ground-based FTS Measurements to Test the OCO X(sub CO2) Retrieval and Validation Approach

Global, space-based observations of atmospheric CO2 with precision, resolution, and coverage needed to monitor sources and sinks: a) Spectra of reflected/scattered sunlight in NIR CO2 and O2 bands used to estimate X(sub CO2) with large sensitivity to surface; b) A-train orbit (1:15 PM polar sun sync); c) 16 day repeat cycle samples seasonal cycle on semi-monthly intervals; and d) NASA ESSP (Earth Space System Pathfinder) scheduled for Sept 2008 launch; 2 yrs lifetime. Initial comparison of SCIAMACHY and FTS retrievals for Park Falls: a) Positive bias in X(sub CO2) of approx. 10 ppm; and b) Negative bias in surface pressure After correction of spectral artifacts in O2A band: a) Largely improved agreement between SCIAMACHY and FTS X(sub CO2) (without clear bias) and in surface pressure; and b) Standard deviation of SCIAMACHY X(sub CO2 approx. 6 ppm. Good qualitative agreement with GEOS-CHEM, with GEOS-CHEM underestimating seasonal cycle. OCO is a dedicated CO2 instrument and will achieve much higher accuracy and precision: a) much higher spectral resolution (by factor of 20); and b) smaller ground pixels (by factor of 600).

CO2 measurements↗

NASA NTRS1990

The sensitivity of terrestrial carbon storage to climate change

The role of the terrestrial biosphere in controlling atmospheric CO2 levels during climate perturbations is estimated. Simulations are used to calculate the local geographical distribution of vegetation during the last glacial maximum. The known changes in sea level at this time, together with the simulated climate-driven spatial arrangement of vegetation, result in a mass transfer of carbon from the terrestrial biosphere to the atmosphere ranging from 30 Gt (corresponding to 15 ppm CO2) to -50 Gt (25 ppm). Thus, although the biosphere may have contributed to the decrease in atmospheric CO2 at 80 ppm, known to have occurred at 18 kyr, it does not seem to have been a dominant factor. For simulations run with twice the present-day CO2 levels, strong negative feedbacks appear which remove 235 Gt of carbon from the atmosphere.

Prentice, Katharine C.↗

NASA NTRS1991

Is CO2 capable to keeping early Mars warm?

One of the goals of NASA's Exobiology Research Program is to determine whether life exists today on Mars (unlikely) or whether it might have existed there at some time in the past (more likely). Speculation about extinct life is driven by the observation of channels on the Martian surface, thought to indicate the past presence of liquid water and, hence, the existence of a warmer climate. Current thinking suggests that such a climate could have been maintained if early Mars had a dense CO2 atmosphere with a surface pressure of 1 to 5 bars. One of the phenomena that Martian climate modelers have not looked at very carefully is the process of CO2 condensation. Reexamination of some of my own calculations indicates that condensation should occur at high altitudes in some high-CO2, Martian atmospheres, particularly those in which the solar constant is set to its initial main sequence value (about 70 percent of present. CO2 condensation should affect the surface temperature in two ways: (1) if it occurs in the convective lower atmosphere, condensation will reduce the magnitude of the greenhouse effect by decreasing the lapse rate; and (2) condensation at any altitude will produce clouds, which can either warm or cool the climate depending on their altitude and optical depth. Preliminary calculations with a 1-D, radiative-convective climate model indicate that the lapse rate change is substantial for low solar luminosity models. Other aspects of this study are discussed.

Kasting, J. F.↗

NASA NTRS1992

Evolution of the Martian atmosphere: The role of the polar caps

Lines of evidence indicate that early in Mars' history, it had a much thicker CO2 atmosphere than it does today. A model was constructed for the evolution of the Martian atmosphere that self consistently calculates the rates at which CO2 is stored in Mars' polar reservoirs. Given some initial abundance, which is assumed to be entirely in the atmosphere, the model calculates the annually averaged temperature of the equatorial region and the polar region, and the planetwide mean. Thus far, results obtained for the case where CO2 condensation in the atmosphere is not a limiting factor. Results fall into two categories: initial inventories above 1 bar and below 1 bar. For inventories above 1 bar, CO2 is partitioned between the atmosphere and regolith with the latter taking up almost 800 mbar of CO2. The rest remains in the atmosphere and is weathered out at a rate proportional to atmospheric pressure. For values less than 1 bar, the evolution scenario is different, polar caps form immediately since there is not enough greenhouse warming to prevent CO2 from going into the regolith and thereby reducing the atmospheric pressure to levels where caps can form. The results do not favor either scenario.

Haberle, R. M.↗

DOE OSTI2023

Autonomous Inversion of In Situ Deformation Measurement Data for Injection-Induced Stress Change

Geologic carbon storage (GCS) is likely to play a key part of the global effort to dramatically reduce CO2 emissions and perhaps even reduce atmospheric CO2 concentrations through carbon negative operations. A critical part of effort to commercialize and widely deploy this technology is developing the capability to rapidly assimilate real-time monitoring data into a form that will enable site operators to make decisions to manage the safe and efficient operations. Two of the risks associate with GCS are the risk of inducing fractures in the sealing formations that can create leakage pathways and the risk of inducing earthquakes of sufficient magnitude to cause public concern, property damage, or safety risks. To properly manage these risks the site operator needs to know the initial state of stress, the change in stress induced by injection, and the relationship between operational parameters such as injection rate and pressure and the change in stress. Current methods of estimating the change in stress require choosing the type of constitutive model and the model parameters based on core, log, and geophysical data during the characterization phase, with little feedback from operational observations to validate or refine these choices. These characterization methods interrogate the geologic formations using length scales, loading rates or magnitudes that are quite different from those encountered by the actual storage system. It is shown that errors in the assumed constitutive response, even when informed by laboratory tests on core samples, are likely to be common, large, and underestimate the magnitude of stress change caused by injection. Recent advances in borehole-based strain instruments and borehole and surface-based tilt and displacement instruments have now enabled monitoring of the deformation of the storage system throughout its operational lifespan. This data can enable validation and refinement of the knowledge of the geomechanical properties and state of the system, but brings with it a challenge to transform the raw data into actionable knowledge. We demonstrate a method that uses automatic differentiation and a finite-element based geomechanical model perform a gradient-based deterministic inversion of geomechanical monitoring data. This approach allows autonomous integration of the instrument data without the need for time consuming manual interpretation and selection of updated model parameters. Furthermore, only isotropic linear elasticity is considered in this paper, the approach presented is very flexible as to what type of geomechanical constitutive response can be used. The approach is easily adaptable to nonlinear physics-based constitutive models to account for common rock behaviors such as creep and plasticity. The approach also enables training of machine learning-based constitutive models by allowing back propagation of errors through the finite element calculations. This enables strongly enforcing known physics, such as conservation of momentum and continuity, while allowing data-driven models to learn the truly unknown physics such as the constitutive or petrophysical responses.

Burghardt, Jeffrey A.↗