Engineering Papers⌕ Search

SEARCH · Engineering Papers

Results for “CO 2”

Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

Quote a phrase for an exact phrase match. Source license links do not imply unrestricted reuse.

At least 505 records · Page 28

A framework for understanding efficient diurnal CO 2 reduction using Si and GaAs photocathodes

Integrated solar fuels and photoelectrochemical (PEC) CO 2 reduction (CO 2 R) are promising pathways toward producing value-added chemicals from CO 2 . However, improvements are needed in activity and selectivity as well as in fundamental understanding of device behavior to engender wide deployment. Here, we report two single-junction, integrated photocathodes for PEC CO 2 R based on TOPCon Si and GaAs substrates, which achieve -10 mA cm -2 at -0.33 V vs. RHE with 41% selectivity to C 2+ products and at -0.03 V vs. RHE with 27% selectivity to C 2+ products, respectively. We investigated the viability of a light-mediated strategy to direct selectivity in buried-junction PEC devices and confirmed that these devices could be optimized independently and described by the physics-based models of the individual components. Finally, we designed a framework to assess operational modes for PEC CO 2 R devices and demonstrated this framework under continuous galvanostatic control and variable illumination conditions.

14 SOLAR ENERGY↗

Isotherm Model for Moisture-Controlled CO 2 Sorption

Moisture-controlled sorption of CO 2 , the basis for moisture-swing CO 2 capture from air, is a novel phenomenon observed in strong-base anion exchange materials. Prior research has shown that Langmuir isotherms provide an approximate fit to moisture-controlled CO 2 sorption isotherm data. However, this fit still lacks a governing equation derived from an analytic model. As such, in this paper we derive an analytic form for an isotherm equation from a bottom-up approach, starting with a fundamental theory for an alkali liquid. In the range of interest relevant to CO 2 capture from air, an isotherm equation for an alkali liquid reduces to a simple analytic form with a single parameter, $K_{\text{eq}}$. In the limit $K_{\text{eq}} \gg 1$, a 2nd order approximation simplifies to a Langmuir isotherm that, however, deviates from experimental data. The isotherm theory for an alkali liquid has been generalized to a strong-base anion exchange material. In a strong-base anion exchange material, water concentration inside a sorbent, [H 2 O], is not large enough to be regarded as constant, which allows us to extend $K_{\text{eq}}$ to $K_{\text{eq(AEM)eff}} = K_{\text{eq(AEM)}} \times$ [H 2 O]$^{–n}$ according to the law of mass action. The final isotherm formula has been validated by experimental data from the literature. For a moisture-controlled CO 2 sorbent, $K_{\text{eq(AEM)eff}}$ varies significantly with moisture content of the sorbent. Depending on moisture level, the observed $K_{\text{eq(AEM)eff}}$ in a specific sorbent ranges from a few times to a few thousand times the value of $K_{\text{eq}}$ of a 2 mol L –1 alkali liquid.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Comparing Tandem Cell Designs for Electrochemical CO 2 Reduction to Ethylene

Electrochemical carbon dioxide reduction (CO 2 R) is a promising approach for the decentralized production of fuels such as ethylene (C 2 H 4 ). However, the use of Cu, the most efficient metal CO 2 R catalyst for the generation of C 2 H 4 known to date, generally yields a product stream with poor selectivity. In an effort to increase selectivity, the reaction from CO 2 to C 2 H 4 can be broken down into two steps using tandem CO 2 R electrolyzers: formation of CO from CO 2 and subsequent reduction of CO to C 2 H 4 . Here, in this study, we present two novel tandem electrolyzer architectures that closely integrate two cathodes, one for CO generation and one for conversion to C 2 H 4 , while still enabling independent electrical control of the cathodic surfaces. Cathode segmentation in each of these designs also permits the controlled sequencing of mass flow of chemical intermediates in the order of Au to Cu cathode catalysts, in contrast to earlier work relying on uncontrolled, passive diffusion to facilitate the flow of chemical intermediates between catalysts. When comparing the performance of the newly developed electrolyzer cell designs with a dual electrolyzer system, we found that the dual electrolyzer system yields the highest C 2 H 4 faradaic efficiencies (FEs) of 31% and C 2 H 4 concentrations (∼8 mol %). However, a single Cu-containing electrolyzer outperformed all three tandem systems in terms of C 2 H 4 FE (34%). Our findings, enabled by independent control of the two tandem cathode surfaces, indicate that tandem CO 2 R systems need to be evaluated carefully by testing them at various relevant current densities.

C2H4↗

Colloidal Synthesis of Palladium Nanocluster‐Decorated Cs 3 Sb 2 Cl 9 Perovskite Heterostructural Nanorods for Enhanced CO 2 Photoreduction

Developing efficient and sustainable photocatalysts for CO 2 reduction remains a significant challenge, particularly with environmentally benign materials. Here, in this study, we report the first one-step synthesis of metal–lead-free perovskite heterostructural nanocrystals by decorating Cs 3 Sb 2 Cl 9 perovskite nanorods with size-controlled Pd nanoclusters via a one-step hot-injection method. The resulting Pd-Cs 3 Sb 2 Cl 9 heteronanorods (HNRs) exhibit strong interfacial electronic coupling, enhanced charge separation, and excellent colloidal stability. Transient absorption spectroscopy and DFT calculations reveal a built-in electric field that drives directional electron transfer from the perovskite host to the Pd domains. Under UV irradiation, the Pd-Cs 3 Sb 2 Cl 9 HNRs demonstrate excellent CO 2 photoreduction activity with high CH 4 selectivity, achieving a record apparent quantum yield (AQY) of 2.62% among halide perovskite nanocrystal-based systems with a large electronic yield of 689.3 ± 12.2 µmol·g cat −1 . In situ spectroscopic monitoring and Gibbs free energy analysis further unveil a Pd-facilitated reaction pathway involving stabilization of key intermediates. This work introduces a new class of lead-free perovskite-based heterostructures through a facile one-step synthesis strategy and offers a new design principle for next-generation photocatalysts for solar fuel production.

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗

Data-Driven Many-Body Models for Molecular Fluids: CO 2 /H 2 O Mixtures as a Case Study

In this study, we extend the scope of the many-body TTM-nrg and MB-nrg potential energy functions (PEFs), originally introduced for halide ion–water and alkali-metal ion–water interactions, to the modeling of carbon dioxide (CO2) and water (H2O) mixtures as prototypical examples of molecular fluids. Both TTM-nrg and MB-nrg PEFs are derived entirely from electronic structure data obtained at the coupled cluster level of theory and are, by construction, compatible with MB-pol, a many-body PEF that has been shown to accurately reproduce the properties of water. Although both TTM-nrg and MB-nrg PEFs adopt the same functional forms for describing permanent electrostatics, polarization, and dispersion, they differ in the representation of short-range contributions, with the TTM-nrg PEFs relying on conventional Born–Mayer expressions and the MB-nrg PEFs employing multidimensional permutationally invariant polynomials. By providing a physically correct description of many-body effects at both short and long ranges, the MB-nrg PEFs are shown to quantitatively represent the global potential energy surfaces of the CO 2 –CO 2 and CO 2 –H 2 O dimers and the energetics of small clusters, as well as to correctly reproduce various properties in both gas and liquid phases. Furthermore, building upon previous studies of aqueous systems, our analysis provides further evidence for the accuracy and efficiency of the MB-nrg framework in representing molecular interactions in fluid mixtures at different temperature and pressure conditions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Unveiling the porosity effect of superbase ionic liquid-modified carbon sorbents in CO 2 capture from air

Direct air capture (DAC) of CO 2 represents one of the most promising technologies to achieve negative carbon emissions. In this work, the superbase ionic liquids (ILs)-modified carbon substrates were developed for DAC of CO 2 by harnessing the strong CO 2 binding capability of IL and the ordered porous channels of the carbon supports. Detailed porosity analysis revealed that the IL with an aromatic cation and an oxygenate anion preferred to fill the micropores, and a thin layer was created on the surface of the mesopores. Strong π-π interaction between the IL layer and the carbon surface was disclosed by wide-angle X-ray scattering (WAXS) analysis, leading to enhanced thermal stability of the IL phase. For the same lL coating amount, the DAC of CO 2 evaluation revealed that a larger mesopore size and pore volume in the carbon/IL composite materials led to higher CO 2 uptake capacity by exposing more active sites to integrate CO 2 from diluted sources. Further, the thermodynamic analysis confirmed the critical role of IL coating in providing strong chemisorption sites and significantly improved selectivity to enrich the diluted CO 2 from the air atmosphere. This work provides guidance on leveraging the scaffolds' surface properties and porosities of the scaffolds to optimize DAC of CO 2 behavior.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Oxygen Solubility in Aqueous Amine Solvents with Common Additives Used for CO 2 Chemical Absorption

Major sources of anthropogenic CO 2 are power generation and transportation industries where researcher continue to explore CO 2 emission mitigation strategies as applied to these CO 2 sources through carbon capture, utilization, and sequestration (CCUS). The most mature CO 2 capture technology is post-combustion carbon capture (PCCC) using aqueous amine solutions/solvents, however solvent degradation and regeneration costs are slowing the widespread adoption of PCCC. Solvent degradation of the aqueous amine solutions is mainly caused from the temperature gradient between the absorber and stripper columns and common flue gas components such as SOx, NOx, and oxygen (O 2 ). The two main classifications of solvent degradation are thermal degradation, occurring when the amine reacts with itself at elevated temperatures and anaerobic conditions and oxidative degradation. Oxidative degradation reactions can occur from oxygen mass transfer and free radical oxidation. Metals, such as iron from the corrosion of steel structures used in industrial applications such as PCCC, can help to catalyze these reactions. Various oxidative degradation studies have shown how O 2 concentrations in flue gas and, to a lesser extent, temperature influence the extent of oxidative degradation. Accurately measuring the O 2 solubility, commonly referred to as dissolved oxygen (DO), in a quick, continuous, and efficient manner in aqueous amine solvents should contribute to determine the effectiveness of mitigation strategies for oxidative degradation. Knowing that commercial PCCC amine solvents contain components beyond water, amine, carbonate species and CO 2 , this investigation was conducted to determine the oxygen solubility changes of common aqueous amines solutions with commonly used and published solvent additives. The impact of carbon loadings with and without the additives was also examined. A commercial dissolved oxygen probe was used to measure the DO concentrations and compared them against standard Winkler Method titration values. The results show that antifoam shows minimal change in [DO]. MBT yielded lower DO values, and NaVO 3 showed a higher DO concentration due to interferences. These results indicate that most common amine solvent additives should be expected to minimally impact oxygen solubility and amine oxidative degradation.

60 APPLIED LIFE SCIENCES↗

Data-assimilated time-lapse visco-acoustic full-waveform inversion: Theory and application for injected CO 2 plume monitoring

Continuous seismic monitoring for quantifying CO 2 plume migration and detection of any potential leakages in the subsurface is essential for the security of long-term anthropogenic carbon dioxide geologic storage. Traditional time-lapse full-waveform inversion (TLFWI) methods aim to map the CO 2 distribution by estimating seismic velocity changes, but recent studies find that CO 2 -induced attenuation is an important complement to seismic velocity for tracking the CO 2 plumes and even quantifying the CO 2 saturation. We have developed a novel data-assimilated TLFWI method to construct high-resolution time-lapse velocity and attenuation changes from dense time-lapse monitoring data. This method consists of two theoretical developments: visco-acoustic full-waveform inversion (QFWI) and multiparameter hierarchical matrix-powered extended Kalman filter (mHiEKF). The method is capable of (1) posing temporal constraints to retrieve time-lapse information from dense monitoring data by using mHiEKF, (2) accurately recovering high-spatial-resolution velocity and attenuation perturbations using first-order equation system-based QFWI, and (3) providing the model uncertainty by estimating their model standard deviation. With numerical examples, we first find the effectiveness of the new QFWI on estimating accurate velocity and attenuation models simultaneously. Then, a CO 2 leakage case and a realistic Frio-II CO 2 monitoring case are presented to find the advantages and applicability of our data-assimilated QFWI method for estimating time-lapse changes using dense time-lapse monitoring surveys. Here, by assimilating time-lapse seismic monitoring data over time, our data-assimilated QFWI method can improve the resolution of velocity and attenuation changes and decrease their model uncertainties.

58 GEOSCIENCES↗

Enhanced Thermal Conductivity in a Diamine-Appended Metal-Organic Framework as a Result of Cooperative CO 2 Adsorption

Using diamine-appended variants of the metal-organic framework M 2 (dobpdc) (M = Mg, Mn, Fe, Co, Zn; dobpdc 4- = 4,4'-dioxidobiphenyl-3,3'-dicarboxylate) exhibit exceptional CO 2 capture properties owing to a unique cooperative adsorption mechanism, and thus hold promise for use in the development of energy- and cost-efficient CO 2 separations. Understanding the nature of thermal transport in these materials is essential for such practical applications, however, as temperature rises resulting from exothermic CO 2 uptake could potentially offset the energy savings offered by such cooperative adsorbents. Here, molecular dynamics (MD) simulations are employed in investigating thermal transport in bare and e-2-appended Zn 2 (dobpdc) (e-2 = N -ethylethylenediamine), both with and without CO 2 as a guest. In the absence of CO 2 , the appended diamines function to enhance thermal conductivity in the ab -plane of e-2-Zn 2 (dobpdc) relative to the bare framework, as a result of noncovalent interactions between adjacent diamines that provide additional heat transfer pathways across the pore channel. Upon introduction of CO 2 , the thermal conductivity along the pore channel (the c -axis) increases due to the cooperative formation of metal-bound ammonium carbamates, which serve to create additional heat transfer pathways. In contrast, the thermal conductivity of the bare framework remains unchanged in the presence of zinc-bound CO 2 but decreases in the presence of additional adsorbed CO 2 .

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Polymeric membranes for CO 2 separation and capture

Over the past decade, CO 2 separation and capture have become the new bandwagon for polymer science and membrane research. This review presents the fundamentals of CO 2 /gas separation in polymeric membranes and discusses how these principles underpin opportunities and challenges for post-combustion carbon capture (CO 2 /N 2 ), hydrogen purification (CO 2 /H 2 ), and natural gas and biogas sweetening (CO 2 /CH 4 ). Emerging polymeric membrane materials are discussed, including a few polymers containing a high content of polar functional groups (i.e., ether oxygen-rich polymers and polymeric ionic liquids), shape-persisting glassy polymers (i.e., perfluoropolymers, thermally rearranged polymers, iptycene-containing polymers), and reactive polymers featuring facilitated transport. Moreover, the promising candidates for each CO 2 separation application are highlighted. Lastly, the permeability-selectivity data reviewed were plotted against their 2008 and 2019 upper bounds.

08 HYDROGEN↗

An experimental and modeling study of the application of membrane contactor reactors to methanol synthesis using pure CO 2 feeds

We describe here a post-combustion CO 2 capture and utilization (CCU) technology that converts the CO 2 into methanol (MeOH), a valuable chemical, thus providing a way to monetize the carbon captured to offset process costs. Methanol synthesis (MeS) has been discussed recently for application to CCU, but thermodynamic limitations make it difficult to convert in a single pass a large CO 2 fraction. Conventional catalysts show slow kinetics in converting CO 2 -rich syngas (or pure CO 2 ) into MeOH. Our Group developed a novel MeS process, employing a membrane contactor reactor (MCR) system that attains carbon conversions significantly higher than equilibrium. Our focus here is to process pure CO 2 streams by combining the MCR with a separate reactor, which converts the CO 2 into a syngas via the reverse water gas shift (RWGS) reaction. In this preliminary effort, the RWGS reactor (RWGSR) is assumed to reach equilibrium. Additional MeS kinetic rate data are generated validating experimentally the ability of the MeS-MCR to process as a feed the RWGSR exit stream. The performance of the combined (RWGSR/MeS-MCR) system is then simulated using a recently developed MeS-MCR model. In conclusion, the findings are encouraging, and research is currently ongoing to experimentally validate the RWGSR/MeS-MCR system performance.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Finite-element-based simulations of electrodes for CO 2 cascade reduction reactions

The multielectron reduction of CO 2 to liquid fuels could be a path to scalable energy storage, but reaching this goal requires major advances in catalysis and systems engineering. Cascade catalysis, which couples sequential reactions without isolating intermediates, has emerged as a promising route to enhance selectivity and efficiency in CO 2 reduction (CO 2 R). In this review, we examine how finite-element-based simulations of continuum model [finite element method (FEM)] approaches are being used to analyze and guide CO 2 R cascade systems. We first outline the fundamentals of cascade catalysis and recent advances in catalytic materials (metallic, molecular, and hybrid architectures). We then focus on FEM developments at the electrode and device scales, emphasizing how these models capture transport phenomena, local microenvironments, and geometry-dependent effects. To clarify design principles, we present case studies of cascade electrodes organized in systems without and with integrated semiconductors. We further emphasize the integration of FEM with multiscale frameworks (density functional theory, molecular dynamics, kinetic Monte Carlo) and its role in bridging atomic-level insights with device-level performance. Finally, we identify current limitations and future prospects, including improved boundary conditions, coupling with operando experiments, and machine learning-accelerated model development. Together, these insights provide design principles for next-generation CO 2 R cascade systems for efficient solar fuel production.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

A novel solid oxide electrolytic cell with reduced endothermic load for CO 2 electrolysis using (La 0.80 Sr 0.20 ) 0.95 MnO 3-δ cathode

CO 2 conversion to CO via solid oxide electrolysis provides a potentially efficient method for converting CO 2 into an industrially relevant product. A solid oxide electrolysis cell with (La 0.80 Sr 0.20 ) 0.95 MnO 3-δ (LSM) as the CO 2 reduction cathode, yttrium stabilized zirconia (YSZ) as electrolyte, and nickel as the H 2 oxidation anode was operated 800 °C and 850 °C. Thermogravimetric analysis of the LSM material showed no catalyst oxidation at operating temperatures allowing for CO 2 electrolysis without reducing safe gas. In addition, no cathode material mass gain was observed in the presence of CO suggesting little to no carbon deposition occurred above 750 °C. The formation rates of CO for the cell reached 1.15 mL∙min-1∙ cm -2 for an applied current of 150 mA∙cm -2 achieving a faradaic efficiency of 100 %. Furthermore, the cell displayed good stability in the short-term CO 2 electrolysis test with a nominal voltage drop of 4 mV h -1 for 10 h at 850°C. This study shows the feasibility of operating a solid oxide CO 2 electrolysis cell for CO production with H 2 at the anode to reduce endothermic process load.

(La0.80Sr0.20)0.95MnO3-δ↗

Characterizing Pore-Scale Geochemical Alterations in Eagle Ford and Barnett Shale from Exposure to Hydraulic Fracturing Fluid and CO 2 /H 2 O

As demand increases for an affordable energy source that is tied to an environmental obligation to reduce greenhouse gas emissions and water usage, there is a growing consideration in shale production utilizing processes such as 1) enhancing hydrocarbon recovery via carbon dioxide (CO 2 ) flooding, 2) using CO 2 as a fracturing agent to minimize water use, and 3) storing CO 2 in depleted shale formations to mitigate emissions to the atmosphere. Understanding the geochemical reactions and alterations that occur as shale is exposed to fluids and CO 2 is necessary to develop and optimize each of these processes for field applications. While the majority of shale formations are stimulated using traditional fracturing fluid, some may be fractured using CO 2 or other non-traditional means. We examine the effect fracturing fluid has on shale and how it behaves with secondary exposure to dry CO 2 or CO 2 -saturated water using in situ Fourier Transform infrared spectroscopy (FTIR), feature relocation scanning electron microscopy (SEM), and surface area and pore size analysis using volumetric gas sorption. These techniques were performed on Eagle Ford and Barnett shale samples that were exposed to fracturing fluid and unexposed (as received). Shales that have been exposed to traditional fracturing fluid experienced two reaction fronts. The first reaction front was formed during exposure to the fracturing fluid (pH of ~1.4). A secondary reaction front was formed as a result of CO 2 -saturated fluid exposure in the form of carbonic acid (pH ~5.6). These two different reaction mechanisms drove multiple dissolution and precipitation cycles which altered petrophysical properties of the shale and could lead to a significant impact on flow pathways. FTIR showed that equilibration of carbonate dissolution and precipitation cycles could take as long as 35 days. Samples exposed to fracturing fluid showed significantly less carbonate reactivity compared to those exposed to water. Pore size analysis results indicate exposure to fracturing fluid blocked small nanopores (10-15 nm) reducing BET surface area and total pore volume. SEM results show barite precipitated heavily during exposure to fracturing fluid. It appeared that carbonic acid was able to extract sulfur from organic matter to form gypsum evaporites. The mineralogical (barite precipitation and calcite dissolution/precipitation) and pore-scale alterations observed in these samples may lead to enhancement of flow pathways for injected CO 2 or produced hydrocarbons.

04 OIL SHALES AND TAR SANDS↗

The Cascade Effectiveness of 3-Terminal Tandem Photocathode Architectures as Applied to CO 2 Reduction

Cascade catalysis for photoelectrochemical CO 2 reduction (CO 2 R) decouples the overall reaction into sequential steps occurring on separately optimized catalysts (for example, Ag and Cu) between which an intermediate species such as CO is transferred. A 3-terminal tandem (3TT) photovoltaic architecture advantageously holds two different catalytic regions at different potentials under a single illumination source, but its overall efficiency is low. Using a stochastic reaction-diffusion model, we have examined 3TT photocathode design principles, focusing on the coupling of surface chemistry and transport of CO both inside the boundary layer and outward, into the bulk electrolyte. We find that ensuring that the lateral diffusion distance within the boundary layer is short compared to the boundary layer thickness and controlling bulk flow are key, with interdigitated designs showing an overall conversion efficiency improvement by 2 orders of magnitude compared to the side-by-side case without flow. These findings can be adapted for other cascaded architectures.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Cascade CO 2 electroreduction enables efficient carbonate-free production of ethylene

CO 2 electroreduction provides a route to convert waste emissions into chemicals such as ethylene (C 2 H 4 ). However, the direct transformation of CO 2 -to-C 2 H 4 suffers from CO 2 loss to carbonate, consuming up to 72% of energy input. A cascade approach—coupling a solid-oxide CO 2 -to-CO electrochemical cell (SOEC) with a CO-to-C 2 H 4 membrane electrode assembly (MEA)—would eliminate CO 2 loss to carbonate. However, this approach requires a CO-to-C 2 H 4 MEA with energy efficiency well beyond demonstrations to date. Focusing on the MEA, in this study we find that an N-tolyl substituted tetrahydro-bipyridine film improves the stabilization of key reaction intermediates, while an SSC ionomer enhances CO transport to the Cu surface, enabling a C 2 H 4 faradaic efficiency of 65% at 150 mA cm –2 for 110 h. Demonstrating a cascade SOEC-MEA approach, we achieve CO 2 -to-C 2 H 4 with a ~48% reduction in energy intensity compared with the direct route. We further reduce the energy intensity by coupling CO electroreduction (CORR) with glucose electrooxidation.

10 SYNTHETIC FUELS↗

Spatial distributions of X CO 2 seasonal cycle amplitude and phase over northern high-latitude regions

Satellite-based observations of atmospheric carbon dioxide (CO 2 ) provide measurements in remote regions, such as the biologically sensitive but undersampled northern high latitudes, and are progressing toward true global data coverage. Recent improvements in satellite retrievals of total column-averaged dry air mole fractions of CO 2 (X CO 2 ) from the NASA Orbiting Carbon Observatory 2 (OCO-2) have allowed for unprecedented data coverage of northern high-latitude regions, while maintaining acceptable accuracy and consistency relative to ground-based observations, and finally providing sufficient data in spring and autumn for analysis of satellite-observed X CO 2 seasonal cycles across a majority of terrestrial northern high-latitude regions. Here, we present an analysis of X CO 2 seasonal cycles calculated from OCO-2 data for temperate, boreal, and tundra regions, subdivided into 5° latitude by 20° longitude zones. We quantify the seasonal cycle amplitudes (SCAs) and the annual half drawdown day (HDD). OCO-2 SCAs are in good agreement with ground-based observations at five high-latitude sites, and OCO-2 SCAs show very close agreement with SCAs calculated for model estimates of X CO 2 from the Copernicus Atmosphere Monitoring Services (CAMS) global inversion-optimized greenhouse gas flux model v19r1 and the CarbonTracker2019 model (CT2019B). Model estimates of X CO 2 from the GEOS-Chem CO 2 simulation version 12.7.2 with underlying biospheric fluxes from CarbonTracker2019 (GC-CT2019) yield SCAs of larger magnitude and spread over a larger range than those from CAMS, CT2019B, or OCO-2; however, GC-CT2019 SCAs still exhibit a very similar spatial distribution across northern high-latitude regions to that from CAMS, CT2019B, and OCO-2. Zones in the Asian boreal forest were found to have exceptionally large SCA and early HDD, and both OCO-2 data and model estimates yield a distinct longitudinal gradient of increasing SCA from west to east across the Eurasian continent. In northern high-latitude regions, spanning latitudes from 47 to 72° N, longitudinal gradients in both SCA and HDD are at least as pronounced as latitudinal gradients, suggesting a role for global atmospheric transport patterns in defining spatial distributions of X CO2 seasonality across these regions. GEOS-Chem surface contact tracers show that the largest X CO 2 SCAs occur in areas with the greatest contact with land surfaces, integrated over 15–30d. The correlation of X CO 2 SCA with these land surface contact tracers is stronger than the correlation of X CO 2 SCA with the SCA of CO 2 fluxes or the total annual CO 2 flux within each 5° latitude by 20° longitude zone. This indicates that accumulation of terrestrial CO 2 flux during atmospheric transport is a major driver of regional variations in X CO 2 SCA.

54 ENVIRONMENTAL SCIENCES↗