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DOE OSTI2025

SPRUCE Measurements of Fine Root Production and Chemistry from Root Ingrowth Cores, Marcell Experimental Forest, Minnesota, 2022-2023

This dataset contains fine root production and tissue chemistry measurements from root ingrowth cores. Ingrowth cores were deployed in peat from June 28, 2022 to June 24, 2023 (2022-06-28 to 2023-06-24) inside SPRUCE Experiment plots at the Marcell Experimental Forest in northern Minnesota. The warming and elevated carbon dioxide (CO2) treatments in this dataset include +0 degrees Celsius (C) (+0 and +500 parts per million (ppm) elevated CO2), +4.5 degrees C (+0 and +500 ppm elevated CO2) and +9 degrees C (+0 and +500 ppm elevated CO2) for both hummocks and hollows, as well as +2.25 degrees C (+0 and +500 ppm) and +6.75 degrees C (+0 and +500 ppm) for hollows from minimum 10 cm depth from the peat surface. Measurements include root average diameter, root length, root biomass, and root tissue nitrogen (%N and δ15N) and carbon (%C and δ13C) concentration per plant functional type and microtopographical feature. Root length and biomass are standardized to 10 cm depth. These data were used to assess the warming and elevated CO2 response of fine roots across different peatland microtopographical features (hummocks and hollows) and plant functional types (shrub, spruce and larch). This dataset contains one data file in comma separate (.csv) format. Additional metadata are provided: one data dictionary and a file-level metadata file in comma separate (.csv) format and a user guide in PDF (*.pdf) format.

ESS-DIVE CSV File Formatting Guidelines Reporting ↗
DOE OSTI2020

The energetics and dynamics of confinement in flexible frameworks and molecular confinement

This project is part of an ongoing and long-term collaboration among Alexandra Navrotsky (who moved recently from UC Davis to Arizona State University), Nancy Ross at Virginia Tech, and Brian Woodfield at Brigham Young University (BYU) on the thermodynamics and lattice dynamics of nanophase and porous materials. Navrotsky emphasizes energetics of formation and guest molecule sorption by ambient and high temperature calorimetry, Woodfield contributes cryogenic heat capacity measurements, and Ross uses inelastic neutron scattering, X-ray and neutron diffraction, and high pressure studies to probe lattice dynamics and phase transitions. Porous frameworks form the chemical and structural basis for critical technologies in separations, catalysis, nuclear waste containment and biomedical applications. Hundreds of zeolites and metal organic frameworks (MOFs) have been synthesized, and their ability to separate and store hydrogen, methane and carbon dioxide has been investigated both experimentally and theoretically. Nevertheless, a fundamental and systematic molecular-level understanding of the thermodynamic and structural factors governing the stability and guest-host interactions in these materials lags behind focused studies of specific systems. Because the guest molecules interact with each other and with the host framework, molecular confinement is a finely balanced and complex phenomenon. The ability of the guest molecules to bind and diffuse through the pores is determined by the nature of the host framework which, in turn, responds to the nature and concentration of guest molecules and to pressure and temperature. The work explores how framework flexibility, tailored by structure, composition, temperature and pressure, is a general phenomenon, similar in nature but variable in extent, in both zeolites and MOFs and is part of a free energy landscape in which framework-guest interactions, pressure, and temperature result in changes in framework geometry and, in some cases, phase transitions. These subtle and/or pronounced changes in lattice geometry, energetics, and dynamics can play a decisive role in confinement and in differentiating the binding of molecules of similar size.

36 MATERIALS SCIENCE↗
DOE OSTI2020

The energetics and dynamics of confinement in flexible frameworks and molecular confinement

Porous frameworks form the chemical and structural basis for critical technologies in separations, catalysis, nuclear waste containment and biomedical applications. Hundreds of zeolites and metal organic frameworks (MOFs) have been synthesized, and their ability to separate and store hydrogen, methane and carbon dioxide has been investigated both experimentally and theoretically. Nevertheless, a fundamental and systematic molecular-level understanding of the thermodynamic and structural factors governing the stability and guest-host interactions in these materials lags behind focused studies of specific systems. Because the guest molecules interact with each other and with the host framework, molecular confinement is a finely balanced and complex phenomenon. The ability of the guest molecules to bind and diffuse through the pores is determined by the nature of the host framework which, in turn, responds to the nature and concentration of guest molecules and to pressure and temperature. The work explores how framework flexibility, tailored by structure, composition, temperature and pressure, is a general phenomenon, similar in nature but variable in extent, in both zeolites and MOFs and is part of a free energy landscape in which framework-guest interactions, pressure, and temperature result in changes in framework geometry and, in some cases, phase transitions. These subtle and/or pronounced changes in lattice geometry, energetics, and dynamics can play a decisive role in confinement and in differentiating the binding of molecules of similar size. The free energy landscape created by these structural changes links polymorphism, amorphization, “breathing,” “gate opening” and confinement. Specifically, the generality of such behavior arises from commonalities in lattice dynamics and energetics of frameworks containing a combination of strong rigid bonds and weaker more flexible deformation modes. Identifying and describing these common and collective phenomena is the focus of the research on a selected group of zeolites and MOFs. Structural studies using X-ray and neutron diffraction explore the mechanical functionality of these important materials, specifically how framework materials respond to changes in temperature, pressure and guest loading. These structural studies are combined with calorimetric measurements, using techniques uniquely developed in the participating laboratories, of heats of formation, heat capacities and entropies, and guest-host interactions. The experimental thermodynamic studies are complemented by inelastic neutron scattering studies of the lattice dynamics related both to framework vibrations and to guest-host interactions. The report below summarizes the work done at UC Davis, which is complemented by work done at BYU (Woodfield) and Virginia Tech (Ross).

36 MATERIALS SCIENCE↗
DOE OSTI2022

The energetics and dynamics of confinement in flexible frameworks and molecular confinement

Porous frameworks form the chemical and structural basis for critical technologies in separations, catalysis, nuclear waste containment and biomedical applications. Hundreds of zeolites and metal organic frameworks (MOFs) have been synthesized, and their ability to separate and store hydrogen, methane and carbon dioxide has been investigated both experimentally and theoretically. Nevertheless, a fundamental and systematic molecular-level understanding of the thermodynamic and structural factors governing the stability and guest-host interactions in these materials lags behind focused studies of specific systems. Because the guest molecules interact with each other and with the host framework, molecular confinement is a finely balanced and complex phenomenon. The ability of the guest molecules to bind and diffuse through the pores is determined by the nature of the host framework which, in turn, responds to the nature and concentration of guest molecules and to pressure and temperature. The work explores how framework flexibility, tailored by structure, composition, temperature and pressure, is a general phenomenon, similar in nature but variable in extent, in both zeolites and MOFs and is part of a free energy landscape in which framework-guest interactions, pressure, and temperature result in changes in framework geometry and, in some cases, phase transitions. These subtle and/or pronounced changes in lattice geometry, energetics, and dynamics can play a decisive role in confinement and in differentiating the binding of molecules of similar size. The free energy landscape created by these structural changes links polymorphism, amorphization, “breathing,” “gate opening” and confinement. Specifically, the generality of such behavior arises from commonalities in lattice dynamics and energetics of frameworks containing a combination of strong rigid bonds and weaker more flexible deformation modes. Identifying and describing these common and collective phenomena is the focus of the research on a selected group of zeolites and MOFs. Structural studies using X-ray and neutron diffraction explore the mechanical functionality of these important materials, specifically how framework materials respond to changes in temperature, pressure and guest loading. These structural studies are combined with calorimetric measurements, using techniques uniquely developed in the participating laboratories, of heats of formation, heat capacities and entropies, and guest-host interactions. The experimental thermodynamic studies are complemented by inelastic neutron scattering studies of the lattice dynamics related both to framework vibrations and to guest-host interactions. This research was a collaboration between UC Davis (A. Navrotsky) BYU (B. Woodfield) and Virginia Tech (N. Ross).

36 MATERIALS SCIENCE↗
NASA NTRS2018

Reliability of the Danish Aerospace Corporation Portable Pulmonary Function System

Metabolic gas analysis is a critical component of investigations that measure cardio-pulmonary exercise responses during and after long-duration spaceflight. The primary purpose of the current study was to determine the reliability and intra-subject repeatability of a metabolic gas analysis device, the Portable Pulmonary Function System (PPFS), designed for use on the International Space Station (ISS). The second objective of this study was to directly compare PPFS measurements of expired oxygen and carbon dioxide (FEO2 and FECO2) to values obtained from a well-validated clinical metabolic gas analysis system (ParvoMedics TrueOne (c) [PM]). Eight subjects performed four peak cycle tests to maximal exertion. The first test was used to prescribe work rates for the subsequent test sessions. Metabolic gas analysis for this test was performed by the PM, but samples of FEO2 and FECO2 also were simultaneously collected for analysis by the PPFS. Subjects then performed three additional peak cycle tests, consisting of three 5-min stages designed to elicit 25%, 50%, and 75% maximal oxygen consumption (VO2max) followed by stepwise increases of 25 W/min until subjects reached volitional exhaustion. Metabolic gas analysis was performed using the PPFS for these tests. Intraclass correlation coefficients (ICC), within-subject standard deviations (WS SD), and coefficients of variation (CV%) were calculated for the repeated exercise tests. Mixed model regression analysis was used to compare paired FEO2 and FECO2 values obtained from the PPFS and the PM during the initial test. The ICC values for oxygen consumption (VO2), carbon dioxide production (VCO2), and ventilation (VE) indicate that the PPFS is highly reliable (0.79 to 0.99) for all exercise levels tested; however, ICCs for respiratory exchange ratio (RER) were low ( 0.11 - 0.51), indicating poor agreement between trials during submaximal and maximal exercise. Overall, CVs ranged from 1.6% to 6.7% for all measurements, a finding consistent with reported values that were obtained using other metabolic gas analysis techniques. The PPFS and PM produced comparable FEO2 data; however, there was less agreement between measures of FECO2 obtained from the two devices, particularly at lower CO2 concentrations. The PPFS appears, in practically all respects, to yield highly reliable metabolic gas analysis data. Lower reliability of RER measurements reported in the literature and likely is not a function of the PPFS device. Further examination of PPFS CO2 data is warranted to better understand the limitations of these PPFS measurements. Overall, the PPFS when used for repeated measures of cardio-pulmonary exercise should provide accurate and reliable data for studies of human adaptation to spaceflight.

Portable Pulmonary Function System (PPFS)↗
DOE OSTI2020

Blodgett Forest CA Warming Experiment Soil Gas Well Data March 2014 to June 2017

These are soil gas data from the whole soil profile warming experiment at the University of California Blodgett Forest Research Station, in the Sierra Nevada foothills near Georgetown, CA at 1370 m above sea level. Mean annual precipitation is 1774 mm with most of it occurring from November through April and mean annual temperature is about 12.5°C . The experiment is in a thinned 80-year-old stand of mixed conifers including ponderosa pine (Pinus ponderosa), sugar pine (Pinus lambertiana), incense cedar (Calodefrus decurrens), white fir (Abies concolor), and douglas fir (Pseudotsuga menziesii). The soils are Holland series: fine-loamy, mixed, superactive, mesic Ultic Haploxeralfs of granitic origin with thick, >5 cm O horizons, minimal carbonates , and a pH that ranges from 5.6 to 6.5. The warming experiment warms the top meter of the soil profile to +4°C above ambient. These data include depth-resolved measurements of CO2 concentrations, 13CO2, apparent respiration quotients, soil temperature, and soil moisture (VWC). These data can be used to model CO2 production rates across the soil profile or to track how the sources and processes contributing to soil respiration change seasonally and with warming.

13C↗
NASA NTRS2019

Global Carbon Budget 2019

Accurate assessment of anthropogenic carbon dioxide (CO2) emissions and their redistribution among the atmosphere, ocean, and terrestrial biosphere – the “global carbon budget” – is important to better understand the global carbon cycle, support the development of climate policies, and project future climate change. Here we describe data sets and methodology to quantify the five major components of the global carbon budget and their uncertainties. Fossil CO2 emissions (E(FF)) are based on energy statistics and cement production data, while emissions from land use change (E(LUC)), mainly deforestation, are based on land use and land use change data and bookkeeping models. Atmospheric CO2 concentration is measured directly and its growth rate (G(ATM)) is computed from the annual changes in concentration. The ocean CO2 sink (S(OCEAN)) and terrestrial CO2 sink (S(LAND)) are estimated with global process models constrained by observations. The resulting carbon budget imbalance (B(IM)), the difference between the estimated total emissions and the estimated changes in the atmosphere, ocean, and terrestrial biosphere, is a measure of imperfect data and understanding of the contemporary carbon cycle. All uncertainties are reported as ±1σ. For the last decade available (2009–2018), E(FF) was 9.5±0.5 GtC/yr, E(LUC) 1.5±0.7 GtC/yr, G(ATM) 4.9±0.02 GtC/yr (2.3±0.01 ppm/yr), S(OCEAN) 2.5±0.6 GtC/yr, and S(LAND) 3.2±0.6 GtC/yr, with a budget imbalance B(IM) of 0.4 GtC/yr indicating overestimated emissions and/or underestimated sinks. For the year 2018 alone, the growth in E(FF) was about 2.1 % and fossil emissions increased to 10.0±0.5 GtC/yr, reaching 10 GtC/yr for the first time in history, E(LUC) was 1.5±0.7 GtC/yr, for total anthropogenic CO2 emissions of 11.5±0.9 GtC/yr (42.5±3.3 GtCO2). Also for 2018, G(ATM) was 5.1±0.2 GtC/yr (2.4±0.1 ppm/yr), S(OCEAN) was 2.6±0.6 GtC/yr, and S(LAND) was 3.5±0.7 GtC/yr, with a B(IM) of 0.3 GtC. The global atmospheric CO2 concentration reached 407.38±0.1 ppm averaged over 2018. For 2019, preliminary data for the first 6–10 months indicate a reduced growth in E(FF) of +0.6 % (range of −0.2 % to 1.5 %) based on national emissions projections for China, the USA, the EU, and India and projections of gross domestic product corrected for recent changes in the carbon intensity of the economy for the rest of the world. Overall, the mean and trend in the five components of the global carbon budget are consistently estimated over the period 1959–2018, but discrepancies of up to 1 GtC/yr persist for the representation of semi-decadal variability in CO2 fluxes. A detailed comparison among individual estimates and the introduction of a broad range of observations shows (1) no consensus in the mean and trend in land use change emissions over the last decade, (2) a persistent low agreement between the different methods on the magnitude of the land CO2 flux in the northern extra-tropics, and (3) an apparent underestimation of the CO2 variability by ocean models outside the tropics. This living data update documents changes in the methods and data sets used in this new global carbon budget and the progress in understanding of the global carbon cycle compared with previous publications of this data set (Le Quéré et al., 2018a, b, 2016, 2015a, b, 2014, 2013).

global carbon budget 2019↗
DOE OSTI2026

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↗
NASA NTRS2018

Removal of Carbon Dioxide from Gas Mixtures Using Ion-Exchanged Silicoaluminophosphates

Na.sup.+-SAPO-34 sorbents were ion-exchanged with several individual metal cations for CO.sub.2 absorption at different temperatures (273-348 K) and pressures (<1 atm). In general, the overall adsorption performance of the exchanged materials increased as follows: Ce.sup.3+<Ti.sup.3+<Mg.sup.2+<Ca.sup.2+<Ag.sup.+<Na.sup.+&- lt;Sr.sup.2+. The strontium exchanged materials excelled at low-pressure ranges, exhibiting very sharp isotherms slopes at all temperatures. The Sr.sup.2+ species were responsible for the surface strong interaction and the cations were occupying exposed sites (SII') in the materials Chabazite cages. All the sorbent materials exhibited higher affinity for CO.sub.2 over the other gases tested (i.e., CH.sub.4, H.sub.2, N.sub.2 and O.sub.2) due to strong ion-quadrupole interactions. Sr.sup.2+-SAPO-34 sorbents are by far the best option for CO.sub.2 removal from CH.sub.4 mixtures, especially at low concentrations.

Hernandez-Maldonado, Arturo J↗
DOE OSTI2021

A Laboratory Corrosion Inhibition Study of Carbon Steel Using 2-Mercaptobenzothiazole (MBT) Under Post-Combustion CO2 Capture Conditions

Corrosion mitigation is an important aspect of amine-based post-combustion carbon dioxide (CO2) capture operations due to the desire to use less expensive but corrosion-vulnerable materials such as low carbon steels in the construction of a capture system. In this study, the corrosion behavior of A106 (grade B) carbon steel with an in-house proprietary amine-based solvent was investigated in a laboratory environment at 80°C using an organic corrosion inhibitor, 2-mercaptobenzothiazole (MBT). The corrosion inhibition mechanism was interpreted by electrochemical methods and surface analyses. The results revealed that the corrosion rates of carbon steel were significantly retarded using MBT. The critical inhibitor concentration was determined to be lie between 10 ppm and 50 ppm under the tested conditions.

Materials Science↗
DOE OSTI2025

Global Carbon Budget 2024

Abstract. Accurate assessment of anthropogenic carbon dioxide (CO2) emissions and their redistribution among the atmosphere, ocean, and terrestrial biosphere in a changing climate is critical to better understand the global carbon cycle, support the development of climate policies, and project future climate change. Here we describe and synthesize datasets and methodologies to quantify the five major components of the global carbon budget and their uncertainties. Fossil CO2 emissions (EFOS) are based on energy statistics and cement production data, while emissions from land-use change (ELUC) are based on land-use and land-use change data and bookkeeping models. Atmospheric CO2 concentration is measured directly, and its growth rate (GATM) is computed from the annual changes in concentration. The global net uptake of CO2 by the ocean (SOCEAN, called the ocean sink) is estimated with global ocean biogeochemistry models and observation-based fCO2 products (fCO2 is the fugacity of CO2). The global net uptake of CO2 by the land (SLAND, called the land sink) is estimated with dynamic global vegetation models. Additional lines of evidence on land and ocean sinks are provided by atmospheric inversions, atmospheric oxygen measurements, and Earth system models. The sum of all sources and sinks results in the carbon budget imbalance (BIM), a measure of imperfect data and incomplete understanding of the contemporary carbon cycle. All uncertainties are reported as ±1σ. For the year 2023, EFOS increased by 1.3 % relative to 2022, with fossil emissions at 10.1 ± 0.5 GtC yr−1 (10.3 ± 0.5 GtC yr−1 when the cement carbonation sink is not included), and ELUC was 1.0 ± 0.7 GtC yr−1, for a total anthropogenic CO2 emission (including the cement carbonation sink) of 11.1 ± 0.9 GtC yr−1 (40.6 ± 3.2 GtCO2 yr−1). Also, for 2023, GATM was 5.9 ± 0.2 GtC yr−1 (2.79 ± 0.1 ppm yr−1; ppm denotes parts per million), SOCEAN was 2.9 ± 0.4 GtC yr−1, and SLAND was 2.3 ± 1.0 GtC yr−1, with a near-zero BIM (−0.02 GtC yr−1). The global atmospheric CO2 concentration averaged over 2023 reached 419.31 ± 0.1 ppm. Preliminary data for 2024 suggest an increase in EFOS relative to 2023 of +0.8 % (−0.2 % to 1.7 %) globally and an atmospheric CO2 concentration increase by 2.87 ppm, reaching 422.45 ppm, 52 % above the pre-industrial level (around 278 ppm in 1750). Overall, the mean of and trend in the components of the global carbon budget are consistently estimated over the period 1959–2023, with a near-zero overall budget imbalance, although discrepancies of up to around 1 GtC yr−1 persist for the representation of annual to semi-decadal variability in CO2 fluxes. Comparison of estimates from multiple approaches and observations shows the following: (1) a persistent large uncertainty in the estimate of land-use change emissions, (2) low agreement between the different methods on the magnitude of the land CO2 flux in the northern extra-tropics, and (3) a discrepancy between the different methods on the mean ocean sink. This living-data update documents changes in methods and datasets applied to this most recent global carbon budget as well as evolving community understanding of the global carbon cycle. The data presented in this work are available at https://doi.org/10.18160/GCP-2024 (Friedlingstein et al., 2024).

Friedlingstein, Pierre (ORCID:0000000333094739)↗
NASA NTRS2010

Portable Dew Point Mass Spectrometry System for Real-Time Gas and Moisture Analysis

A portable instrument incorporates both mass spectrometry and dew point measurement to provide real-time, quantitative gas measurements of helium, nitrogen, oxygen, argon, and carbon dioxide, along with real-time, quantitative moisture analysis. The Portable Dew Point Mass Spectrometry (PDP-MS) system comprises a single quadrupole mass spectrometer and a high vacuum system consisting of a turbopump and a diaphragm-backing pump. A capacitive membrane dew point sensor was placed upstream of the MS, but still within the pressure-flow control pneumatic region. Pressure-flow control was achieved with an upstream precision metering valve, a capacitance diaphragm gauge, and a downstream mass flow controller. User configurable LabVIEW software was developed to provide real-time concentration data for the MS, dew point monitor, and sample delivery system pressure control, pressure and flow monitoring, and recording. The system has been designed to include in situ, NIST-traceable calibration. Certain sample tubing retains sufficient water that even if the sample is dry, the sample tube will desorb water to an amount resulting in moisture concentration errors up to 500 ppm for as long as 10 minutes. It was determined that Bev-A-Line IV was the best sample line to use. As a result of this issue, it is prudent to add a high-level humidity sensor to PDP-MS so such events can be prevented in the future.

Arkin, C.↗
DOE OSTI2025

Sulfide stress tolerance as a controller of methane production in temperate wetlands

Abstract Wetlands are a major source of methane emissions and contribute to the observed increase in atmospheric methane over the last 20 years. Methane production in wetlands is the final step of carbon decomposition performed by anaerobic archaea. Although hydrogen/carbon dioxide and acetate are the substrates most often attributed to methanogenesis, other substrates—such as methylated compounds—may additionally play important roles in driving methane production in wetland systems. Here we conducted mesocosm experiments combined with genome-resolved metatranscriptomics to investigate the impact of diverse methanogenic substrate amendment on methanogenesis in two high methane-emitting wetlands with distinct geochemistry, termed P7 and P8. Methanol amendment resulted in high methane production at both sites, whereas acetate and formate amendment only stimulated methanogenesis in P7 mesocosms, where aqueous sulfide concentrations were lower. In P7 sediments, formate amendment fueled acetogenic microbes that produced acetate, which was subsequently utilized by acetoclastic methanogens. In contrast to expression profiles in P7 mesocosms, active methylotrophic methanogen genomes from P8 showed increased expression of genes related to membrane remodeling and DNA damage repair, indicative of stress tolerance mechanisms to counter sulfide toxicity. Methylotrophic methanogenesis generates higher free energy yields than acetoclastic methanogenesis, which likely enables allocation of more energy toward stress responses. These findings contribute to the growing body of literature highlighting methylotrophic methanogenesis as an important methane production pathway in wetlands. By using less competitive substrates like methanol that provide greater energy yields, methylotrophic methanogens may invest in physiological strategies that provide competitive advantages across a range of environmental stresses.

Environmental Sciences & Ecology↗
DOE OSTI2022

Global Carbon Budget 2021

Abstract. Accurate assessment of anthropogenic carbon dioxide (CO2) emissions and their redistribution among the atmosphere, ocean, and terrestrial biosphere in a changing climate is critical to better understand the global carbon cycle, support the development of climate policies, and project future climate change. Here we describe and synthesize datasets and methodology to quantify the five major components of the global carbon budget and their uncertainties. Fossil CO2 emissions (EFOS) are based on energy statistics and cement production data, while emissions from land-use change (ELUC), mainly deforestation, are based on land use and land-use change data and bookkeeping models. Atmospheric CO2 concentration is measured directly, and its growth rate (GATM) is computed from the annual changes in concentration. The ocean CO2 sink (SOCEAN) is estimated with global ocean biogeochemistry models and observation-based data products. The terrestrial CO2 sink (SLAND) is estimated with dynamic global vegetation models. The resulting carbon budget imbalance (BIM), the difference between the estimated total emissions and the estimated changes in the atmosphere, ocean, and terrestrial biosphere, is a measure of imperfect data and understanding of the contemporary carbon cycle. All uncertainties are reported as ±1σ. For the first time, an approach is shown to reconcile the difference in our ELUC estimate with the one from national greenhouse gas inventories, supporting the assessment of collective countries' climate progress. For the year 2020, EFOS declined by 5.4 % relative to 2019, with fossil emissions at 9.5 ± 0.5 GtC yr−1 (9.3 ± 0.5 GtC yr−1 when the cement carbonation sink is included), and ELUC was 0.9 ± 0.7 GtC yr−1, for a total anthropogenic CO2 emission of 10.2 ± 0.8 GtC yr−1 (37.4 ± 2.9 GtCO2). Also, for 2020, GATM was 5.0 ± 0.2 GtC yr−1 (2.4 ± 0.1 ppm yr−1), SOCEAN was 3.0 ± 0.4 GtC yr−1, and SLAND was 2.9 ± 1 GtC yr−1, with a BIM of −0.8 GtC yr−1. The global atmospheric CO2 concentration averaged over 2020 reached 412.45 ± 0.1 ppm. Preliminary data for 2021 suggest a rebound in EFOS relative to 2020 of +4.8 % (4.2 % to 5.4 %) globally. Overall, the mean and trend in the components of the global carbon budget are consistently estimated over the period 1959–2020, but discrepancies of up to 1 GtC yr−1 persist for the representation of annual to semi-decadal variability in CO2 fluxes. Comparison of estimates from multiple approaches and observations shows (1) a persistent large uncertainty in the estimate of land-use changes emissions, (2) a low agreement between the different methods on the magnitude of the land CO2 flux in the northern extra-tropics, and (3) a discrepancy between the different methods on the strength of the ocean sink over the last decade. This living data update documents changes in the methods and datasets used in this new global carbon budget and the progress in understanding of the global carbon cycle compared with previous publications of this dataset (Friedlingstein et al., 2020, 2019; Le Quéré et al., 2018b, a, 2016, 2015b, a, 2014, 2013). The data presented in this work are available at https://doi.org/10.18160/gcp-2021 (Friedlingstein et al., 2021).

Friedlingstein, Pierre (ORCID:0000000333094739)↗
DOE OSTI2022

Global Carbon Budget 2022

Abstract. Accurate assessment of anthropogenic carbon dioxide (CO2) emissions and their redistribution among the atmosphere, ocean, and terrestrial biosphere in a changing climate is critical to better understand the global carbon cycle, support the development of climate policies, and project future climate change. Here we describe and synthesize data sets and methodologies to quantify the five major components of the global carbon budget and their uncertainties. Fossil CO2 emissions (EFOS) are based on energy statistics and cement production data, while emissions from land-use change (ELUC), mainly deforestation, are based on land use and land-use change data and bookkeeping models. Atmospheric CO2 concentration is measured directly, and its growth rate (GATM) is computed from the annual changes in concentration. The ocean CO2 sink (SOCEAN) is estimated with global ocean biogeochemistry models and observation-based data products. The terrestrial CO2 sink (SLAND) is estimated with dynamic global vegetation models. The resulting carbon budget imbalance (BIM), the difference between the estimated total emissions and the estimated changes in the atmosphere, ocean, and terrestrial biosphere, is a measure of imperfect data and understanding of the contemporary carbon cycle. All uncertainties are reported as ±1σ. For the year 2021, EFOS increased by 5.1 % relative to 2020, with fossil emissions at 10.1 ± 0.5 GtC yr−1 (9.9 ± 0.5 GtC yr−1 when the cement carbonation sink is included), and ELUC was 1.1 ± 0.7 GtC yr−1, for a total anthropogenic CO2 emission (including the cement carbonation sink) of 10.9 ± 0.8 GtC yr−1 (40.0 ± 2.9 GtCO2). Also, for 2021, GATM was 5.2 ± 0.2 GtC yr−1 (2.5 ± 0.1 ppm yr−1), SOCEAN was 2.9 ± 0.4 GtC yr−1, and SLAND was 3.5 ± 0.9 GtC yr−1, with a BIM of −0.6 GtC yr−1 (i.e. the total estimated sources were too low or sinks were too high). The global atmospheric CO2 concentration averaged over 2021 reached 414.71 ± 0.1 ppm. Preliminary data for 2022 suggest an increase in EFOS relative to 2021 of +1.0 % (0.1 % to 1.9 %) globally and atmospheric CO2 concentration reaching 417.2 ppm, more than 50 % above pre-industrial levels (around 278 ppm). Overall, the mean and trend in the components of the global carbon budget are consistently estimated over the period 1959–2021, but discrepancies of up to 1 GtC yr−1 persist for the representation of annual to semi-decadal variability in CO2 fluxes. Comparison of estimates from multiple approaches and observations shows (1) a persistent large uncertainty in the estimate of land-use change emissions, (2) a low agreement between the different methods on the magnitude of the land CO2 flux in the northern extratropics, and (3) a discrepancy between the different methods on the strength of the ocean sink over the last decade. This living data update documents changes in the methods and data sets used in this new global carbon budget and the progress in understanding of the global carbon cycle compared with previous publications of this data set. The data presented in this work are available at https://doi.org/10.18160/GCP-2022 (Friedlingstein et al., 2022b).

54 ENVIRONMENTAL SCIENCES↗
NASA NTRS1989

Respiration rate in maize roots is related to concentration of reduced nitrogen and proliferation of lateral roots

The relationship between specific rate of respiration (respiration rate per unit root dry weight) and concentration of reduced nitrogen was examined for maize (Zea mays L.) roots. Plants with 2 primary nodal root axes were grown for 8 days in a split-root hydroponic system in which NO3- was supplied to both axes at 1.0 mol m-3, to one axis at 1.0 mol m-3 and the other axis at 0.0 mol m-3, or to both axes at 0.0 mol m-3. Respiration rates and root characteristics were measured at 2-day intervals. Specific rate of respiration was positively correlated in a nonlinear relationship with concentration of reduced nitrogen. The lowest specific rates of respiration occurred when neither axis received exogenous NO3- and the concentration of reduced nitrogen in the axes was less than 9 mg g-1. The greatest rates occurred in axes that were actively absorbing NO3- and contained more than 35 mg g-1 of reduced nitrogen. At 23 mg g-1 of reduced nitrogen, below which initiation of lateral branches was decreased by 30-50%, specific rate of respiration was 17% greater for roots actively absorbing NO3- than for roots not absorbing NO3-. Increases in specific rate of respiration associated with concentrations of reduced nitrogen greater than 23 mg g-1 were concluded to be attributable primarily to proliferation of lateral branches.

Non-NASA Center↗
DOE OSTI2025

Carbon Mineralization of Sulfate Wastes Containing Pb: Synchrotron Pb M3-Edge XANES Analysis of Simultaneous Heavy Metal and Carbon Sequestration

Sulfate wastes are produced in large quantities and contain toxic heavy metals such as lead (Pb), posing environmental risks. Because of favorable solubility differences, these wastes can be repurposed for engineered carbon dioxide (CO 2 ) sequestration. Understanding the fate and mobility of heavy metals during this process is important. This study focuses on Pb and the effect of zinc (Zn) on Pb in carbon mineralization. Synthesized gypsum was treated with a carbonate-rich solution at pH 11.5 to convert the sulfates to carbonates. Aqueous solutions and mineral solids were analyzed. Synchrotron-based micro-X-ray fluorescence and a novel application of Pb M3-edge X-ray absorption near-edge structure provided detailed insights into Pb distribution and mineral forms. Results showed significant reductions in aqueous Pb and Zn concentrations, indicating effective metal sequestration. Carbon mineralization transformed Pb from soluble anglesite (PbSO 4 ) into insoluble cerussite (PbCO 3 ) and hydrocerussite (Pb 3 (CO 3 ) 2 (OH) 2 ). Pb primarily precipitated onto calcium carbonate surfaces through surface-mediated precipitation reactions. While the presence of Zn modified crystallization dynamics, it did not impede Pb sequestration and potentially enhanced surface reactivity, facilitating greater Pb immobilization. These findings highlight carbon mineralization as a sustainable approach to immobilize toxic metals in sulfate wastes while advancing CO 2 sequestration efforts.

54 ENVIRONMENTAL SCIENCES↗