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At least 1,045 records · Page 58
All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

SPRUCE Warming Promotes the Use of Organic Matter as an Electron Acceptor in a Peatland: Supporting Data

These data are provided in support of the publication: Warming Promotes the Use of Organic Matter as an Electron Acceptor in a Peatland (Rush et al., 2021). Rush et al. (2021) reported on the effect of temperature on microbial organic matter reduction at the SPRUCE study site and S1 bog. Specifically, electron shuttling capacity (ESC), CH4 production, CO2 production, and acetate concentration were measured to explore both direct and indirect (through changes in soil quality and water-table level) effects of warming on microbial activity. Samples were collected in the summer of 2016 and 2017 depending on the experiment. This dataset contains five files in comma separated (*.csv) format. The SPRUCE Experiment Site is located in a Picea mariana [black spruce] Sphagnum spp. bog forest in northern Minnesota, 40 km north of Grand Rapids, in the USDA Forest Service Marcell Experimental Forest (MEF). This ecosystem, which is located at the southern margin of the boreal forest, is considered especially vulnerable to climate change and anticipated to be near its tipping point.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2018

History of chemically and radiatively important atmospheric gases from the Advanced Global Atmospheric Gases Experiment (AGAGE)

In the ALE/GAGE/AGAGE global network program, continuous high frequency gas chromatographic measurements of four biogenic/anthropogenic gases (methane, CH4; nitrous oxide, N2O; hydrogen, H; and carbon monoxide, CO) and several anthropogenic gases that contribute to stratospheric ozone destruction and/or to the greenhouse effect have been carried out at five globally distributed sites for several years. The program, which began in 1978, is divided into three parts associated with three changes in instrumentation: the Atmospheric Lifetime Experiment (ALE), which used Hewlett Packard HP5840 gas chromatographs; the Global Atmospheric Gases Experiment (GAGE), which used HP5880 gas chromatographs; and the present Advanced GAGE (AGAGE). AGAGE uses two types of instruments: a gas chromatograph with multiple detectors (GC-MD), and a gas chromatograph with mass spectrometric analysis (GC-MS). Beginning in January 2004, an improved cryogenic preconcentration system (Medusa) replaced the absorption-desorption module in the GC-MS systems at Mace Head and Cape Grim; this provided improved capability to measure a broader range of volatile perfluorocarbons with high global warming potentials. More information may be found at the AGAGE home page: https://agage.mit.edu/instruments.In the latest update (Agage_gcmd_gcms_data_2020_07_04_tar.gz), all AGAGE data up to Sep. 2019 is included. A new compound, PFC-318, is also included in this update. For all released compounds and scales used by the AGAGE network, please see the "AGAGE_scale_2020_v2.pdf" file (included in "Agage_gcmd_gcms_data_2020_07_04_tar.gz").

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2019

Soil Mesocosm CO2 Emissions after 13C-glucose Addition, Soil Physical and Chemical Characteristics, and Microbial Biomass, Barrow, Alaska, 2014-2016

Measurements made from a 2014-2016 field glucose addition experiment. Dataset includes measurements of surface trace gas emissions (Delta13C of ecosystem respiration and source-partitioned surface CO2 flux, CH4 flux, and GPP), soil profile information (concentrations of carbon, nitrogen, and soil microbial biomass carbon, Delta13C of soil organic matter and microbial biomass, gravimetric water content, and bulk density), soil mineral nitrogen availability, and field-measured soil temperature, air temperature and soil moisture. Experiment was conducted in a region of high-centered polygons on the BEO. Data will be available Summer 2018.

54 ENVIRONMENTAL SCIENCES↗
NASA NTRS2012

Methane from the Tropospheric Emission Spectrometer (TES)

TES V5 CH4 captures latitudinal gradients, regional variability and interannual variation in the free troposphere. V5 joint retrievals offer improved sensitivity to lower troposphere. Time series extends from 2004 to present. V5 reprocessing in progress. Upper tropospheric bias. Mitigated by N2O correction. Appears largely spatially uniform, so can be corrected. How to relate free-tropospheric values to surface emissions.

methane gas (CH4)↗
NASA NTRS2012

CARVE: The Carbon in Arctic Reservoirs Vulnerability Experiment

The Carbon in Arctic Reservoirs Vulnerability Experiment (CARVE) is a NASA Earth Ventures (EV-1) investigation designed to quantify correlations between atmospheric and surface state variables for the Alaskan terrestrial ecosystems through intensive seasonal aircraft campaigns, ground-based observations, and analysis sustained over a 5-year mission. CARVE bridges critical gaps in our knowledge and understanding of Arctic ecosystems, linkages between the Arctic hydrologic and terrestrial carbon cycles, and the feedbacks from fires and thawing permafrost. CARVE's objectives are to: (1) Directly test hypotheses attributing the mobilization of vulnerable Arctic carbon reservoirs to climate warming; (2) Deliver the first direct measurements and detailed maps of CO2 and CH4 sources on regional scales in the Alaskan Arctic; and (3) Demonstrate new remote sensing and modeling capabilities to quantify feedbacks between carbon fluxes and carbon cycle-climate processes in the Arctic (Figure 1). We describe the investigation design and results from 2011 test flights in Alaska.

Arctic Carbon Cycle↗
NASA NTRS2015

Geology of Pluto and Charon Overview

Pluto's surface was found to be remarkably diverse in terms of its range of landforms, terrain ages, and inferred geological processes. There is a latitudinal zonation of albedo. The conspicuous bright albedo heart-shaped feature informally named Tombaugh Regio is comprised of several terrain types. Most striking is Texas-sized Sputnik Planum, which is apparently level, has no observable craters, and is divided by polygons and ovoids bounded by shallow troughs. Small smooth hills are seen in some of the polygon-bounding troughs. These hills could either be extruded or exposed by erosion. Sputnik Planum polygon/ovoid formation hypotheses range from convection to contraction, but convection is currently favored. There is evidence of flow of plains material around obstacles. Mountains, especially those seen south of Sputnik Planum, exhibit too much relief to be made of CH4, CO, or N2, and thus are probably composed of H2O-ice basement material. The north contact of Sputnik Planum abuts a scarp, above which is heavily modified cratered terrain. Pluto's large moon Charon is generally heavily to moderately cratered. There is a mysterious structure in the arctic. Charon's surface is crossed by an extensive system of rift faults and graben. Some regions are smoother and less cratered, reminiscent of lunar maria. On such a plain are large isolated block mountains surrounded by moats. At this conference we will present highlights of the latest observations and analysis. This work was supported by NASA's New Horizons project

Sputnik Planum↗
NASA NTRS2017

Bladed Terrain on Pluto: Possible Origins and Evolution

We conclude that Bladed Terrain on Pluto is a deposit of massive CH4, which preferentially precipitates at high elevations, and has since its initial formation, undergone episodes of sublimation erosion that has given this deposit its characteristic texture.

Bladed Terrain↗
DOE OSTI2014

Organic Matter Transformation in the Peat Column at Marcell Experimental Forest: Humification and Vertical Stratification

A large-scale ecosystem manipulation (Spruce and Peatland Responses under Climatic and Environmental Change, SPRUCE) is being constructed in the Marcell Experimental Forest, Minnesota, USA, to determine the effects of climatic forcing on ecosystem processes in northern peatlands. Prior to the initiation of the manipulation, we characterized the solid-phase peat to a depth of 2 meters using a variety of techniques, including peat C:N ratios, 13C and 15N isotopic composition, Fourier Transform Infrared (FT IR), and 13C Nuclear Magnetic Resonance spectroscopy (13C NMR). FT IR determined peat humification-levels increased rapidly between and 75 cm, indicating a highly reactive zone. We observed a rapid drop in the abundance of O-alkyl-C, carboxyl-C, and other oxygenated functionalities within this zone and a concomitant increase in the abundance of alkyl- and nitrogen-containing compounds. Below 75-cm, minimal change was observed except that aromatic functionalities accumulated with depth. Incubation studies revealed the highest methane production rates and greatest CH4:CO2 ratios within this and 75 cm zone. Hydrology and surface vegetation played a role in belowground carbon cycling. Radiocarbon signatures of microbial respiration products in deeper porewaters resembled the signatures of dissolved organic carbon rather than solid phase peat, indicating that more recently photosynthesized organic matter fueled the bulk of subsurface microbial respiration. Oxygen-containing functionalities, especially O-alkyl-C, appear to serve as an excellent proxy for soil decomposition rate, and in addition should be a sensitive indicator of the response of the solid phase peat to the climatic manipulation.

FT-IR spectroscopy↗
DOE OSTI2015

Top-down estimate of methane emissions in California using a mesoscale inverse modeling technique: The South Coast Air Basin

Methane (CH 4 ) is the primary component of natural gas and has a larger global warming potential than CO 2 . Some recent top-down studies based on observations showed CH 4 emissions in California's South Coast Air Basin (SoCAB) were greater than those expected from population-apportioned bottom-up state inventories. In this study, we quantify CH 4 emissions with an advanced mesoscale inverse modeling system at a resolution of 8 km × 8 km, using aircraft measurements in the SoCAB during the 2010 Nexus of Air Quality and Climate Change campaign to constrain the inversion. To simulate atmospheric transport, we use the FLEXible PARTicle-Weather Research and Forecasting (FLEXPART-WRF) Lagrangian particle dispersion model driven by three configurations of the Weather Research and Forecasting (WRF) mesoscale model. We determine surface fluxes of CH 4 using a Bayesian least squares method in a four-dimensional inversion. Simulated CH4 concentrations with the posterior emission inventory achieve much better correlations with the measurements (R2 = 0.7) than using the prior inventory (U.S. Environmental Protection Agency's National Emission Inventory 2005, R 2 = 0.5). The emission estimates for CH 4 in the posterior, 46.3 ± 9.2 Mg CH 4 /h, are consistent with published observation-based estimates. Changes in the spatial distribution of CH 4 emissions in the SoCAB between the prior and posterior inventories are discussed. Missing or underestimated emissions from dairies, the oil/gas system, and landfills in the SoCAB seem to explain the differences between the prior and posterior inventories. Furthermore, we estimate that dairies contributed 5.9 ± 1.7 Mg CH 4 /h and the two sectors of oil and gas industries (production and downstream) and landfills together contributed 39.6 ± 8.1 Mg CH 4 /h in the SoCAB.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2016

Relative importance between biogeochemical and biogeophysical effects in regulating terrestrial ecosystem-climate feedback in northern high latitudes

Warming-induced changes in structures and functions of northern terrestrial ecosystems (NTEs), including their regulation on terrestrial biogeochemistry and surface energy balance, may exert positive or negative feedback to the climate system. However, the relative importance among these biogeochemical and biogeophysical feedback is not well understood. Here we use a terrestrial ecosystem model to quantify spatially explicit ecosystem-climate feedback over NTEs (north of 50°N) under four climate change scenarios from 2010 to 2100, including biogeochemical feedback from climate-induced changes in net CH4 exchanges (NME) and net CO 2 exchanges (NCE) and biogeophysical feedback from changes in surface energy partitioning associated with snow cover and vegetation biomass dynamics. Our results indicate that (1) biogeochemical and biogeophysical feedback are attributed more to the changes in NME and snow cover dynamics, respectively; (2) net biogeophysical feedback is much larger than net biogeochemical feedback; (3) NTEs will cause a net positive radiative forcing of 0.04–0.26 Wm -2 between 2010 and 2100. Our findings support the notion that NTEs will exert positive net climate feedback; however, our estimation of positive net biogeochemical feedback including NME- and NCE-induced effects is contrary to previous studies showing negative net biogeochemical feedback including NCE-induced effect only. In conclusion, this study highlights the importance of NME-induced biogeochemical effect in regulating ecosystem-climate feedback in NTEs and implies that previous studies without considering NME-induced effect might have underestimated the intensity of total terrestrial feedback to the climate system.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2026

A Global Methane Observation System to Reduce Uncertainty for Anthropogenic and Natural Sources and Sinks for Detecting and Attributing Climate Feedbacks

Atmospheric methane (CH4) concentrations are accelerating global warming as net emissions increase. Observing systems that quantify sources remain too sparse and fragmented to detect trends—especially in remote regions where climate‐driven natural emissions may be rising. We provide a framework for quantifying uncertainty reductions through the implementation of a global ecosystem‐methane observing system designed to: (i) substantially lower uncertainty in sectoral and regional emissions, (ii) separate co‐occurring anthropogenic and natural fluxes, and (iii) trend detection at regional scales to verify mitigation progress and provide early warning of natural feedbacks. Using bottom‐up inventories and process‐model ensembles for 2014–2023, we show that anthropogenic emissions remain uncertain by ∼32% globally, while natural sources—tropical and boreal‐arctic wetlands, fires, and inland waters—carry far larger uncertainties (+ 70%) and trend uncertainties reaching ∼200%. Additional observations must match spatial emission structure to increase observability of emissions: high‐resolution satellite constellations for point sources combined with expanded flux networks and wetland mapping for diffuse sources, and denser ground‐based atmospheric column measurements to restore observability in under‐sampled tropics and high latitudes. Notional analyses indicate that targeted additions of flux towers and ∼20 in situ atmospheric column concentration instruments per key tropical region could reduce continental‐scale uncertainties at modest cost. Conceptual illustration of a Global Ecosystem Methane Observing System (GEM‐OS) integrating satellites, aircraft, atmospheric networks, and ecosystem measurements to quantify methane emissions from anthropogenic and natural sources. The multi‐scale observing framework improves source attribution, reduces uncertainty in regional methane budgets, and enables early detection of climate‐driven feedbacks from wetlands, fires, permafrost, agriculture, and fossil‐fuel emissions.

Ciais, P↗
DOE OSTI2022

CO2 Hydrogenation to Hydrocarbons over Fe/BZY Catalysts

This manuscript reports a CO2 hydrogenation process in a catalytic laboratory-scale packed-bed reactor using an Fe/BZY15 (BaZr0.8Y0.15O3-d) catalyst to form hydrocarbons (e.g., CH4, C2+) at elevated pressure of 30 bar and temperatures in the range 270 = T = 375 degrees C. The effects of temperature, feed composition (i.e., CO2/H2 ratio, and residence time (i.e., Weight Hourly Space Velocity (WHSV) are studied to understand the relationship between CO2 conversion and carbon selectivity. Catalyst characterization elucidates the relationships between the catalyst structure, surface adsorbates, and reaction pathways. Thermodynamic analyses guide the experimental conditions and assist interpreting results. While the feed composition and temperature influence the product distribution, the results suggest that the higher-carbon (C2+) selectivity and yield depend strongly on residence time. The results suggest that the CO2 hydrogenation reaction pathway is similar to Fischer-Tropsch (FT) synthesis. The reaction begins with CO2 activation to form CO, followed by chain-growth reactions similar to the FT process. The CO2 activation depends on the redox activity of the catalyst. However, the carbon chain growth depends primarily on the residence time. as is the case for the FT synthesis, high residence time (on the orders of hours) is required to achieve high C2+ yield. For such high residence times, catalyst-fouling carbon deposition can be problematic. The coke-resistant BZY15 catalyst support contributes to the catalytic activity and enables a coke-free operation for more than 100 h time-on-stream.

bi-functional catalyst↗
DOE OSTI2013

Computational approaches to the chemical conversion of carbon dioxide

The conversion of CO2 into fuels and chemicals is viewed as an attractive route for controlling the atmospheric concentration of this greenhouse gas and recycling it, but its industrial application is limited by the low selectivity and activity of the current catalysts. Theoretical modeling, in particular density-functional theory (DFT) simulations, provides a powerful and effective tool to discover chemical reaction mechanisms and design new catalysts for the chemical conversion of CO2, overcoming the repetitious and time/labor consuming trial-and-error experimental processes. In this article we give a comprehensive survey of recent advances on mechanism determination by DFT calculations for the catalytic hydrogenation of CO2 into CO, CH4, CH3OH, and HCOOH, and CO2 methanation, as well as the photo- and electrochemical reduction of CO2. DFT-guided design procedures of new catalytic systems are also reviewed, and challenges and perspectives in this field are outlined.

Cheng, Daojian↗
DOE OSTI2017

Using greenhouse gas fluxes to define soil functional types

Soils provide key ecosystem services and directly control ecosystem functions; thus, there is a need to define the reference state of soil functionality. Most common functional classifications of ecosystems are vegetation-centered and neglect soil characteristics and processes. We propose Soil Functional Types (SFTs) as a conceptual approach to represent and describe the functionality of soils based on characteristics of their greenhouse gas (GHG) flux dynamics. We used automated measurements of CO2, CH4 and N2O in a forested area to define SFTs following a simple statistical framework. This study supports the hypothesis that SFTs provide additional insights on the spatial variability of soil functionality beyond information represented by commonly measured soil parameters (e.g., soil moisture, soil temperature, litter biomass). We discuss the implications of this framework at the plot-scale and the potential of this approach at larger scales. This approach is a first step to provide a framework to define SFTs, but a community effort is necessary to harmonize any global classification for soil functionality. A global application of the proposed SFT framework will only be possible if there is a community-wide effort to share data and create a global database of GHG emissions from soils.

Petrakis, Sandra↗
DOE OSTI2019

Simulation of Gas Production from Multilayered Hydrate-Bearing Media with Fully Coupled Flow, Thermal, Chemical and Geomechanical Processes Using TOUGH + Millstone. Part 1: Numerical Modeling of Hydrates

TOUGH + Millstone has been developed for the analysis of coupled flow, thermal and geomechanical processes associated with the formation and/or dissociation of CH4-hydrates in geological media. It is composed of two constituent codes: (a) a significantly enhanced version of the TOUGH + HYDRATE simulator, V2.0, that accounts for all known flow, physical, thermodynamic and chemical processes associated with the behavior of hydrate-bearing systems undergoing changes and includes the most recent advances in the description of the system properties, coupled seamlessly with (b) Millstone V1.0, a new code that addresses the conceptual, computational and mathematical shortcomings of earlier codes used to describe the geomechanical response of these systems. The capabilities of TOUGH + Millstone are demonstrated in the simulation and analysis of the system flow, thermal and geomechanical behavior during gas production from a realistic complex offshore hydrate deposit. In the first paper of this series, we discuss the physics underlying the T + H hydrate simulator, the constitutive relationships describing the physical, chemical (equilibrium and kinetic) and thermal processes, the states of the CH 4 + H 2 O system and the sources of critically important data, as well as the mathematical approaches used for the development of the of mass and energy balance equations and their solution. Finally, we provide verification examples of the hydrate code against numerical results from the simulation of laboratory and field experiments.

58 GEOSCIENCES↗
DOE OSTI2013

Ethanol Steam Reforming on Co/CeO2: The Effect of ZnO Promoter

A series of ZnO promoted Co/CeO2 catalysts were synthesized and characterized using XRD, TEM, H2-TPR, CO chemisorption, O2-TPO, IR-Py, and CO2-TPD. The effects of ZnO on the catalytic performances of Co/CeO2 were studied in ethanol steam reforming. It was found that the addition of ZnO facilitated the oxidation of Co0 via enhanced oxygen mobility of the CeO2 support which decreased the activity of Co/CeO2 in C–C bond cleavage of ethanol. 3 wt% ZnO promoted Co/CeO2 exhibited minimum CO and CH4 selectivity and maximum CO2 selectivity. This resulted from the combined effects of the following factors with increasing ZnO loading: (1) enhanced oxygen mobility of CeO2 facilitated the oxidation of CHx and CO to form CO2; (2) increased ZnO coverage on CeO2 surface reduced the interaction between CHx/CO and Co/CeO2; and (3) suppressed CO adsorption on Co0 reduced CO oxidation rate to form CO2. In addition, the addition of ZnO also modified the surface acidity and basicity of CeO2, which consequently affected the C2–C4 product distributions.

CeO2↗
DOE OSTI2014

Atomic and Molecular Adsorption on Re(0001)

Using periodic, self-consistent density functional theory calculations, the adsorption of several atomic (H, S, N, O and C) and molecular (CO2, N2, NH3, HCN, CO and NO) species and molecular fragments (NH2, NH, CN, CNH2, HNO, NOH, CH3, CH2, CH and OH) on the (0001) facet of rhenium at a coverage of 0.25 ML has been studied. Preferred binding sites with their corresponding binding energy and deformation energy of the surface, as well as an estimated diffusion barrier of each species have been determined. Atomic species and molecular fragments tend to bind to threefold sites, whereas molecular species tend to bind to top sites. The binding strength, with respect to the corresponding gas phase species and in increasing order for all species studied, is: CO2 < N2 < NH3 < CO < CH3 < HCN < NO < H < NH2 < OH < CH2 < CNH2 < CN < HNO < NH < NOH < S < N < O < CH < C. The vibrational frequencies of all species in their most energetically favorable adsorbed configuration have been calculated. Finally, the thermochemistry of adsorption and decomposition of NO, NO + H, NH3, N2, CO2, CO and CH4 on Re(0001) has been analyzed.

Environmental Molecular Sciences Laboratory↗
DOE OSTI2023

Carbon-Assisted, Continuous Syngas Production in a Chemical Looping Scheme

In the current energy and environment scenario, it is imperative to develop energy efficient routes for chemical manufacturing that also pave the way for mitigation of greenhouse gas emissions. This work presents an efficient pathway for continuous syngas production via a chemical looping conversion of the two most potent greenhouse gases—CH 4 , and CO 2 . The well-known dry-reforming process of converting CH 4 , and CO 2 to syngas is energy-intensive and suffers from catalyst deactivation. The chemical looping approach, on the other hand, provides avenues for mitigating catalyst deactivation and enabling improved energy efficiency. The key to such process enhancements lies in the intricate structure–function relationships of the catalyst and its correlation to the process variables. We present the reduction and oxidation characteristics of 5 wt.% Ni/Ce 1-x Zr x O 2 -based catalysts (x = 0, 0.4, and 0.625). We demonstrate low temperature CH4 activation over Ni-promoted samples as opposed to pure Ce 1-x Zr x O 2 . Moreover, our results depict an optimum regeneration of these catalysts when oxidized by CO 2 , and H 2 O, which allows for chemical looping operation of steam reforming of methane as well. Process variables were tuned to optimize the CH 4 conversion (over 80%), and H 2 /CO ratio at 650 °C. The critical surface reactions—carbon accumulation and gasification, and thermocatalytic CO 2 splitting were investigated to elucidate the dynamic nature of the catalyst surface. In conclusion, the impact of this work lies in showcasing the opportunities to design chemical looping reactors for energy efficient syngas production from waste greenhouse gases.

25 ENERGY STORAGE↗