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All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

Life Cycle Analysis of Renewable Natural Gas and Lactic Acid Production from Waste Feedstocks

Producing fuels and chemicals from waste is considered economically favorable, due to low feedstock cost, and environmentally favorable, due to avoided emissions from conventional waste management practices. In this study, we evaluate the life cycle greenhouse gas (GHG) emission reduction benefits of renewable natural gas (RNG) and lactic acid (LA) production from four types of wet waste feedstocks (wastewater sludge, food waste, swine manure, and fats, oil, and grease [FOG]) via anaerobic digestion (AD) and LA fermentation, respectively. RNG can be used as an alternative to fossil natural gas, while LA from waste feedstocks can displace conventional LA production pathways (mainly from corn via fermentation). Providing comprehensive life cycle GHG emissions of the combinations of waste feedstocks and products through different routes helps identify the GHG hotspots and show where emissions savings come from. The results show that the carbon intensities (CIs) of waste-derived RNG and LA are much lower than those of their counterparts. We estimated the life cycle GHG emissions for RNG to be between -146 and 27 g carbon dioxide equivalent (CO2e)/MJ, much lower than the CI of fossil fuels. Waste-derived LA pathways also show substantially lower CIs, ranging from -4.2 to -1.4 kgCO2e/kg LA, compared to the CIs of LA from corn and corn stover (1.2 and 0.3 kgCO2e/kg LA, respectively). We will also discuss that the low CIs of waste-derived products can come from low yields leading to high emission credits. Thus, life cycle analysis results presented per weight of treated waste can be used to support decisions about which waste feedstocks and products are to be used for sustainable waste valorization. In addition, we found that monetary emission reduction credits can play an important role in driving waste valorization.

29 ENERGY PLANNING, POLICY, AND ECONOMY↗
DOE OSTI2016

Lifecycle analysis of renewable natural gas and hydrocarbon fuels from wastewater treatment plants’ sludge

Wastewater treatment plants (WWTPs) produce sludge as a byproduct when they treat wastewater. In the United States, over 8 million dry tons of sludge are produced annually just from publicly owned WWTPs. Sludge is commonly treated in anaerobic digesters, which generate biogas; the biogas is then largely flared to reduce emissions of methane, a potent greenhouse gas. Because sludge is quite homogeneous and has a high energy content, it is a good potential feedstock for other conversion processes that make biofuels, bioproducts, and power. For example, biogas from anaerobic digesters can be used to generate renewable natural gas (RNG), which can be further processed to produce compressed natural gas (CNG) and liquefied natural gas (LNG). Sludge can be directly converted into hydrocarbon liquid fuels via thermochemical processes such as hydrothermal liquefaction (HTL). Currently, the environmental impacts of converting sludge into energy are largely unknown, and only a few studies have focused on the environmental impacts of RNG produced from existing anaerobic digesters. As biofuels from sludge generate high interest, however, existing anaerobic digesters could be upgraded to technology with more economic potential and more environmental benefits. The environmental impacts of using a different anaerobic digestion (AD) technology to convert sludge into energy have yet to be analyzed. In addition, no studies are available about the direct conversion of sludge into liquid fuels. In order to estimate the energy consumption and greenhouse gas (GHG) emissions impacts of these alternative pathways (sludge-to-RNG and sludge-to-liquid), this study performed a lifecycle analysis (LCA) using the Greenhouse gases, Regulated Emissions, and Energy use in Transportation (GREET®) model. The energy uses and GHG emissions associated with the RNG and hydrocarbon liquid are analyzed relative to the current typical sludge management case, which consists of a single-stage mesophilic digester with biogas flaring. Along with the alternative HTL process, four types of AD technologies with fuel production—single-stage mesophilic, mesophilic 2-stage, single-stage mesophilic with thermohydrolysis treatment, and mesophilicmesophilic acid/gas phase—are studied. Results show that the sludge-to-CNG pathway via AD and the sludge-to-liquid pathway via HTL reduce GHG emissions consumptions significantly. When we compare the GHG emissions of the alternative fuel production pathways to that of the counterfactual case in terms of the amount of sludge treated, reductions in GHG emissions are 39%–80% and 87% for alternative AD and HTL, respectively. Compared to petroleum gasoline and diesel GHG emission results in terms of MJ, the renewable CNG production pathway via AD and the renewable diesel production pathway via HTL reduce GHG emissions by 193% and 46%, respectively. These large reductions are mainly due to GHG credits from avoiding GHGs under the counterfactual scenario, and/or fertilizer displacement credits. Similarly, reductions in fossil fuel use for sludge-based fuels are huge. However, well-defined counterfactual scenarios are needed because the results of the study depend on the counterfactual scenario, which might vary over time.

03 NATURAL GAS↗
DOE OSTI2017

Lab-scale pyrolysis of the Automotive Shredder Residue light fraction and characterization of tar and solid products

Highlights: • Car fluff was pyrolysed at various temperatures. • Condensable gases (tar) and solid residue obtained were characterized. • Char had low HHV, high metal content and low PAH concentration. • Tar had high HHV and can be used as an alternative fuel. • Toxicity of tar changes with temperature, the greatest contribution is from PCDFs. - Abstract: The general aim of this study is the recovery of Automotive Shredder Residue (ASR). The ASR light fraction, or car fluff, that was collected at an Italian shredding plant was pyrolysed at various temperatures (500–800 °C) in a lab-scale reactor. The condensable gases (tar) and solid residue yields increased with decreasing temperature, and these products were characterized to suggest a potential use to reclaim them. The higher heating value (HHV) of tar was 34–37 MJ/kg, which is comparable with those of fossil fuels. Furthermore, the ash content was low (0.06–4.98%). Thus, tar can be used as an alternative fuel. With this prospect, the concentrations of polychlorinated dibenzodioxins (PCDDs) and polychlorinated dibenzofurans (PCDFs) in tar were determined. The toxicity of tar changes with temperature (1–5 ng I-TEQ/g), and the PCDFs significantly contribute to tar toxicity, which was 75–100% with a maximum of 99.6% at 700 °C. Regarding the characterization of the solid residue, the low HHV (2.4–3.3 MJ/kg) does not make it suitable for energy recovery. Regarding material recovery, we considered its use as a filler in construction materials or a secondary source for metals. It shows a high metal concentration (280,000–395,000 mg/kg), which is similar at different pyrolysis temperatures. At 500 °C, polycyclic aromatic hydrocarbons (PAHs) were not detected in the solid residue, whereas the maximum total PAH concentration (19.41 ng/g, 700 °C) was lower than that in fly ash from MSWI. In conclusion, 500 °C is a suitable pyrolysis temperature to obtain valuable tar and solid residue.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2016

Desalination of brines produced from the geologic storage of carbon dioxide

Geologic carbon dioxide sequestration (GCS) will play a crucial role in limiting anthropogenic greenhouse gas emissions. GCS is the practice of capturing carbon dioxide (CO 2 ) from industrial sources and storing it in subsurface geologic formations, such as saline formations. These saline formations are typified by a porous interconnected rock strata, saturated with saline brine at a depth of >800 m. Because of the large volumes available, storage of CO 2 into deep saline formations with caprock seals and far from exiting faults will be key for long term reductions of anthropogenic CO 2 emissions. The high pressure injection of CO 2 into the subsurface can cause an increase in subsurface pressure. Open and highly porous formations can have CO 2 injected without causing a significant rise in formation pressure; however, closed or low porosity formations are more sensitive to the subsurface injection of CO 2 with regard to subsurface pressure. Such formations would ideally be located near existing fossil fuel power plants or other industrial emitters of CO 2 who would require GCS. In order to reduce the risk of induced seismic activity near minor fault structures, formation pressure management is needed. This will require the extraction of brines from the formation and these brines could be extracted prior to or during GCS. This extraction will maintain or reduce the subsurface pressure and enhance CO 2 storage capacity. The extracted brine can be dewatered/desalinated, becoming both a source of usable water and a concentrated brine which could be either reinjected into a nearby formation, crystallized, or discharged into an evaporation pond. The Department of Energy Office of Fossil Energy’s commitment to studying formation pressure management in GCS has been demonstrated with the recent awarding of $30,000,000 for two Brine Extraction Storage Test (BEST) projects, whose main goal is to develop and validate strategies for managing formation pressure through brine (Martin 2016). A secondary goal of these projects is to develop and demonstrate processes to extract usable water from these high salinity produced brines.

54 ENVIRONMENTAL SCIENCES↗
NASA NTRS2003

Emissions of Trace Gases and Particles from Two Ships in the Southern Atlantic Ocean

Measurements were made of the emissions of particles and gases from two diesel-powered ships in the southern Atlantic Ocean off the coast of Namibia. The measurements are used to derive emission factors from ships of three species not reported previously, namely, black carbon, accumulation-mode particles, and cloud condensation nuclei (CCN), as well as for carbon dioxide, carbon monoxide (CO), methane (CH4), non-methane hydrocarbons, sulfur dioxide (SO2), nitrogen oxides (NOx), and condensation nuclei. The effects of fuel grade and engine power on ship emissions are discussed. The emission factors are combined with fuel usage data to obtain estimates of global annual emissions of various particles and gases from ocean-going ships. Global emissions of black carbon, accumulation- mode particles, and CCN from ocean-going ships are estimated to be 19-26 Gg yr(sup -1), (4.4-6.1) x 10(exp 26) particles yr(sup -1), and (1.0-1.5) x l0(exp 26) particles yr(sup -1), respectively. Black carbon emissions from ocean-going ships are approximately 0.2% of total anthropogenic emissions. Emissions of NOx and SO2 from ocean-going ships are approximately 10-14% and approximately 3-4%, respectively, of the total emissions of these species from the burning of fossil fuels, and approximately 40% and approximately 70%, respectively, of the total emissions of these species from the burning of biomass. Global annual emissions of CO and CH4 from ocean-going ships are approximately 2% and approximately 2-5%, respectively, of natural oceanic emissions of these species.

Sinha, Parikhit↗
DOE OSTI2021

Renewable energy and biological conservation in a changing world

Without a shift to renewable energy sources, climate change will have adverse effects on many terrestrial and aquatic species. On the other hand, replacing fossil fuels with renewable energy will have different effects on wildlife, some negative. To protect biota, while navigating the complexities surrounding the transition to renewable energy, will require sharing knowledge between energy experts and wildlife experts, as well as policy makers and resource managers. This special issue is intended to advance the conversation. Interactions between renewable energy facilities and fauna are complex. Each source of renewable energy has its own conservation concerns, and each presents its own set of opportunities for mitigation; Other concerns and mitigations are shared. In this overview, we review climate risks to biota, clarify the complementarities among renewables for the conservation community, and summarize research on energy effects on biota for the energy community. The papers invited for this special issue address fossil (coal, oil, natural gas) and renewable energy (terrestrial biomass energy, hydropower, marine-hydrokinetic energy, wind energy, solar energy) and affected fauna. Finally, we hope that the results of these studies, and others like them, set us on a path toward low-carbon energy systems that provide society with energy while protecting future biodiversity.

29 ENERGY PLANNING, POLICY, AND ECONOMY↗
DOE OSTI2024

The role of the iron and steel sector in achieving net zero U.S. CO 2 emissions by 2050

The U.S. steel sector is a hard-to-abate sector because of its heavy dependence on fossil fuels and its high capital requirements. In 2015, the sector was one of the major carbon emitters, contributing 10 % of the U.S. industrial CO 2 emissions. The ability to decarbonize the U.S. iron and steel sector directly affects the ability of the U.S. to achieve economy-wide net zero CO 2 by 2050. In this paper, we use the Global Change Analysis Model (GCAM) to analyze different U.S. steel sector decarbonization pathways under varying technology, policy, and demand futures. These pathways provide insights on how various low-carbon steelmaking technologies such as those using carbon capture and storage (CCS), hydrogen, or scrap could help reduce U.S. steel emissions by mid-century. In our primary decarbonization pathway, we find that nearly all of the conventional fossil-based steelmaking capacity is fully integrated with CCS by 2050. However, without CCS availability, almost all of the conventional fossil-based steelmaking is phased-out by 2050 and is replaced by hydrogen-based production. Scrap-based production continues to remain vital across both of these decarbonization pathways. Furthermore, we find that demand reduction could help reduce the required levels of CCS and hydrogen-based production in the decarbonization pathways. Implementation of advanced energy efficiency measures could help substantially reduce the sector's energy usage. Finally, we observe that addressing the embodied carbon transfer associated with steel imports will be crucial for fully decarbonizing the U.S. steel sector.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2020

Catalina Repower Feasibility Study: NREL Phases I & II Summary Report

Engineers at the National Renewable Energy Laboratory (NREL) supported Southern California Edison (SCE) and the United States Environmental Protection Agency (EPA) by conducting technical and economic analyses for energy systems at Santa Catalina (Catalina) Island, which is located 22 miles off the coast of Long Beach, California. This effort was part of a broader Repower Catalina Feasibility Study that was also supported by NV5, an engineering consulting firm and project partner to NREL for this analysis. This document describes NREL’s techno-economic modeling and optimization analysis for the first two phases of this project which focus on supply-side generation and energy storage options for Catalina. SCE’s goal for this analysis is to determine a strategy for electricity generation on Catalina Island that results in lower energy costs, improved energy resiliency, and reduced air emissions. EPA goals for this effort are to reduce emissions of air pollution and encourage renewable energy development on contaminated and formerly contaminated lands when such development is aligned with the community’s vision for the site. Currently, an on-island SCE power plant serves the Catalina Island electrical load with 6 reciprocating diesel generators totaling 9.4 MW; 23 propane-fueled microturbines totaling 1.5 MW; and a 1-MW, 7.2-MWh sodium sulfur battery energy storage system (BESS). In 2017, the electricity consumption on the island was 29.1 GWh, with an average load of 3.3 MW and peak load of approximately 5.5 MW. Considering new environmental standards on diesel generator emissions from California’s South Coast Air Quality Management District, a 60% renewable energy target for 2030 laid out in California’s Senate Bill 100, SCE’s Clean Power Electrification Pathway, and the characteristics of the island’s existing diesel generators, SCE is seeking to evaluate the technical and economic implications of different energy technology options to determine a path forward. Phases I and II of the Repower Catalina Feasibility Study, summarized in this document, evaluated the following: Interconnection with the mainland via an undersea cable; On-island fossil fuel generation, including diesel, propane, and/or liquified natural gas (LNG); On-island renewable energy (RE) technologies, including solar photovoltaics (PV), wind turbines, and wave energy devices; BESS to support the above generation technologies; Initial analysis of the potential impacts of implementing energy efficiency measures. Results indicate strong techno-economic potential for a mix of on-island diesel and/or propane generators, solar PV, BESS, and energy efficiency measures to help SCE and Catalina achieve their goals compliant with California’s emissions and clean energy standards while minimizing electricity life cycle costs (LCC) over the 30-year analysis period. This document summarizes the considerations and findings of Phases I and II, focusing on high-level takeaways from Phase I and more detailed results from Phase II, and discusses a potential path forward for Phase III.

29 ENERGY PLANNING, POLICY, AND ECONOMY↗
NASA NTRS2015

An Inversion Analysis of Recent Variability in Natural CO2 Fluxes Using GOSAT and In Situ Observations

About one-half of the global CO2 emissions from fossil fuel combustion and deforestation accumulates in the atmosphere, where it contributes to global warming. The rest is taken up by vegetation and the ocean. The precise contribution of the two sinks, and their location and year-to-year variability are, however, not well understood. We use two different approaches, batch Bayesian synthesis inversion and variational data assimilation, to deduce the global spatiotemporal distributions of CO2 fluxes during 2009-2010. One of our objectives is to assess different sources of uncertainties in inferred fluxes, including uncertainties in prior flux estimates and observations, and differences in inversion techniques. For prior constraints, we utilize fluxes and uncertainties from the CASA-GFED model of the terrestrial biosphere and biomass burning driven by satellite observations and interannually varying meteorology. We also use measurement-based ocean flux estimates and two sets of fixed fossil CO2 emissions. Here, our inversions incorporate column CO2 measurements from the GOSAT satellite (ACOS retrieval, filtered and bias-corrected) and in situ observations (individual flask and afternoon-average continuous observations) to estimate fluxes in 108 regions over 8-day intervals for the batch inversion and at 3 x 3.75 weekly for the variational system. Relationships between fluxes and atmospheric concentrations are derived consistently for the two inversion systems using the PCTM atmospheric transport model driven by meteorology from the MERRA reanalysis. We compare the posterior fluxes and uncertainties derived using different data sets and the two inversion approaches, and evaluate the posterior atmospheric concentrations against independent data including aircraft measurements. The optimized fluxes generally resemble those from other studies. For example, the results indicate that the terrestrial biosphere is a net CO2 sink, and a GOSAT-only inversion suggests a shift in the global sink from the tropics south to the north relative to the prior and to an in-situ-only inversion. We also find a smaller terrestrial sink in higher-latitude northern regions in boreal summer of 2010 relative to 2009.

Carbon dioxide↗
DOE OSTI2021

The effect of increasing temperature on crop photosynthesis: from enzymes to ecosystems

Abstract As global land surface temperature continues to rise and heatwave events increase in frequency, duration, and/or intensity, our key food and fuel cropping systems will likely face increased heat-related stress. A large volume of literature exists on exploring measured and modelled impacts of rising temperature on crop photosynthesis, from enzymatic responses within the leaf up to larger ecosystem-scale responses that reflect seasonal and interannual crop responses to heat. This review discusses (i) how crop photosynthesis changes with temperature at the enzymatic scale within the leaf; (ii) how stomata and plant transport systems are affected by temperature; (iii) what features make a plant susceptible or tolerant to elevated temperature and heat stress; and (iv) how these temperature and heat effects compound at the ecosystem scale to affect crop yields. Throughout the review, we identify current advancements and future research trajectories that are needed to make our cropping systems more resilient to rising temperature and heat stress, which are both projected to occur due to current global fossil fuel emissions.

59 BASIC BIOLOGICAL SCIENCES↗
NASA NTRS2021

Improved Constraints on Global Methane Emissions and Sinks Using δ13C-CH4

We study the drivers behind the global atmospheric methane (CH4) increase observed after 2006. Candidate emission and sink scenarios are constructed based on proposed hypotheses in the literature. These scenarios are simulated in the TM5 tracer transport model for 1984–2016 to produce three-dimensional fields of CH4 and δ13C-CH4, which are compared with observations to test the competing hypotheses in the literature in one common model framework. We find that the fossil fuel (FF) CH4 emission trend from the Emissions Database for Global Atmospheric Research 4.3.2 inventory does not agree with observed δ13C-CH4. Increased FF CH4 emissions are unlikely to be the dominant driver for the post-2006 global CH4 increase despite the possibility for a small FF emission increase. We also find that a significant decrease in the abundance of hydroxyl radicals (OH) cannot explain the post-2006 global CH4 increase since it does not track the observed decrease in global mean δ13C-CH4. Different CH4 sinks have different fractionation factors for δ13C-CH4, thus we can investigate the uncertainty introduced by the reaction of CH4 with tropospheric chlorine (Cl), a CH4 sink whose abundance, spatial distribution, and temporal changes remain uncertain. Our results show that including or excluding tropospheric Cl as a 13 Tg/year CH4 sink in our model changes the magnitude of estimated fossil emissions by ∼20%. We also found that by using different wetland emissions based on a static versus a dynamic wetland area map, the partitioning between FF and microbial sources differs by 20 Tg/year, ∼12% of estimated fossil emissions.

X. Lan↗
DOE OSTI2019

H2@Scale: Economic Potential of Hydrogen as an Energy Intermediate

The H2@Scale concept envisions hydrogen as an energy intermediate across multiple energy sectors. The concept is motivated both by the opportunity to produce hydrogen from low-cost energy resources, and by the many potential applications of hydrogen, including as energy for transportation - used directly in fuel cell electric vehicles (FCEVs), as a feedstock for synthetic fuels, and to upgrade oil and biomass - feedstock for industry (e.g., for ammonia production, metals refining, and other end uses), heat for industry and buildings, and electricity storage. A key hydrogen production opportunity is using variable renewable electricity (i.e., electricity generated by wind turbines or solar photovoltaic panels) during hours when generation exceeds the load on the grid as a source of low-cost, dispatch constrained electricity (LDE). In addition to producing low-cost hydrogen, electrolysis can also serve as a form of responsive load on the electric grid, which can enhance grid stability, reduce curtailment, and create a supplementary revenue stream for generators. The future use and adoption of hydrogen across end-use applications depends both the cost of hydrogen production and on each application's threshold price (i.e., the maximum price each application will pay for hydrogen - above that price, the application has an alternative that is more economic). We estimate economic potential of the hydrogen market - the quantity of hydrogen at an equilibrium price at which suppliers are willing to produce and consumers are willing to buy the same quantity of hydrogen - by developing supply and demand curves for hydrogen production and use. The demand curves are based on the threshold price for various quantities of hydrogen in each market, which is affected by projected prices for alternatives that could provide the same service (e.g., fuel for vehicles, feedstock for metals refining). The supply curves include hydrogen produced via natural gas steam methane reforming, high-temperature electrolysis coupled with nuclear power plants, biomass gasification, and low-temperature electrolysis using LDE. We use a range of market and technology-advancement assumptions to estimate the economic potential for five scenarios in the mid 21st century timeframe, and the corresponding impacts on energy use and emissions. We estimate hydrogen's economic potential to be 14-48 MMT/yr in the contiguous United States - corresponding to 1.5-5 times current annual consumption - depending on key assumptions about the future market conditions and the success of hydrogen production research and development (R&D) in our five scenarios. As a result of the estimated economic potential markets, we also approximate that grid-integrated electrolysis can increase the penetration of wind generation in the electricity market by providing a value stream for LDE, and that total U.S. fossil fuel use could decline below a scenario with high renewable penetration on the grid. We find that hydrogen has potential to provide technical and economic synergies when integrated across multiple sectors of the U.S. energy system, but continued R&D, infrastructure, and market development for LDE are required.

08 HYDROGEN↗
DOE OSTI2018

Integrated Energy Planning with a High Share of Variable Renewable Energy Sources for a Caribbean Island

Although it can be complex to integrate variable renewable energy sources such as wind power and photovoltaics into an energy system, the potential benefits are large, as it can help reduce fuel imports, balance the trade, and mitigate the negative impacts in terms of climate change. In order to try to integrate a very large share of variable renewable energy sources into the energy system, an integrated energy planning approach was used, including ice storage in the cooling sector, a smart charging option in the transport sector, and an excess capacity of reverse osmosis technology that was utilised in order to provide flexibility to the energy system. A unit commitment and economic dispatch tool (PLEXOS) was used, and the model was run with both 5 min and 1 h time resolutions. The case study was carried out for a typical Caribbean island nation, based on data derived from measured data from Aruba. The results showed that 78.1% of the final electricity demand in 2020 was met by variable renewable energy sources, having 1.0% of curtailed energy in the energy system. The total economic cost of the modelled energy system was similar to the current energy system, dominated by the fossil fuel imports. Here, the results are relevant for many populated islands and island nations.

24 POWER TRANSMISSION AND DISTRIBUTION↗
DOE OSTI2017

Heterogeneous Creep Deformations and Correlation to Microstructures in Fe-30Cr-3Al Alloys Strengthened by an Fe 2 Nb Laves Phase

We have develooped a new Fe-Cr-Al (FCA) alloy system with good oxidation resistance and creep strength at high temperature. The alloy system is a candidate for use in future fossil-fueled power plants. The creep strength of these alloys at 973 K (700 °C) was found to be comparable with traditional 9 pct Cr ferritic–martensitic steels. A few FCA alloys with general composition of Fe-30Cr-3Al-.2Si-xNb (x = 0, 1, or 2) with a ferrite matrix and Fe 2 Nb-type Laves precipitates were prepared. The detailed microstructural characterization of samples, before and after creep rupture testing, indicated precipitation of the Laves phase within the matrix, Laves phase at the grain boundaries, and a 0.5 to 1.5 μm wide precipitate-free zone (PFZ) parallel to all the grain boundaries. In these alloys, the areal fraction of grain boundary Laves phase and the width of the PFZ controlled the cavitation nucleation and eventual grain boundary ductile failure. Finally, we used a phenomenological model to compare the creep strain rates controlled by the effects of the particles on the dislocations within the grain and at grain boundaries. (The research sponsored by US-DOE, Office of Fossil Energy, the Crosscutting Research Program).

36 MATERIALS SCIENCE↗
NASA NTRS2017

Variability and Quasi-Decadal Changes in the Methane Budget over the Period 2000-2012

Following the recent Global Carbon Project (GCP) synthesis of the decadal methane (CH4) budget over 2000- 2012, we analyse here the same dataset with a focus on quasi-decadal and inter-annual variability in CH4 emissions. The GCP dataset integrates results from top-down studies (exploiting atmospheric observations within an atmospheric inverse-modelling framework) and bottom-up models (including process-based models for estimating land surface emissions and atmospheric chemistry), inventories of anthropogenic emissions, and data-driven approaches. The annual global methane emissions from top-down studies, which by construction match the observed methane growth rate within their uncertainties, all show an increase in total methane emissions over the period 2000-2012, but this increase is not linear over the 13 years. Despite differences between individual studies, the mean emission anomaly of the top-down ensemble shows no significant trend in total methane emissions over the period 2000-2006, during the plateau of atmospheric methane mole fractions, and also over the period 2008-2012, during the renewed atmospheric methane increase. However, the top-down ensemble mean produces an emission shift between 2006 and 2008, leading to 22 [16-32] Tg CH4 yr(exp -1) higher methane emissions over the period 2008-2012 compared to 2002-2006. This emission increase mostly originated from the tropics, with a smaller contribution from mid-latitudes and no significant change from boreal regions. The regional contributions remain uncertain in top-down studies. Tropical South America and South and East Asia seem to contribute the most to the emission increase in the tropics. However, these two regions have only limited atmospheric measurements and remain therefore poorly constrained. The sectorial partitioning of this emission increase between the periods 2002-2006 and 2008-2012 differs from one atmospheric inversion study to another. However, all top-down studies suggest smaller changes in fossil fuel emissions (from oil, gas, and coal industries) compared to the mean of the bottom-up inventories included in this study. This difference is partly driven by a smaller emission change in China from the top-down studies compared to the estimate in the Emission Database for Global Atmospheric Research (EDGARv4.2) inventory, which should be revised to smaller values in a near future. We apply isotopic signatures to the emission changes estimated for individual studies based on five emission sectors and find that for six individual top-down studies (out of eight) the average isotopic signature of the emission changes is not consistent with the observed change in atmospheric 13CH4. However, the partitioning in emission change derived from the ensemble mean is consistent with this isotopic constraint. At the global scale, the top-down ensemble mean suggests that the dominant contribution to the resumed atmospheric CH4 growth after 2006 comes from microbial sources (more from agriculture and waste sectors than from natural wetlands), with an uncertain but smaller contribution from fossil CH4 emissions. In addition, a decrease in biomass burning emissions (in agreement with the biomass burning emission databases) makes the balance of sources consistent with atmospheric 13CH4 observations. In most of the top-down studies included here, OH concentrations are considered constant over the years (seasonal variations but without any inter-annual variability). As a result, the methane loss (in particular through OH oxidation) varies mainly through the change in methane concentrations and not its oxidants. For these reasons, changes in the methane loss could not be properly investigated in this study, although it may play a significant role in the recent atmospheric methane changes as briefly discussed at the end of the paper.

Saunois, Marielle↗
DOE OSTI2017

Variability and quasi-decadal changes in the methane budget over the period 2000–2012

Following the recent Global Carbon Project (GCP) synthesis of the decadal methane (CH 4 ) budget over 2000–2012 (Saunois et al., 2016), we analyse here the same dataset with a focus on quasi-decadal and inter-annual variability in CH 4 emissions. The GCP dataset integrates results from top-down studies (exploiting atmospheric observations within an atmospheric inverse-modelling framework) and bottom-up models (including process-based models for estimating land surface emissions and atmospheric chemistry), inventories of anthropogenic emissions, and data-driven approaches. The annual global methane emissions from top-down studies, which by construction match the observed methane growth rate within their uncertainties, all show an increase in total methane emissions over the period 2000-2012, but this increase is not linear over the 13 years. Despite differences between individual studies, the mean emission anomaly of the top-down ensemble shows no significant trend in total methane emissions over the period 2000-2006, during the plateau of atmospheric methane mole fractions, and also over the period 2008-2012, during the renewed atmospheric methane increase. However, the top-down ensemble mean produces an emission shift between 2006 and 2008, leading to 22 [16-32]Tg CH 4 yr -1 higher methane emissions over the period 2008-2012 compared to 2002-2006. This emission increase mostly originated from the tropics, with a smaller contribution from mid-latitudes and no significant change from boreal regions. The regional contributions remain uncertain in top-down studies. Tropical South America and South and East Asia seem to contribute the most to the emission increase in the tropics. However, these two regions have only limited atmospheric measurements and remain therefore poorly constrained. The sectorial partitioning of this emission increase between the periods 2002-2006 and 2008-2012 differs from one atmospheric inversion study to another. However, all top-down studies suggest smaller changes in fossil fuel emissions (from oil, gas, and coal industries) compared to the mean of the bottom-up inventories included in this study. This difference is partly driven by a smaller emission change in China from the top-down studies compared to the estimate in the Emission Database for Global Atmospheric Research (EDGARv4.2) inventory, which should be revised to smaller values in a near future. We apply isotopic signatures to the emission changes estimated for individual studies based on five emission sectors and find that for six individual top-down studies (out of eight) the average isotopic signature of the emission changes is not consistent with the observed change in atmospheric 13 CH 4 . However, the partitioning in emission change derived from the ensemble mean is consistent with this isotopic constraint. At the global scale, the top-down ensemble mean suggests that the dominant contribution to the resumed atmospheric CH 4 growth after 2006 comes from microbial sources (more from agriculture and waste sectors than from natural wetlands), with an uncertain but smaller contribution from fossil CH 4 emissions. In addition, a decrease in biomass burning emissions (in agreement with the biomass burning emission databases) makes the balance of sources consistent with atmospheric 13 CH 4 observations. In most of the top-down studies included here, OH concentrations are considered constant over the years (seasonal variations but without any inter-annual variability). As a result, the methane loss (in particular through OH oxidation) varies mainly through the change in methane concentrations and not its oxidants. For these reasons, changes in the methane loss could not be properly investigated in this study, although it may play a significant role in the recent atmospheric methane changes as briefly discussed at the end of the paper.

58 GEOSCIENCES↗
DOE OSTI2022

Using Multiscale Ethane/Methane Observations to Attribute Coal Mine Vent Emissions in the San Juan Basin From 2013 to 2021

Abstract Source attribution of natural gas emissions from fossil fuels in New Mexico's San Juan Basin (SJB) is challenging due to source heterogeneity and emissions transience. We demonstrate that ethane (C 2 H 6 ) to methane (CH 4 ) mixing ratios can identify and separate sources over different scales using various measurement techniques. We report simultaneous CH 4 and C 2 H 6 observations near a coal mine vent and oil and gas (O&G) emission sources using ground‐based in situ measurements in 2020/2021. During these campaigns, we observed a stable coal vent C 2 H 6 :CH 4 ratio of 1.28% ± 0.11%, discernibly different than nearby O&G source ratios ranging from 0.9% to 16.8%. We analyze airborne observations of the SJB taken in 2014/2015 that exhibit similar coal vent ratios and further show the region's heterogeneity. We identify episodic O&G sources, including a gas plant source detected in 2014/2015 that is absent in our 2020/2021 data. We examine total column observations of C 2 H 6 and CH 4 made in 2013 with a solar spectrometer and find a C 2 H 6 :CH 4 ratio of 1.3% ± 0.4% for the coal vent. The stable and unique coal vent ratio relative to other O&G sources in the region is used to demonstrate that consistent attribution is possible using various measurement methods at multiple scales across many years. Finally, we demonstrate that using C 2 H 6 as a proxy for fossil CH 4 inversions can inform detailed basin‐scale inversions, provided we understand source specific changes in the C 2 H 6 :CH 4 ratio like we report in the SJB.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2018

Global Carbon Budget 2017

Here an accurate assessment of anthropogenic carbon dioxide (CO 2 ) 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. CO 2 emissions from fossil fuels and industry ( E FF ) are based on energy statistics and cement production data, respectively, while emissions from land-use change ( E LUC ), mainly deforestation, are based on land-cover change data and bookkeeping models. The global atmospheric CO 2 concentration is measured directly and its rate of growth ( G ATM ) is computed from the annual changes in concentration. The ocean CO 2 sink ( S OCEAN ) and terrestrial CO 2 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 ±1 σ . For the last decade available (2007–2016), E FF was 9.4 ± 0.5 GtC yr –1 , E LUC 1.3 ± 0.7 GtC yr –1 , G ATM 4.7 ± 0.1 GtC yr –1 , S OCEAN 2.4 ± 0.5 GtC yr –1 , and S LAND 3.0 ± 0.8 GtC yr –1 , with a budget imbalance B IM of 0.6 GtC yr –1 indicating overestimated emissions and/or underestimated sinks. For year 2016 alone, the growth in E FF was approximately zero and emissions remained at 9.9 ±\ 0.5 GtC yr –1 . Also for 2016, E LUC was 1.3 ± .7 GtC yr –1 , G ATM was 6.1 ± 0.2 GtC yr –1 , S OCEAN was 2.6 ± 0.5 GtC yr –1 , and S LAND was 2.7 ± 1.0 GtC yr –1 , with a small B IM of –0.3 GtC. G ATM continued to be higher in 2016 compared to the past decade (2007–2016), reflecting in part the high fossil emissions and the small S LAND consistent with El Niño conditions. The global atmospheric CO 2 concentration reached 402.8 ± 0.1 ppm averaged over 2016. For 2017, preliminary data for the first 6–9 months indicate a renewed growth in E FF of +2.0 % (range of 0.8 to 3.0 %) based on national emissions projections for China, USA, and India, and projections of gross domestic product (GDP) corrected for recent changes in the carbon intensity of the economy for the rest of the world. This living data update documents changes in the methods and data sets used in this new global carbon budget compared with previous publications of this data set.

54 ENVIRONMENTAL SCIENCES↗