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

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At least 325 records · Page 18
All sourcesNASA NTRSDOE OSTI
DOE OSTI2020

Prestack Waveform Inversion at GC 955: Trials and sensitivity of PWI to high-resolution seismic data (Data Report)

Understanding the spatial extent and variability of hydrate deposits has important implications for potential economic production, climate change, and assessing natural hazards risks. Seismic reflection techniques are capable of determining the extent of gas hydrate deposits and can shed light on hydrate concentrations and properties. Using high resolution prestack time migrated seismic data collected during a 2013 US Geological Survey expedition and prestack waveform inversion (PWI) techniques, we produce highly resolved velocity models and compare them to co-located well logs. Coupling our PWI results with velocity-porosity relationships and nearby well control, we compare hydrate properties at site 955 in the Green Canyon and site 313 at Walker Ridge.

03 NATURAL GAS↗
DOE OSTI2024

Phenotypic and genomic characterization of Methanothermobacter wolfeii strain BSEL, a CO 2 -capturing archaeon with minimal nutrient requirements

A new variant of Methanothermobacter wolfeii was isolated from an anaerobic digester using enrichment cultivation in anaerobic conditions. Here, the new isolate was taxonomically identified via 16S rRNA gene sequencing and tagged as M. wolfeii BSEL. The whole genome of the new variant was sequenced and de novo assembled. Genomic variations between the BSEL strain and the type strain were discovered, suggesting evolutionary adaptations of the BSEL strain that conferred advantages while growing under a low concentration of nutrients. M. wolfeii BSEL displayed the highest specific growth rate ever reported for the wolfeii species (0.27 ± 0.03 h –1 ) using carbon dioxide (CO 2 ) as unique carbon source and hydrogen (H 2 ) as electron donor. M. wolfeii BSEL grew at this rate in an environment with ammonium (NH 4 + ) as sole nitrogen source. The minerals content required to cultivate the BSEL strain was relatively low and resembled the ionic background of tap water without mineral supplements. Optimum growth rate for the new isolate was observed at 64°C and pH 8.3. In this work, it was shown that wastewater from a wastewater treatment facility can be used as a low-cost alternative medium to cultivate M. wolfeii BSEL. Continuous gas fermentation fed with a synthetic biogas mimic along with H 2 in a bubble column bioreactor using M. wolfeii BSEL as biocatalyst resulted in a CO 2 conversion efficiency of 97% and a final methane (CH 4 ) titer of 98.5%v, demonstrating the ability of the new strain for upgrading biogas to renewable natural gas.

09 BIOMASS FUELS↗
DOE OSTI2020

Methanotrophic-Mediated Methylmercury Transformation: Characterization of Products, Mechanism, and Environmental Significance (Final Technical Report)

Previous work in the laboratories of the PIs found that methanotrophs, through the production of a novel metal chelator called methanobactin (MB), can bind inorganic mercury (Hg[II]). By doing so, methanotrophs substantially reduce Hg[II] toxicity. We have also recently shown that MB can bind a much more toxic form of mercury, the neurotoxin methylmercury (MeHg). MeHg bioaccumulates and biomagnifies in biota such as fish, and is of significant concern. Further, certain methanotrophs expressing MB are able to demethylate significant amounts of MeHg despite lacking merB, the organomercurial lyase. Further, unlike the canonical organomercurial lyase, methanotrophs take up and degrade MeHg at environmentally relevant pH and Hg concentrations (i.e., picomolar to nanomolar), suggesting that methanotrophs likely play a critical role in controlling net MeHg production and toxicity in situ. However, although MB is necessary for methanotrophic-mediated MeHg degradation, it is not sufficient as purified MB binds, but does not degrade MeHg. That is, MB appears to serve as binding device leading to demethylation of MeHg by an as yet unknown mechanism. The major goals of this project were to extend this initial work and characterize the mechanism of methanotrophic-mediated MeHg demethylation and how methanobactin production may affect net methylmercury production in situ.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2022

2D imaging of absolute methyl concentrations in nanosecond pulsed plasma by photo-fragmentation laser-induced fluorescence

The methyl radical plays a central role in plasma-assisted hydrocarbon chemistry but is challenging to detect due to its high reactivity and strongly pre-dissociative electronically excited states. In this work, we report the development of a photo-fragmentation laser-induced fluorescence (PF-LIF) diagnostic for quantitative 2D imaging of methyl profiles in a plasma. This technique provides temporally and spatially resolved measurements of local methyl distributions, including in near-surface regions that are important for plasma-surface interactions such as plasma-assisted catalysis. The technique relies on photo-dissociation of methyl by the fifth harmonic of a Nd:YAG laser at 212.8 nm to produce CH fragments. These photofragments are then detected with LIF imaging by exciting a transition in the B-X(0, 0) band of CH with a second laser at 390 nm. Fluorescence from the overlapping A-X(0, 0), A-X(1, 1), and B-X(0, 1) bands of CH is detected near 430 nm with the A-state populated by collisional B-A electronic energy transfer. This non-resonant detection scheme enables interrogation close to a surface. The PF-LIF diagnostic is calibrated by producing a known amount of methyl through photo-dissociation of acetone vapor in a calibration gas mixture. We demonstrate PF-LIF imaging of methyl production in methane-containing nanosecond pulsed plasmas impinging on dielectric surfaces. Absolute calibration of the diagnostic is demonstrated in a diffuse, plane-to-plane discharge. Measured profiles show a relatively uniform distribution of up to 30 ppm of methyl. Relative methyl measurements in a filamentary plane-to-plane discharge and a plasma jet reveal highly localized intense production of methyl. The utility of the PF-LIF technique is further demonstrated by combining methyl measurements with formaldehyde LIF imaging to capture spatiotemporal correlations between methyl and formaldehyde, which is an important intermediate species in plasma-assisted oxidative coupling of methane.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2020

Verification of diesel spray ignition phenomenon in dual-fuel diesel-piloted premixed natural gas engine

Dual-fuel (DF) engines, in which premixed natural gas and air in an open-type combustion chamber is ignited by diesel-fuel pilot sprays, have been more popular for marine use than pre-chamber spark ignition (PCSI) engines because of their superior durability. However, control of ignition and combustion in DF engines is more difficult than in PCSI engines. In this context, here we focus on the ignition stability of n-heptane pilot-fuel jets injected into a compressed premixed charge of natural gas and air at low-load conditions. To aid understanding of the experimental data, chemical-kinetics simulations were carried out in a simplified engine-environment that provided insight into the chemical effects of methane (CH4) on pilot-fuel ignition. The simulations reveal that CH4 has an effect on both stages of n-heptane autoignition: the small, first-stage, cool-flame-type, low-temperature ignition (LTI) and the larger, second-stage, high-temperature ignition (HTI). As the ratio of pilot-fuel to CH4 entrained into the spray decreases, the initial oxidization of CH4 consumes the OH radicals produced by pilot-fuel decomposition during LTI, thereby inhibiting its progression to HTI. Using imaging diagnostics, the spatial and temporal progression of LTI and HTI in DF combustion are measured in a heavy-duty optical engine, and the imaging data are analyzed to understand the cause of severe fluctuations in ignition timing and combustion completeness at low-load conditions. Images of cool-flame and hydroxyl radical (OH*) chemiluminescence serve as indicators of LTI and HTI, respectively. The cycle-to-cycle and spatial variation in ignition extracted from the imaging data are used as key metrics of comparison. The imaging data indicate that the local concentration of the pilot-fuel and the richness of the surrounding natural-gas air mixture are important for LTI and HTI, but in different ways. In particular, higher injection pressures and shorter injection durations increase the mixing rate, leading to lower concentrations of pilot-fuel more quickly, which can inhibit HTI even as LTI remains relatively robust. Decreasing the injection pressure from 80 MPa to 40 MPa and increasing the injection duration from 500 µs to 760 µs maintained constant pilot-fuel mass, while promoting robust transition from LTI to HTI by effectively slowing the mixing rate. This allows enough residence time for the OH radicals, produced by the two-stage ignition chemistry of the pilot-fuel, to accelerate the transition from LTI to HTI before being consumed by CH4 oxidation. Thus from a practical perspective, for a premixed natural gas fuel–air equivalence-ratio, it is possible to improve the “stability” of the combustion process by solely manipulating the pilot-fuel injection parameters while maintaining constant mass of injected pilot-fuel. This allows for tailoring mixing trajectories to offset changes in fuel ignition chemistry, so as to promote a robust transition from LTI to HTI by changing the balance between the local concentration of the pilot-fuel and richness of the premixed natural gas and air. This could prove to be a valuable tool for combustion design to improve fuel efficiency or reduce noise or perhaps even reduce heat-transfer losses by locating early combustion away from in-cylinder walls.

42 ENGINEERING↗
DOE OSTI2024

Controls on Stable Methane Isotope Values in Northern Peatlands and Potential Shifts in Values Under Permafrost Thaw Scenarios

Abstract Northern peatlands are a globally significant source of methane (CH 4 ), and emissions are projected to increase due to warming and permafrost loss. Understanding the microbial mechanisms behind patterns in CH 4 production in peatlands will be key to predicting annual emissions changes, with stable carbon isotopes (δ 13 C‐CH 4 ) being a powerful tool for characterizing these drivers. Given that δ 13 C‐CH 4 is used in top‐down atmospheric inversion models to partition sources, our ability to model CH 4 production pathways and associated δ 13 C‐CH 4 values is critical. We sought to characterize the role of environmental conditions, including hydrologic and vegetation patterns associated with permafrost thaw, on δ 13 C‐CH 4 values from high‐latitude peatlands. We measured porewater and emitted CH 4 stable isotopes, pH, and vegetation composition from five boreal‐Arctic peatlands. Porewater δ 13 C‐CH 4 was strongly associated with peatland type, with δ 13 C enriched values obtained from more minerotrophic fens (−61.2 ± 9.1‰) compared to permafrost‐free bogs (−74.1 ± 9.4‰) and raised permafrost bogs (−81.6 ± 11.5‰). Variation in porewater δ 13 C‐CH 4 was best explained by sedge cover, CH 4 concentration, and the interactive effect of peatland type and pH (r 2 = 0.50,p < 0.001). Emitted δ 13 C‐CH 4 varied greatly but was positively correlated with porewater δ 13 C‐CH 4 . We calculated a mixed atmospheric δ 13 C‐CH 4 value for northern peatlands of −65.3 ± 7‰ and show that this value is more sensitive to landscape drying than wetting under permafrost thaw scenarios. Our results suggest northern peatland δ 13 C‐CH 4 values are likely to shift in the future which has important implications for source partitioning in atmospheric inversion models.

Environmental Sciences & Ecology↗
DOE OSTI2020

Influences of Hillslope Biogeochemistry on Anaerobic Soil Organic Matter Decomposition in a Tundra Watershed

In this work, we investigated rates and controls on greenhouse gas (CO 2 and CH 4 ) production in two contrasting water-saturated tundra soils within a permafrost-affected watershed near Nome, Alaska, United States. Three years of field sample analysis have shown that soil from a fen-like area in the toeslope of the watershed had higher pH and higher porewater ion concentrations than soil collected from a bog-like peat plateau at the top of the hillslope. The influence of these contrasting geochemical and topographic environments on CO 2 and CH 4 production was tested in soil microcosms by incubating both the organic- and mineral-layer soils anaerobically for 55 days. Additionally, nitrogen (as NH 4 Cl) was added to half of the microcosms to test potential effects of N limitation on microbial greenhouse gas production. We found that the organic toeslope soils produced more CO 2 and CH 4 , fueled by higher pH and higher concentrations of water-extractable organic C (WEOC). Our results also indicate N limitation on CO 2 production in the peat plateau soils but not the toeslope soils. Together these results suggest that the weathering and leaching of ions and nutrients from tundra hillslopes can increase the rate of anaerobic soil organic matter decomposition in downslope soils by (1) increasing the pH of soil porewater; (2) providing bioavailable WEOC and fermentation products such as acetate; and (3) relieving microbial N limitation through nutrient runoff. We conclude that the soil geochemistry as mediated by landscape position is an important factor influencing the rate and magnitude of greenhouse gas production in tundra soils.

58 GEOSCIENCES↗
DOE OSTI2025

ELM–Wet: Inclusion of a Wet–Landunit With Sub–Grid Representation of Eco–Hydrological Patches and Hydrological Forcing Improves Methane Emission Estimations in the E3SM Land Model (ELM)

Wetlands are the largest emitters of biogenic methane (CH 4 ) and represent the highest source of uncertainty in global CH 4 budgets. Here, we aim to improve the realism of wetland representation in the U.S. Department of Energy's Exascale Earth System Model land surface model, ELM, thereby reducing uncertainty of CH 4 flux predictions. We develop an updated version, ELM-Wet, where we activate a separate landunit for wetlands that handles multiple wetland-specific eco-hydrological patch functional types. We introduce more realistic hydrological forcing through prescribing site-level constraints on surface water elevation, which allows resolving different sustained inundation depth for different patches, and if data exists, prescribing inundation depth. We modified the calculation of aerenchyma transport diffusivity based on observed conductance per leaf area for different vegetation types. We use Bayesian Optimization to parameterize CO 2 and CH 4 fluxes in the developed wet-landunit. Site-level simulations of a coastal non-tidal freshwater wetland in Louisiana were performed with the updated model. Eddy covariance observations of CO 2 and CH 4 fluxes from 2012 to 2013 were used to train the model and data from 2021 were used for validation. Patch-specific chamber flux observations and observations of CH 4 concentration profiles in the soil porewater from 2021 were used for evaluation of the model performance. Our results show that ELM-Wet reduces the model's CH 4 emission root mean squared error by up to 33% and is able to represent inter-daily CO 2 and CH 4 flux variability across the wetland's eco-hydrological patches, including during periods of extreme dry or wet conditions.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2021

Investigation of species-mass diffusion in binary-species boundary layers at high pressure using direct numerical simulations

Here, direct numerical simulations of single-species and binary-species temporal boundary layers at high pressure are performed with special attention to species-mass diffusion. The working fluids are nitrogen or a mixture of nitrogen and methane. Mean profiles and turbulent fluctuations of mass fraction show that their qualitative characteristics are different from those of streamwise velocity and temperature, due to the different boundary conditions. In a wall-parallel plane near the wall, the streamwise velocity and temperature have streaky patterns and the fields are similar. However, the mass fraction field at the same location is different from the streamwise velocity and temperature fields indicating that species-mass diffusion is not similar to the momentum and thermal diffusion. In contrast, at the centre and near the edge of the boundary layer, the mass fraction and temperature fields have almost the same pattern, indicating that the similarity between thermal and species-mass diffusion holds away from the wall. The lack of similarity near the wall is traced to the Soret effect that induces a temperature-gradient-dependent species-mass flux. As a result, a new phenomenon has been identified for a non-isothermal binary-species system – uphill diffusion, which in its classical isothermal definition can only occur for three or more species. A quadrant analysis for the turbulent mass flux reveals that near the wall the Soret effect enhances the negative contributions of the quadrants. Due to the enhancement of the negative contributions, small species-concentration fluid tends to be trapped near the wall.

42 ENGINEERING↗
DOE OSTI2022

An approach to sulfate geoengineering with surface emissions of carbonyl sulfide

Sulfate geoengineering (SG) methods based on lower stratospheric tropical injection of sulfur dioxide (SO 2 ) have been widely discussed in recent years, focusing on the direct and indirect effects they would have on the climate system. Here a potential alternative method is discussed, where sulfur emissions are located at the surface or in the troposphere in the form of carbonyl sulfide (COS) gas. There are two time-dependent chemistry–climate model experiments designed from the years 2021 to 2055, assuming a 40 Tg-Syr -1 artificial global flux of COS, which is geographically distributed following the present-day anthropogenic COS surface emissions (SG-COS-SRF) or a 6 Tg-Syr -1 injection of COS in the tropical upper troposphere (SG-COS-TTL). The budget of COS and sulfur species is discussed, as are the effects of both SG-COS strategies on the stratospheric sulfate aerosol optical depth (~Δτ=0.080 in the years 2046–2055), aerosol effective radius (0.46 µm), surface SO x deposition (+8.9 % for SG-COS-SRF; +3.3 % for SG-COS-TTL), and tropopause radiative forcing (RF; ~-1.5 W m –2 in all-sky conditions in both SG-COS experiments). Indirect effects on ozone, methane and stratospheric water vapour are also considered, along with the COS direct contribution. According to our model results, the resulting net RF is –1.3 W m –2 , for SG-COS-SRF, and –1.5 W m –2 , for SG-COS-TTL, and it is comparable to the corresponding RF of –1.7 W m –2 obtained with a sustained injection of 4 Tg-Syr -1 in the tropical lower stratosphere in the form of SO 2 (SG-SO2, which is able to produce a comparable increase of the sulfate aerosol optical depth). Significant changes in the stratospheric ozone response are found in both SG-COS experiments with respect to SG-SO2 (~5 DU versus +1.4 DU globally). According to the model results, the resulting ultraviolet B (UVB) perturbation at the surface accounts for –4.3 % as a global and annual average (versus –2.4 % in the SG-SO2 case), with a springtime Antarctic decrease of –2.7 % (versus a +5.8 % increase in the SG-SO2 experiment). Overall, we find that an increase in COS emissions may be feasible and produce a more latitudinally uniform forcing without the need for the deployment of stratospheric aircraft. However, our assumption that the rate of COS uptake by soils and plants does not vary with increasing COS concentrations will need to be investigated in future work, and more studies are needed on the prolonged exposure effects to higher COS values in humans and ecosystems.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2020

Benchmark calculations of radiative forcing by greenhouse gases

Changes in concentrations of greenhouse gases lead to changes in radiative fluxes throughout the atmosphere. The value of this change, the instantaneous radiative forcing, varies across climate models, due partly to differences in the distribution of clouds, humidity, and temperature across models, and partly due to errors introduced by approximate treatments of radiative transfer. This paper describes an experiment within the Radiative Forcing Model Intercomparision Project that uses benchmark calculations made with line–by–line models to identify parameterization error in the representation of absorption and emission by greenhouse gases. Clear–sky instantaneous forcing by greenhouse gases is computed using a set of 100 profiles, selected from a re–analysis of present–day conditions, that represent the global annual mean forcing from pre–industrial times to the present–day with sampling errors of less than 0.01 W m –2 . Six contributing line–by–line models agree in their estimate of this forcing to within 0.025 W m –2 while even recently–developed parameterizations have typical errors four or more times larger, suggesting both that the samples reveal true differences among line–by–line models and that parameterization error will be readily identifiable. Agreement among line–by–line models is better in the longwave than in the shortwave where differing treatments of the water vapor vapor continuum affect estimates of forcing by carbon dioxide and methane. The impacts of clouds on instantaneous radiative forcing are estimated from climate model simulations. Here, the adjustment due to stratospheric temperature change by assuming fixed dynamical heating. Adjustments are large only for ozone and for carbon dioxide, for which stratospheric cooling introduces modest non–linearity.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2026

Insights from Initial Engineering Designs of Point Source Capture at Industrial Facilities

Initial engineering design studies examining the application of state-of-the-art carbon capture technology at industrial plants contain generally overlooked real-world design considerations for near-term deployment of point source capture (PSC). The implementation of PSC across a wide range of industrial applications presents unique challenges associated with fluctuating CO<sub>2</sub> concentrations, flue gas composition, and utility and land availability. In this article, seven recent industrial retrofit PSC projects are reviewed to investigate the impact of site-specific factors on project design and cost. Across the seven projects, three capture technology classes and four industrial applications are considered, allowing insight into industry-specific opportunities for PSC technology synergy. Common challenges across projects and proposed design solutions are highlighted to propagate ideas and solutions to close the technology gaps and accelerate learning rates.

FEED Studies↗
DOE OSTI2021

Results of the 2018 Wood Stove Design Challenge

The 2018 Wood Stove Design Challenge was an international design competition which sought to identify top performing residential wood stoves based on automation. To prepare for the event, the Northeast States for Coordinated Air Use Management (NESCAUM) developed a testing protocol that challenged the stoves by testing them in more field-like conditions—capturing emissions from start-up, reloading a stove, and the use of larger piece sizes. Flue gas emissions were measured using a combination of in-stack and novel dilution sampling methods, as the event occurred on the National Mall in Washington D.C. in a non-laboratory setting. Particulate matter (PM), carbon monoxide (CO), carbon dioxide (CO2), and methane (CH4) were measured from three stoves in real-time. A combustion efficiency was also calculated for each stove in real-time. Measured PM emission rates ranged between 1.8 and 8.0 g/hr for all stoves and operating conditions, with the highest emissions being measured during cold start in all cases. The test average PM emission rates were 2.4, 4.0, and 2.4 g/hr for stoves A, B, and C, respectively. Results showed emissions measured during transient operations, which are often excluded in current certification methods, can be significantly higher than steady-state periods—echoing other studies and highlighting the importance of testing in various operational modes for more realistic emission estimates. Additionally, the stoves had overall CO emission rates of 48.8, 284.8, and 100.8 g/hr, for stoves A, B and C, respectively. Calculated PM and CO emission factors overall were low considering the testing protocol sought to follow more challenging yet realistic practices in terms of fuel loading and operating procedures. The overall estimated combustion efficiency for stoves A, B, and C was 85%, 78%, 76%, respectively and in all cases was lowest during the cold start period.This report details the successfully proposed and assembled instrumentation that was relatively portable for field-site testing and the results of the emissions measurements for the 2018 Wood Stove Design Challenge competition. Overall, the repeatability of each stove was favorable with coefficients of variation (COV) ranging from 7 to 15% for measured PM concentrations.

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗
DOE OSTI2023

Electrochemical Reduction of Flue Gas Carbon Dioxide to Commercially Viable C2-C4 Products (Final Report)

This is the final scientific/technical report for a DOE project focused on the electrochemical conversion of CO 2 in non-aqueous solvents to novel products. Electrochemical reduction of CO 2 provides an attractive route to produce valuable fuels and chemicals that can simultaneously lower greenhouse gas emissions when powered by renewable electricity. While recent technological advances have shown the feasibility of industrial CO 2 electroreduction, many challenges remain to improve this technology and expand the list of economically viable products. The vast majority of electrochemical CO 2 reduction research has been conducted in aqueous media under neutral to alkaline conditions, leading to commonly reported products including carbon monoxide, formic acid, methane, methanol, ethylene, acetic acid, and ethanol. In comparison, non-aqueous media for CO 2 reduction has been underexplored but represents a possible avenue to yield new products and improved operating conditions. The aim of the project was to convert waste CO 2 in the form of flue gas to a multicarbon C2 - C4 chemical product in a reactor designed to achieve economically competitive values of current density and selectivity. The project strived to advance the technology readiness of an electrochemical CO 2 reduction process in alcohol solvents from the proof-of-concept stage to a device capable of meeting performance metrics for commercial viability. In the initial plan, the University of Louisville researchers were to focus on investigating the electrochemical process and improving the faradaic efficiency for novel C2 – C4 species, while also working on a parallel effort to build a practical electrolysis reactor to markedly increase the CO 2 reduction current density. The reactor development effort also aimed to engineer a dual-electrolyte feed strategy with non-aqueous catholyte and aqueous anolyte to promote water oxidation as the coupling anodic half-reaction to enable a sustainable and economical overall process. At the outset, the University of North Dakota was to investigate the feasibility of operating directly from coal-derived flue gas without separate capture and purification. The research team sought to determine impurity effects and test mitigation strategies, as well as engineer the gaseous feed system for high reactor tolerance to lower CO 2 concentration. In the last half year of the project, the focus was planned to shift to integrating the advances in the catalysis, electrochemical conditions, reactor design, and flue gas compatibility into a fully functional device and improve it for maximum current density and faradaic efficiency for C2 – C4 species. Knowledge of the full system components, constraints, and maximum performance was then to be used as the basis for a thorough technoeconomic analysis (TEA) and life cycle analysis (LCA) at the end of the project.

01 COAL, LIGNITE, AND PEAT↗
DOE OSTI2021

Fuel Stratification Influence on NO x Emission in a Premixed Axial Reacting Jet-in-Crossflow at High Pressure

Three reacting jet-in-crossflow (JiC) methane/air flames were numerically investigated in a lean axially staged combustor at a pressure of five atmospheres. A detailed chemistry Star-CCM+ computational fluid dynamics (CFD) model was used with 53 species considered and the result of turbulence-governed finite-rate modeling was validated with in-house experimental data. An optically accessible test section features three side windows, allowing local flow and flame analysis with particle image velocimetry (PIV) and CH* chemiluminescence as well as pressure, temperature, and species exit measurements. The research objective was to predict and verify NO x formation of the premixed 12.7 mm axial jet. Three headend temperature levels were investigated along with three premixed jets at lean (φ Jet = 0.75), near-stoichiometric (φ Jet = 1.07), and rich (φ Jet = 1.78) axial fuel line equivalence ratio. Based on the matching exit emission concentration, global emission benefits were investigated by adjustment of the fuel stratification. The perfectly premixed methane/air flames of this study were shown to ignite at the lee-side of the jet. For the elevated headend temperature level T = 1800 K, the flame extended beyond the windward jet trajectory and caused high axial NO production. For industry application, a firing temperature of 1920 K was achieved with a NO x optimized fuel split of 25%, combining a lean headend (φ Headend = 0.61) with a rich (φ Jet = 1.78) jet equivalence ratio. As a result, this operating point allowed minimization of the combustor residence time at temperatures above 1700 K as well as combustion in a compact flame at the jet lee-side along the counter rotating vortex pair.

03 NATURAL GAS↗
DOE OSTI2023

Climate warming and elevated CO 2 alter peatland soil carbon sources and stability

Peatlands are an important carbon (C) reservoir storing one-third of global soil organic carbon (SOC), but little is known about the fate of these C stocks under climate change. Here, we examine the impact of warming and elevated atmospheric CO 2 concentration (eCO 2 ) on the molecular composition of SOC to infer SOC sources (microbe-, plant- and fire-derived) and stability in a boreal peatland. We show that while warming alone decreased plant- and microbe-derived SOC due to enhanced decomposition, warming combined with eCO 2 increased plant-derived SOC compounds. We further observed increasing root-derived inputs (suberin) and declining leaf/needle-derived inputs (cutin) into SOC under warming and eCO 2 . The decline in SOC compounds with warming and gains from new root-derived C under eCO 2 , suggest that warming and eCO 2 may shift peatland C budget towards pools with faster turnover. Together, our results indicate that climate change may increase inputs and enhance decomposition of SOC potentially destabilising C storage in peatlands.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2024

The need for carbon-emissions-driven climate projections in CMIP7

Abstract. Previous phases of the Coupled Model Intercomparison Project (CMIP) have primarily focused on simulations driven by atmospheric concentrations of greenhouse gases (GHGs), for both idealized model experiments and climate projections of different emissions scenarios. We argue that although this approach was practical to allow parallel development of Earth system model simulations and detailed socioeconomic futures, carbon cycle uncertainty as represented by diverse, process-resolving Earth system models (ESMs) is not manifested in the scenario outcomes, thus omitting a dominant source of uncertainty in meeting the Paris Agreement. Mitigation policy is defined in terms of human activity (including emissions), with strategies varying in their timing of net-zero emissions, the balance of mitigation effort between short-lived and long-lived climate forcers, their reliance on land use strategy, and the extent and timing of carbon removals. To explore the response to these drivers, ESMs need to explicitly represent complete cycles of major GHGs, including natural processes and anthropogenic influences. Carbon removal and sequestration strategies, which rely on proposed human management of natural systems, are currently calculated in integrated assessment models (IAMs) during scenario development with only the net carbon emissions passed to the ESM. However, proper accounting of the coupled system impacts of and feedback on such interventions requires explicit process representation in ESMs to build self-consistent physical representations of their potential effectiveness and risks under climate change. We propose that CMIP7 efforts prioritize simulations driven by CO2 emissions from fossil fuel use and projected deployment of carbon dioxide removal technologies, as well as land use and management, using the process resolution allowed by state-of-the-art ESMs to resolve carbon–climate feedbacks. Post-CMIP7 ambitions should aim to incorporate modeling of non-CO2 GHGs (in particular, sources and sinks of methane and nitrous oxide) and process-based representation of carbon removal options. These developments will allow three primary benefits: (1) resources to be allocated to policy-relevant climate projections and better real-time information related to the detectability and verification of emissions reductions and their relationship to expected near-term climate impacts, (2) scenario modeling of the range of possible future climate states including Earth system processes and feedbacks that are increasingly well-represented in ESMs, and (3) optimal utilization of the strengths of ESMs in the wider context of climate modeling infrastructure (which includes simple climate models, machine learning approaches and kilometer-scale climate models).

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2021

An experimental and kinetic modeling study of NO x sensitization on methane autoignition and oxidation

An experimental and kinetic modeling study of the influence of NO x (i.e. NO 2 , NO and N 2 O) addition on the ignition behavior of methane/‘air’ mixtures is performed. Ignition delay time measurements are taken in a rapid compression machine (RCM) and in a shock tube (ST) at temperatures and pressures ranging from 900–1500 K and 1.5–3.0 MPa, respectively for equivalence ratios of 0.5–2.0 in ‘air’. The conditions chosen are relevant to spark ignition and homogeneous charge compression ignition engine operating conditions where exhaust gas recirculation can potentially add NO x to the premixed charge. The RCM measurements show that the addition of 200 ppm NO 2 to the stoichiometric CH 4 /oxidizer mixture results in a factor of three increase in reactivity compared to the baseline case without NOx for temperatures in the range 600–1000 K. However, adding up to 1000 ppm N 2 O does not show any appreciable effect on the measurements. The promoting effect of NO 2 was found to increase with temperature in the range 950–1150 K, while the sensitization effect decreases at higher pressures. The experimental results measured are simulated using NUIGMech1.2 comprising an updated NO x sub-chemistry in this work. A kinetic analysis indicates that the competition between the reactions ĊH 3 + NO 2 ↔ CH 3 Ȯ + NO and ĊH 3 + NO 2 (+M) ↔ CH 3 NO 2 (+M), the former being a propagation reaction and the latter being a termination reaction governs NO x sensitization on CH 4 ignition. Recent calculations by Matsugi and Shiina (A. Matsugi, H. Shiina, J. Phys. Chem. A. 121 (2017) 4218–4224) for the nitromethane formation reaction CH 3 + NO 2 (+M) ↔ CH 3 NO 2 (+M), together with the recently calculated rate constants for HONO/HNO 2 reactions significantly improve ignition delay time predictions in the temperature range 600–1000 K. Furthermore, the experiments with NO addition reveal a non-monotonous sensitization impact on CH 4 ignition at lower temperatures with NO initially acting as an inhibitor at low NO concentrations and then as a promoter as NO concentrations increase in the mixture. This non-monotonous trend is attributed to the role of the chain-termination reaction ĊH 3 + NO 2 (+M) ↔ CH 3 NO 2 (+M) and the impact of NO on the transition to the chain-branching steps CH 2 O + HȮ 2 ↔ HĊO + H 2 O 2 , H 2 O 2 (+M) ↔ ȮH + ȮH (+M), HĊO ↔ CO + Ḣ followed by CO + O 2 ↔ CO 2 + Ö and Ḣ + O 2 ↔ Ö + ȮH. NUIGMech1.2 is systematically validated against the new ignition delay measurements taken here together with species measurements and high temperature ignition delay time data available in the literature for CH 4 /oxidizer mixtures diluted with NO 2 /N 2 O/NO and is observed to accurately capture the sensitization trends.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗