Search NASA⌕ Search

SEARCH · Search NASA

Results for “N2O emission”

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

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

46 records · Page 3

Nitrous oxide reduction by two partial denitrifying bacteria requires denitrification intermediates that cannot be respired

ABSTRACT Denitrification is a form of anaerobic respiration wherein nitrate (NO 3 − ) is sequentially reduced via nitrite (NO 2 − ), nitric oxide, and nitrous oxide (N 2 O) to dinitrogen gas (N 2 ) by four reductase enzymes. Partial denitrifying bacteria possess only one or some of these four reductases and use them as independent respiratory modules. However, it is unclear if partial denitrifiers sense and respond to denitrification intermediates outside of their reductase repertoire. Here, we tested the denitrifying capabilities of two purple nonsulfur bacteria,Rhodopseudomonas palustrisCGA0092 andRhodobacter capsulatusSB1003. Each had denitrifying capabilities that matched their genome annotation; CGA0092 reduced NO 2 − to N 2 , and SB1003 reduced N 2 O to N 2 . For each bacterium, N 2 O reduction could be used both for electron balance during growth on electron-rich organic compounds in light and for energy transformation via respiration in darkness. However, N 2 O reduction required supplementation with a denitrification intermediate, including those for which there was no associated denitrification enzyme. For CGA0092, NO 3 − served as a stable, non-catalyzable molecule that was sufficient to activate N 2 O reduction. Using a β-galactosidase reporter, we found that NO 3 − acted, at least in part, by stimulating N 2 O reductase gene expression. In SB1003, NO 2 − but not NO 3 − activated N 2 O reduction, but NO 2 − was slowly removed, likely by a promiscuous enzyme activity. Our findings reveal that partial denitrifiers can still be subject to regulation by denitrification intermediates that they cannot use. IMPORTANCE Denitrification is a form of microbial respiration wherein nitrate is converted via several nitrogen oxide intermediates into harmless dinitrogen gas. Partial denitrifying bacteria, which individually have some but not all denitrifying enzymes, can achieve complete denitrification as a community by cross-feeding nitrogen oxide intermediates. However, the last intermediate, nitrous oxide (N2O), is a potent greenhouse gas that often escapes, motivating efforts to understand and improve the efficiency of denitrification. Here, we found that at least some partial denitrifying N2O reducers can sense and respond to nitrogen oxide intermediates that they cannot otherwise use. The regulatory effects of nitrogen oxides on partial denitrifiers are thus an important consideration in understanding and applying denitrifying bacterial communities to combat greenhouse gas emissions.

Biotechnology & Applied Microbiology↗

Dynamics of N 2 O in vicinity of plant residues: a microsensor approach

Plant residues decomposing within the soil matrix are known to serve as hotspots of N 2 O production. However, the lack of technical tools for microscale in-situ N 2 O measurements limits understanding of hotspot functioning. Our aim was to assess performance of microsensor technology for evaluating the temporal patterns of N 2 O production in immediate vicinity to decomposing plant residues. We incorporated intact switchgrass leaves and roots into soil matrix and monitored O 2 depletion and N 2 O production using electrochemical microsensors along with N 2 O emission from the soil. We also measured residue’s water absorption and b-glucosidase activity on the surface of the residue - the characteristics related to microenvironmental conditions and biological activity near the residue. N 2 O production in the vicinity of switchgrass residues began within 0–12 h after the wetting, reached peak at ~0.6 day and decreased by day 2. N 2 O was higher near leaf than near root residues due to greater leaf N contents and water absorption by the leaves. However, N 2 O production near the roots started sooner than near the leaves, in part due to high initial enzyme levels on root surfaces. Electrochemical microsensor is a useful tool for in-situ micro-scale N 2 O monitoring in immediate vicinity of soil incorporated plant residues. Monitoring provided valuable information on N 2 O production near leaves and roots, its temporal dynamic, and the factors affecting it. The N 2 O production from residues measured by microsensors was consistent with the N 2 O emission from the whole soil, demonstrating the validity of the microsensors for N 2 O hotspot studies.

59 BASIC BIOLOGICAL SCIENCES↗

Chamber Flux and Porewater Concentration of CH4, CO2 and N2O, 2018, Columbia River bank at the Hanford site, WA, USA

This is the corresponding observations data for the paper: Jorge A Villa; Garrett J Smith; Yang Ju; Lupita Renteria; Jordan C Angle; Evan Arntzen; Samuel F Harding; Huiying Ren; Xingyuan Chen; Audrey H Sawyer; Emily B Graham; James C Stegen; Kelly C Wrighton; Gil Bohrer (2020) Methane and nitrous oxide porewater concentrations and surface fluxes of a regulated river. Science of the Total Environment.Greenhouse gas (GHG) emissions from rivers are a critical missing component of current global GHG models. Their exclusion is mainly due to a lack of in-situ measurements and a poor understanding of the spatiotemporal dynamics of GHG production and emissions, which prevents optimal model parametrization. We combined simultaneous observations of porewater concentrations along different beach positions and depths, and surface fluxes of methane and nitrous oxide at a plot scale in a large regulated river during three water stages: rising, falling, and low. Our goal was to gain insights into the interactions between hydrological exchanges and GHG emissions and elucidate possible hypotheses that could guide future research on the mechanisms of GHG production, consumption, and transport in the hyporheic zone (HZ). Results indicate that the site functioned as a net source of methane. Surface fluxes of methane during river water stages at three beach positions (shallow, intermediate and deep) correlated with porewater concentrations of methane. However, fluxes were significantly higher in the intermediate position during the low water stage, suggesting that low residence time increased methane emissions. Vertical profiles of methane peaked at different depths, indicating an influence of the magnitude and direction of the hyporheic mixing during the different river water stages on methane production and consumption. The site acted as either a sink or a source of nitrous oxide depending on the elevation of the water column. Nitrous oxide porewater concentrations peaked at the upper layers of the sediment throughout the different water stages. River hydrological stages significantly influenced porewater concentrations and fluxes of GHG, probably by influencing heterotrophic respiration (production and consumption processes) and transport to and from the HZ. Our results highlight the importance of including dynamic hydrological exchanges when studying and modeling GHG production and consumption in the HZ of large rivers.

54 ENVIRONMENTAL SCIENCES↗

Project Development of an Electrochemical Denitration and Caustic Generation System for HLW Pretreatment at Hanford - 26350

An engineering-scale electrochemical processing skid is proposed to perform the denitration of Hanford tank waste, which would help to mitigate a key process concern with the direct feed processing of the Hanford Tank Waste Treatment and Immobilization Plant (WTP). The reduction of nitrates and organic compounds in the waste feed will directly reduce hazardous NOx and ammonia gases generated during the vitrification process, which in turn will aid in addressing potential regulatory and safety challenges associated with processing large volumes of tank waste. This paper highlights the past legacy work, project layout, accomplishments from Phase 1 and research and development envisioned for Phase 2. An innovative electrochemical denitration and caustic generation (EDCGe) process was demonstrated for the pretreatment of tank waste at the Savannah River Site (SRS) in the early 2000s. The denitration electrolyzer, off-gas abatement system, and caustic generator electrolyzer are being developed with the intent that the denitration electrolyzer will convert nitrate and nitrite anions to nitrogen gas while also yielding other gaseous byproducts, which may include N2O, NH3, VOCs, and H2. The gaseous byproducts will be managed via a tandem off-gas catalyst-bed treatment system. The caustic generation electrolyzer will recycle NaOH from the feed to produce a clean caustic stream for use within the batching tanks at Hanford, aiding in the preparation of waste for WTP. The reduction in hazardous emissions and improved waste treatment processes provides a robust solution for nuclear waste management, contributing to environmental safety and regulatory compliance. The EDCGe technology is being adapted, modified, and updated for the preparation of the Direct Feed-High Level Waste (DF-HLW) flowsheet at Hanford. Phase 1 demonstrated a bench-scale proof-of-concept for reactions involving the denitration electrolyzer and gas phase abatement of ammonia. The electrochemical technology is drawing on the scientific outcomes that were reported in the legacy work. The results from Phase 1 demonstrated the viability of the EDCGe system in reducing the nitrogen species of simple non-radioactive waste simulants. Commercially available alloys used as electrode materials and membranes are being studied for the denitration and caustic generation electrolyzers. The continuation of this project holds promise for broader applications, such as energy-efficient ammonia production, and contributes significant advancements in nuclear waste management. Additional material discovery has been investigated into ceramic Na super ion conductive (NaSICON) materials and off-gas abatement catalyst discovery. NaSICON is of interest for selective transport of Na within the electrolyzers to make a clean caustic stream. Future integration and optimization efforts, informed by Phase 1 results and ongoing research, will continue to drive advancements in nuclear waste management technology. The technology developed for the EDCGe treatment of tank waste will also have broader potential to inform other fields, such as energy-efficient ammonia production, as well as ammonia abatement catalysis through the lessons learned in electrochemical nitrate reduction. The applications and benefits of this research extend beyond Hanford and the Savannah River Site, supported by a collaborative team of scientists and engineers from national labs, academia, and industry, ensuring a comprehensive approach to solving complex waste treatment challenges. The team is leveraging advanced electrochemical technologies, machine learning, novel catalysts tailored for gaseous nitrogen species, and cutting-edge reactor systems to enhance the process efficiency and effectiveness of the denitration process.

Rodene, Dylan [Savannah River National Laboratory ↗

Economizing on Precious Metals in Three-Way Catalysts: Thermally Stable and Highly Active Single-Atom Rhodium on Cera for NO Abatement under Dry and Industrially Relevant Conditions

We show for the first time that atomically dispersed Rh cations on ceria, prepared via high-temperature atom trapping synthesis, are the active species for (CO+NO) reaction. This provides a direct link with the organometallic homogeneous Rh(I) complexes capable of catalyzing dry (CO+NO) reaction but without the stability concern. In particular, thermally stable Rh cations in 0.1wt% Rh1/CeO2 achieve full NO conversion with a TOF of ~ 330 hr-1 per Rh atom at 120 °C. Under dry conditions, the main product above 100 °C is N2 with N2O being the minor product. The presence of water promotes low-temperature activity of 0.1wt% Rh1/CeO2 starting at 50 °C with full NO conversion at ~120 °C. In the case with the wet stream, however, ammonia and nitrogen are the main products with only minor N2O amounts. NH3 formation at such low temperatures is attractive because of the potential to use this as a passive SCR system. Because of the uniformity of Rh ions on the support, we are able to observe the intermediates of (CO+NO) reaction via infrared measurements on Rh cations on zeolite and ceria. Furthermore, we show that ammonia formation correlates with the WGS activity of the material and thus, rhodium hydride Rh-H species are involved in this reaction: we detect Rh(CO)Hx species on ceria using isotopic IR measurements. These findings provide new mechanistic understanding for the catalytically active species in TWC catalysis and open up a new avenue for the synthesis of novel emissions control catalysts with 100% atom economy of ultra-expensive precious metals such as Rh.

Khivantsev, Konstantin↗

Changes in soil pore structure generated by the root systems of maize , sorghum and switchgrass affect in situ N 2 O emissions and bacterial denitrification

Due to the heterogeneous nature of soil pore structure, processes such as nitrification and denitrification can occur simultaneously at microscopic levels, making prediction of small-scale nitrous oxide (N 2 O) emissions in the field notoriously difficult. We assessed N 2 O+N 2 emissions from soils under maize (Zea mays L.), switchgrass (Panicum virgatum L.), and energy sorghum (Sorghum bicolor L.), three potential bioenergy crops in order to identify the importance of different N 2 O sources to microsite production, and relate N 2 O source differences to crop-associated differences in pore structure formation. The combination of isotopic surveys of N 2 O in the field during one growing season and X-ray computed tomography (CT) enabled us to link results from isotopic mappings to soil structural properties. Further, our methodology allowed us to evaluate the potential for in situ N 2 O suppression by biological nitrification inhibition (BNI) in energy sorghum. Our results demonstrated that the fraction of N 2 O originating from bacterial denitrification and reduction of N 2 O to N 2 is largely determined by the volume of particulate organic matter occluded within the soil matrix and the anaerobic soil volume. Bacterial denitrification was greater in switchgrass than in the annual crops, related to changes in pore structure caused by the coarse root system. This led to high N-loses through N 2 emissions in the switchgrass system throughout the season a novel finding given the lack of data in the literature for total denitrification. Isotopic mapping indicated no differences in N 2 O-fluxes or their source processes between maize and energy sorghum that could be associated with the release of BNI by the investigated sorghum variety. The results of this research show how differences in soil pore structures among cropping systems can determine both N 2 O production via denitrification and total denitrification N losses in situ.

59 BASIC BIOLOGICAL SCIENCES↗

N 2 O Formation Mechanism and Suppression Strategy on Pt Catalysts for NO x Removal from Hydrogen-Internal Combustion Engines

Pt-based catalysts exhibit excellent low-temperature activity in the selective catalytic reduction of NO x with H 2 (H 2 -SCR), but their tendency to form N 2 O poses a significant challenge for practical use. This issue is further complicated by unclear formation mechanisms, hindering the development of more efficient catalysts. This study explored the N 2 O generation mechanisms on Pt catalysts supported by MgO, Al 2 O 3 , SiO 2 , and TiO 2 , aiming to achieve a deep understanding that could advance the Pt catalysts with high NO x conversion and minimized N 2 O emissions. Through systematic kinetics and characterization analyses, the direct influence of the support acidity and reactant dynamics (O 2 and NO) on N 2 O formation was clearly revealed. Notably, the Pt catalysts with strong NO adsorption capacity showed reduced N 2 O generation, highlighting the critical role of NO adsorption sites in the H 2 -SCR process. By incorporation of NO adsorption sites (i.e., MgO, BaO, CeO 2 ) onto Pt/SiO 2 , both the H 2 -SCR efficiency and N 2 selectivity (reduced N 2 O selectivity) were significantly enhanced, effectively reducing the N 2 O emissions through optimized surface NO adsorption. These findings provide a design framework for more selective Pt-based catalysts, advancing H 2 -SCR systems for effective NO x abatement from hydrogen-internal combustion engines, which is a promising carbon-free transportation technology.

36 MATERIALS SCIENCE↗

Establishing Validation Sites for Field-Level Emissions Quantification from Grain Sorghum in Southern Great Plains

Establish publicly available open-source, high-resolution datasets of greenhouse gas (GHG) emissions, meteorology, soil, and vegetation to support testing and validation of emerging biofuel production monitoring technologies. The project team deployed latest technologies to collect “Gold Standard” data for field- level fluxes of CO 2 , N 2 O, CH 4 and H 2 O in grain sorghum production systems in Texas, Oklahoma, and Kansas. The Oklahoma State University led SMARTFARM was initiated on Oct 1, 2020, due to COVID-19 pandemic delay. We installed closed-path dual laser Eddy Covariance (EC) flux measurement system along with a well-established open-path EC system for simultaneously measuring field-level fluxes of CO 2 , N 2 O, CH 4 , and H2O. The eddy flux data are combined with sub-acre soil moisture and temperature measurements, plant and soil analysis data (nutrient, composition, carbon, growth, and phenology), spatial surveys of soil EC, and pH. Grain sorghum crop was managed including planting and harvesting by producers. All teams recruited postdocs and students for the project and submitted purchase orders for field equipment. The team has developed a draft impact sheet and finalized the advisory board for the project.

09 BIOMASS FUELS↗

Chemical identity of carbon substrates drives differences in denitrification and N 2 O reduction within agricultural soils

Rates of nitrous oxide (N 2 O) production from agricultural soils are highly variable across space and time. Improving predictions of N 2 O emissions will require improving our understanding of the drivers of denitrification and the sources of variability in the rates of N 2 O production between soils and over time. While the amount of available carbon (C) is a known control on denitrification and N 2 O reduction, relatively little attention has been paid to the effect of the chemical identity of C substrates on rates of denitrification and N 2 O reduction. We investigated the effects of twelve different C-substrate additions on the production and reduction of N 2 O in five soils taken from two distinct agricultural locations in Michigan under multiple land uses. We provided additions of glucose, cellulose, N-acetyl-glucosamine, chitin, amino acids, protein, vanillyl alcohol, lignin, citrate, succinate, methanol, and water in laboratory denitrification potential assays to determine the effects of denitrifier C preference on denitrification rates. We found that amino acids, protein, and organic acids stimulated the greatest rates of denitrification potential across all land uses. Similarly, we found these same substrates caused the most N 2 O reduction, resulting in the lowest net concentrations of N 2 O. Soils from agricultural rotations without cover crops had overall lower rates of denitrifier activity, leading to less net N 2 O production compared to soils from other land uses. In general, C-utilization patterns were similar among all soils, and C-substrate identity had a much stronger effect than land use. Here, we demonstrate that the chemical identity of available C gives rise to wide variability in rates of denitrification and N 2 O reduction.

60 APPLIED LIFE SCIENCES↗

N 2 Onet: a global collaborative network facilitating advances in measurement, modeling, and mitigation of agricultural soil nitrous oxide emissions

Nitrogen (N) fertilizer supports global food production, but its use and overuse drive emissions of nitrous oxide (N 2 O), a potent and long-lived greenhouse gas. Understanding the drivers of N 2 O fluxes remains elusive, making it difficult to predict emissions in time and space and to develop and evaluate ways to lower emissions through management. Major scientific uncertainties underlying the understanding of the drivers of N 2 O fluxes identified in a workshop of N 2 O emissions experts include poor process-based understanding of controls on soil N 2 O emissions in the field; insufficient data to reduce uncertainty in N 2 O budgets from the field to regional scales, including N 2 O emission measurements and importantly, field-scale N balances; and high uncertainty in model predictions of soil N 2 O emissions across environmental and management conditions. To reduce these uncertainties, we present the concept of N 2 Onet, a global collaborative initiative to accelerate advances in N 2 O measurement, analyses, and mitigation. N 2 Onet will serve as an observational network of supersites with multi-scale measurements; a database hub for N 2 O flux and ancillary data; and a catalyst for community building, information sharing, and training. By coalescing and coordinating the global community of researchers, N 2 Onet will provide a roadmap for reducing N 2 O emissions from agriculture worldwide.

54 ENVIRONMENTAL SCIENCES↗