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At least 19 records
All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

Beyond denitrification: The role of microbial diversity in controlling nitrous oxide reduction and soil nitrous oxide emissions

Many biotic and abiotic processes contribute to nitrous oxide (N 2 O) production in the biosphere, but N 2 O consumption in the environment has heretofore been attributed primarily to canonical denitrifying microorganisms. The nosZ genes encoding the N 2 O reductase enzyme, NosZ, responsible for N 2 O reduction to dinitrogen are now known to include two distinct groups: the well-studied Clade I which denitrifiers typically possess, and the novel Clade II possessed by diverse groups of microorganisms, most of which are non-denitrifiers. Clade II N 2 O reducers could play an important, previously unrecognized role in controlling N 2 O emissions for several reasons, including: (1) the consumption of N 2 O produced by processes other than denitrification, (2) hypothesized non-respiratory functions of NosZ as an electron sink or for N 2 O detoxification, (3) possible differing enzyme kinetics of Clade II NosZ compared to Clade I NosZ, and (4) greater nosZ gene abundance for Clade II compared to Clade I in soils of many ecosystems. Despite the potential ecological significance of Clade II NosZ, a census of 800 peer-reviewed original research articles discussing nosZ and published from 2013 to 2019 showed that the percentage of articles evaluating or mentioning Clade II nosZ increased from 5% in 2013 to only 22% in 2019. The census revealed that the slowly spreading awareness of Clade II nosZ may result in part from disciplinary silos, with the percentage of nosZ articles mentioning Clade II nosZ ranging from 0% in Agriculture and Agronomy journals to 32% in Multidisciplinary Sciences journals. In addition, inconsistent nomenclature for Clade I nosZ and Clade II nosZ, with 17 different terminologies used in the literature, may have created confusion about the two distinct groups of N 2 O reducers. Furthermore, we provide recommendations to accelerate advances in understanding the role of the diversity of N 2 O reducers in regulating soil N 2 O emissions.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2024

Contribution of Microorganisms with the Clade II Nitrous Oxide Reductase to Suppression of Surface Emissions of Nitrous Oxide

The sources and sinks of nitrous oxide, as control emissions to the atmosphere, are generally poorly constrained for most environmental systems. Initial depth-resolved analysis of nitrous oxide flux from observation wells and the proximal surface within a nitrate contaminated aquifer system revealed high subsurface production but little escape from the surface. Further, to better understand the environmental controls of production and emission at this site, we used a combination of isotopic, geochemical, and molecular analyses to show that chemodenitrification and bacterial denitrification are major sources of nitrous oxide in this subsurface, where low DO, low pH, and high nitrate are correlated with significant nitrous oxide production. Depth-resolved metagenomes showed that consumption of nitrous oxide near the surface was correlated with an enrichment of Clade II nitrous oxide reducers, consistent with a growing appreciation of their importance in controlling release of nitrous oxide to the atmosphere. Our work also provides evidence for the reduction of nitrous oxide at a pH of 4, well below the generally accepted limit of pH 5.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Post-fire soil emissions of nitric oxide (NO) and nitrous oxide (N 2 O) across global ecosystems: a review

Wildfires may increase soil emissions of trace nitrogen (N) gases like nitric oxide (NO) and nitrous oxide (N 2 O) by changing soil physicochemical conditions and altering microbial processes like nitrification and denitrification. When 34 studies were synthesized, we found a significant increase in both NO and N 2 O emissions up to 1 year post-fire across studies spanning ecosystems globally. However, when fluxes were separated by ecosystem type, we found that individual ecosystem types responded uniquely to fire. Forest soils tended to emit more N 2 O after fire, but there was no significant effect on NO. Shrubland soils showed significant increases in both NO and N 2 O emissions after fires; often with extremely large but short-lived NO pulses occurring immediately after fire. Grassland NO emissions increased after fire, but the size of this effect was small relative to shrublands. N 2 O emissions from burned grasslands were highly variable with no significant effect. To better understand the variation in responses to fire across global ecosystems, more consistent measurements of variables recognized as important controls on soil fluxes of NO and N 2 O (e.g., N cycling rates, soil water content, pH, and substrate availability) are needed across studies. We also suggest that fire-specific elements like burn severity, microbial community succession, and the presence of char be considered by future studies. Our synthesis suggests that fires can exacerbate ecosystem N loss long after they burn, increasing soil emissions of NO and N 2 O with implications for ecosystem N loss, climate, and regional air quality as wildfires increase globally.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Selective Electrocatalytic Reduction of Nitrous Oxide to Dinitrogen with an Iron Porphyrin Complex

Nitrous oxide (N 2 O) is the third largest contributor to anthropogenic greenhouse gas emissions and plays a detrimental role in the depletion of ozone. Despite the contribution of N 2 O as an atmospheric pollutant, there are currently only a few examples of electrochemical N 2 O remediation to N 2 . Herein we report the electrocatalytic deoxygenation of N 2 O by iron tetraphenylporphyrin (FeTPP) to form N 2 with quantitative Faradaic efficiency and an observed rate of 1.91 s –1 . No degradation was observed after controlled potential electrolysis. Mechanistic investigation of the proposed catalytic steps determined that hydrogen-bond donors are critical for accelerating N 2 O activation and that proton transfer is involved in the rate-determining step.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2018

Inverse Estimation of an Annual Cycle of California's Nitrous Oxide Emissions

Nitrous oxide (N 2 O) is a potent long-lived greenhouse gas (GHG) and the strongest current emissions of global anthropogenic stratospheric ozone depletion weighted by its ozone depletion potential. In California, N 2 O is the third largest contributor to the state's anthropogenic GHG emission inventory, though no study has quantified its statewide annual emissions through top-down inverse modeling. Here we present the first annual (2013–2014) statewide top-down estimates of anthropogenic N 2 O emissions. Utilizing continuous N 2 O observations from six sites across California in a hierarchical Bayesian inversion, we estimate that annual anthropogenic emissions are 1.5–2.5 times (at 95% confidence) the state inventory (41 Gg N 2 O in 2014). Without mitigation, this estimate represents 4–7% of total GHG emissions assuming that other reported GHG emissions are reasonably correct. This suggests that control of N 2 O could be an important component in meeting California's emission reduction goals of 40% and 80% below 1990 levels of the total GHG emissions (in CO 2 equivalent) by 2030 and 2050, respectively. Finally, our seasonality analysis suggests that emissions are similar across seasons within posterior uncertainties. Future work is needed to provide source attribution for subregions and further characterization of seasonal variability.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2025

A novel bacterial protein family that catalyses nitrous oxide reduction

Nitrous oxide (N 2 O), a driver of global warming and climate change, has reached unprecedented concentrations in Earth’s atmosphere. Current N 2 O sources outpace N 2 O sinks, emphasizing the need for comprehensive understanding of processes that consume N 2 O. Microbes that express the enzyme N 2 O reductase (N 2 OR) convert N 2 O to climate change-neutral dinitrogen (N 2 ). Known N 2 ORs belong to the canonical clade I and clade II NosZ reductases and are considered key enzymes for N 2 O reduction. Here we report a previously unrecognized protein family with a role in N 2 O reduction, clade III lactonase-type N 2 OR (L-N 2 OR), which diverges in sequence from canonical NosZ but conserves three-dimensional protein structural features. Integrated physiological, metagenomic, proteomic and structural modelling studies demonstrate that L-N 2 ORs catalyse N 2 O reduction. L-N 2 OR genes occur in several phyla, predominantly in uncultured taxa with broad geographic distribution. Our findings expand the known diversity of N 2 ORs and implicate previously unrecognized taxa (for example, Nitrospinota) in N 2 O consumption. In conclusion, the expansion of N 2 OR diversity and the identification of a novel type of catalyst for N 2 O reduction advances the understanding of N 2 O sinks, has implications for greenhouse gas emission and climate change modelling, and expands opportunities for innovative biotechnologies aimed at curbing N 2 O emissions.

He, Guang 何广 [Univ. of Tennessee, Knoxville, TN (U↗
DOE OSTI2021

Bedrock weathering contributes to subsurface reactive nitrogen and nitrous oxide emissions

Atmospheric nitrous oxide contributes directly to global warming, yet models of the nitrogen cycle do not account for bedrock, the largest pool of terrestrial nitrogen, as a source of nitrous oxide. Although it is known that release rates of nitrogen from bedrock are large, there is an incomplete understanding of the connection between bedrock-hosted nitrogen and atmospheric nitrous oxide. Here, we quantify nitrogen fluxes and mass balances at a hillslope underlain by marine shale. We found that, at this site, bedrock weathering contributes 78% of the subsurface reactive nitrogen, while atmospheric sources (commonly regarded as the sole sources of reactive nitrogen in pristine environments) account for only the remaining 22%. About 56% of the total subsurface reactive nitrogen denitrifies, including 14% emitted as nitrous oxide. The remaining reactive nitrogen discharges in porewaters to a floodplain where additional denitrification probably occurs. We also found that the release of bedrock nitrogen occurs primarily within the zone of the seasonally fluctuating water table and suggest that the accumulation of nitrate in the vadose zone, often attributed to fertilization and soil leaching, may also include contributions from weathered nitrogen-rich bedrock. Our hillslope study suggests that, under oxygenated and moisture-rich conditions, weathering of deep, nitrogen-rich bedrock makes an important contribution to the nitrogen cycle.

58 GEOSCIENCES↗
DOE OSTI2021

The influence of tillage and fertilizer on the flux and source of nitrous oxide with reference to atmospheric variation using laser spectroscopy

Nitrous oxide (N 2 O) is the third most important long-lived greenhouse gas and agriculture is the largest source of N 2 O emissions. Curbing N 2 O emissions requires understanding influences on the flux and sources of N 2 O. We measured flux and evaluated microbial sources of N 2 O using site preference ( S P ; the intramolecular distribution of 15 N in N 2 O) in flux chambers from a grassland tilling and agricultural fertilization experiments and atmosphere. We identified values greater than that of the average atmosphere to reflect nitrification and/or fungal denitrification and those lower than atmosphere as increased denitrification. Our spectroscopic approach was based on an extensive calibration with 18 standards that yielded S P accuracy and reproducibility of 0.7 ‰ and 1.0 ‰, respectively, without preconcentration. Chamber samples from the tilling experiment taken ~ monthly over a year showed a wide range in N 2 O flux (0–1.9 g N 2 O-N ha -1 d -1 ) and S P (- 1.8 to 25.1 ‰). Flux and S P were not influenced by tilling but responded to sampling date. Large fluxes occurred in October and May in no-till when soils were warm and moist and during a spring thaw, an event likely representing release of N 2 O accumulated under snow cover. These high fluxes could not be ascribed to a single microbial process as S P differed among chambers. However, the year-long S P and flux data for no-till showed a slight direct relationship suggesting that nitrification increased with flux. The comparative data in till showed an inverse relationship indicating that high flux events are driven by denitrification. Corn ( Zea mays ) showed high fluxes and S P values indicative of nitrification ~ 4 wk after fertilization with subsequent declines in S P indicating denitrification. Although there was no effect of fertilizer treatment on flux or S P in switchgrass ( Panicum virgatum) , high fluxes occurred ~1 month after fertilization. In both treatments, S P was indicative of denitrification in many instances, but evidence of nitrification/fungal denitrification also prevailed. At 2 m atmospheric N 2 O S P had a range of 31.1 ‰ and 14.6 ‰ in the grassland tilling and agricultural fertilization experiments, respectively. These data suggest the influence of soil microbial processes on atmospheric N 2 O and argue against the use of the global average atmospheric S P in isotopic modeling approaches.

Environmental Sciences & Ecology↗
DOE OSTI2022

Effects of Vegetation on Fluxes of Nitric Oxide, Nitrogen Dioxide, and Nitrous Oxide in a Mixed Deciduous Forest Clearing

Atmosphere-terrestrial exchange of nitrogen oxides, such as nitric oxide (NO), nitrogen dioxide (NO2) and nitrous oxide (N2O), plays an important role in controlling atmospheric composition and the radiative forcing of Earth’s atmosphere. In this study, the impact of vegetation ground cover on NOx (NOx = NO + NO2) and N2O fluxes in a deciduous forest clearing was studied using dynamic flow chambers located on three experimental plots with differing vegetation ground cover. Microbial emissions of NO and N2O were observed throughout the measurement period, while NO2 was exclusively deposited. Vegetation had no observable impact on NO2 deposition. Under dry conditions, total measured nitrogen emissions were numerically similar across all plots, although the N2O:NO ratio was higher for plots containing plants. Vegetation elevates soil water content through enhanced water retention, a condition that favors denitrification and more N2O production, relative to NO. Two rain events induced pulses of NO and N2O that were higher for bare soil compared to the vegetated plots. Lower NO and N2O emissions in plant-containing chambers stemmed from enhanced root uptake of N following rewetting, which diminished the amount of N substrate available for microbial NO and N2O production. The sensitivity of soil N emissions to vegetation ground cover highlights the need for more studies that investigate this effect over a wide range of ecosystems and to include vegetation effects in future parameterizations of soil NOx and N2O used in atmospheric models. This dataset includes processed data collected from 4 dynamic flux chambers and 17 sensors. Data includes ambient gas measurements made 1 m from the surface and soil flux measurements of NO, NO2, N2O, ozone (O3) and carbon dioxide (CO2). Also included is a suite of meteorological (air temperature, humidity, pressure) and soil parameters (water filled pore space, soil temperature). Refer to the readme for more information about each of the data sets.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2024

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↗
DOE OSTI2022

Lewis acid-assisted reduction of nitrite to nitric and nitrous oxides via the elusive nitrite radical dianion

Reduction of nitrite anions (NO 2 - ) to nitric oxide (NO), nitrous oxide (N 2 O) and ultimately dinitrogen (N 2 ) takes place in a variety of environments, including in the soil as part of the biogeochemical nitrogen cycle and in acidified nuclear waste. Nitrite reduction typically takes place within the coordination sphere of a redox-active transition metal. In this report we show that Lewis acid coordination can substantially modify the reduction potential of this polyoxoanion to allow for its reduction under non-aqueous conditions (-0.74 V versus NHE). Detailed characterization confirms the formation of the borane-capped radical nitrite dianion (NO 2 2- ), which features a N(II) oxidation state. Protonation of the nitrite dianion results in the facile loss of nitric oxide (NO), whereas its reaction with NO results in disproportionation to nitrous oxide (N 2 O) and nitrite (NO 2 - ). This system connects three redox levels in the global nitrogen cycle and provides fundamental insights into the conversion of NO 2 - to NO.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2016

Nitrosomonas europaea cytochrome P460 is a direct link between nitrification and nitrous oxide emission

Significance Nitrous oxide (N 2 O) is a potent ozone-depleting greenhouse gas. This work identifies a means by which N 2 O is generated during nitrification, or biological ammonia oxidation. Fertilizer use in agriculture stimulates nitrification, thus increasing the volume of N 2 O emissions worldwide. The results presented herein will inform models and strategies toward optimized, sustainable agriculture. Moreover, these results highlight a rare example of biological N–N bond formation.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2017

Portable nitrous oxide sensor for understanding agricultural and soil emissions

Nitrous oxide (N2O) is the third most important greenhouse gas (GHG,) with an atmospheric lifetime of ~114 years and a global warming impact ~300 times greater than that of carbon dioxide. The main cause of nitrous oxide’s atmospheric increase is anthropogenic emissions, and over 80% of the current global anthropogenic flux is related to agriculture, including associated land-use change. An accurate assessment of N2O emissions from agriculture is vital not only for understanding the global N2O balance and its impact on climate but also for designing crop systems with lower GHG emissions. Such assessments are currently hampered by the lack of instrumentation and methodologies to measure ecosystem-level fluxes at appropriate spatial and temporal scales. Southwest Sciences and Princeton University are developing and testing new open-path eddy covariance instrumentation for continuous and fast (10 Hz) measurement of nitrous oxide emissions. An important advance, now being implemented, is the use of new mid-infrared laser sources that enable the development of exceptionally low power (<10 W) compact instrumentation that can be used even in remote sites lacking in power. The instrumentation will transform the ability to measure and understand ecosystem-level nitrous oxide fluxes. The Phase II results included successful extended field testing of prototype flux instruments, based on quantum cascade lasers, in collaboration with Michigan State University. Results of these tests demonstrated a flux detection limit of 5 µg m-2 s-1 and showed excellent agreement and correlation with measurements using chamber techniques. Initial tests of an instrument using an interband cascade laser (ICL) were performed, verifying that an order of magnitude reduction in instrument power requirements can be realized. These results point toward future improvements and testing leading to introduction of a commercial open path instrument for N2O flux measurements that is truly portable and cost-effective. The technology developed on this project is especially groundbreaking as it could be widely applied across FLUXNET and AmeriFlux sites (>1200 worldwide) for direct measurements of N2O exchange. The technology can be more broadly applied to gas monitoring requirements in industry, environmental monitoring, health and safety, etc.

47 OTHER INSTRUMENTATION↗
DOE OSTI2016

KCMP Minnesota Tall Tower Nitrous Oxide Inverse Modeling Dataset 2010-2015

This data set contains nitrous oxide mixing ratios and supporting information measured at a tall tower (KCMP, 244 meter) site near St. Paul, Minnesota, USA. The data include nitrous oxide and carbon dioxide mixing ratios measured at the 100 meter level. Turbulence and wind data were measured using a sonic anemometer at the 185 meter level. Also included in this data set are estimates of the “background” nitrous oxide mixing ratios. This data was collected to improve understanding of the reactive nitrogen budget for the region.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2021

Bedrock weathering rates, reactive nitrogen influxes and effluxes, and nitrous oxide emissions rates from the Pumphouse Hillslope, East River Watershed, Colorado

Atmospheric nitrous oxide contributes directly to global warming, yet models of the nitrogen cycle do not account for bedrock, the largest pool of terrestrial nitrogen, as a source of nitrous oxide. Although it is known that release rates of nitrogen from bedrock are large, there is an incomplete understanding of the connection between bedrock-hosted nitrogen and atmospheric nitrous oxide. Here, we quantify nitrogen fluxes and mass balances at a hillslope underlain by marine shale. We found that at this site bedrock weathering contributes 78% of the subsurface reactive nitrogen, while atmospheric sources (commonly regarded as the sole sources of reactive nitrogen in pristine environments) account for only the remaining 22%. About 56% of the total subsurface reactive nitrogen denitrifies, including 14% emitted as nitrous oxide. The remaining reactive nitrogen discharges in porewaters to a floodplain where additional denitrification likely occurs. We also found that the release of bedrock nitrogen occurs primarily within the zone of the seasonally fluctuating water table and suggest that the accumulation of nitrate in the vadoes zone, often attributed to fertilization and soil leaching, may also include contributions from weathered nitrogen-rich bedrock. Our hillslope study suggests that under oxygenated and moisture-rich conditions, weathering of deep, nitrogen-rich bedrock makes an important contribution to the nitrogen cycle. The data files are in Excel, which can be accessed using Microsoft Office, and consist of many data sets from the Pumphouse Hillslope PLM (Pumphouse Lower Montane) 1, 2, 3, and 4. They include soil to rock (0-10 meters) solid phase minerals and elements compositions; time- and depth-resolved pore-water chemistry and pore-gas compositions; time- and depth-resolved water table depths and water fluxes; subsurface weathering rates; nitrogen influxes and effluxes and mass balance. The attached paper is in a Word document, which can be accessed using Microsoft Office, and in pdf format.

54 ENVIRONMENTAL SCIENCES↗