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NASA NTRS2022

Mineral-Catalysed Formation of Marine NO and N 2 O on the Anoxic Early Earth

Microbial denitrification converts fixed nitrogen species into gases in extant oceans. However, it is unclear how such transformations occurred within the early nitrogen cycle of the Archean. Here 5we present experimental anoxic surface-catalyzed reduction of nitrite and nitrate via green rust and magnetite combined with diffusion and photochemical modeling. We find that in a Fe 2+ -rich marine environment, Fe minerals could have catalyzed abiotic denitrification reactions leading to the formation of nitric oxide (NO) and nitrous oxide (N 2 O). Nitrate did not exhibit reactivity in the presence of either mineral or aqueous Fe2+, however, both minerals induced rapid nitrite reduction 10to NO and N 2 O. While N 2 O escaped into the atmosphere (63% of nitrite-nitrogen, with green rust as catalyst), NO remained associated with precipitates (7%) serving as a potential shuttle to the benthic ocean.The modeling suggests that marine N 2 O emissions would have sustained 0.8-6 ppb of atmospheric N 2 O without a protective ozone layer. Our findings add detail to the as yet incompletely documented Archean nitrogen cycle, implying a globally distributed process driven 15by chemical kinetics similar to those of modern enzymatically mediated conversions.

Steffen Buessecker↗
NASA NTRS2009

Continuous Lidar Monitoring of Polar Stratospheric Clouds at the South Pole

Polar stratospheric clouds (PSC) play a primary role in the formation of annual ozone holes over Antarctica during the austral sunrise. Meridional temperature gradients in the lower stratosphere and upper troposphere, caused by strong radiative cooling, induce a broad dynamic vortex centered near the South Pole that decouples and insulates the winter polar airmass. PSC nucleate and grow as vortex temperatures gradually fall below equilibrium saturation and frost points for ambient sulfate, nitrate, and water vapor concentrations (generally below 197 K). Cloud surfaces promote heterogeneous reactions that convert stable chlorine and bromine-based molecules into photochemically active ones. As spring nears, and the sun reappears and rises, photolysis decomposes these partitioned compounds into individual halogen atoms that react with and catalytically destroy thousands of ozone molecules before they are stochastically neutralized. Despite a generic understanding of the ozone hole paradigm, many key components of the system, such as cloud occurrence, phase, and composition; particle growth mechanisms; and denitrification of the lower stratosphere have yet to be fully resolved. Satellite-based observations have dramatically improved the ability to detect PSC and quantify seasonal polar chemical partitioning. However, coverage directly over the Antarctic plateau is limited by polar-orbiting tracks that rarely exceed 80 degrees S. In December 1999, a NASA Micropulse Lidar Network instrument (MPLNET) was first deployed to the NOAA Earth Systems Research Laboratory (ESRL) Atmospheric Research Observatory at the Amundsen-Scott South Pole Station for continuous cloud and aerosol profiling. MPLNET instruments are eye-safe, capable of full-time autonomous operation, and suitably rugged and compact to withstand long-term remote deployment. With only brief interruptions during the winters of 2001 and 2002, a nearly continuous data archive exists to the present.

OZONE DESTRUCTION↗
NASA NTRS1976

A versatile system for biological and soil chemical tests on a planetary landing craft. I - Scientific objectives

We describe an approach for the remote detection and characterization of life in planetary soil samples. A mass spectrometer is used as the central sensor to monitor changes in the gas phase in eleven test cells filled with soil. Many biological assays, ranging from general 'in situ' assays to specific metabolic processes (such as photosynthesis, respiration, denitrification, etc.) can be performed by appropriate additions to the test cell via attached preloaded injector capsules. The system is also compatible with a number of chemical assays such as the analysis of atmospheric composition (both chemical and isotopic), the status of soil water, and the determination of compounds of carbon, nitrogen and sulfur in the soil.

Radmer, R. J.↗
NASA NTRS1986

Wet-oxidation waste management system for CELSS

A wet oxidation system will be useful in the Closed Ecological Life Support System (CELSS) as a facility to treat organic wastes and to redistribute inorganic compounds and elements. However at rather higher temperatures needed in this reaction, for instance, at 260 deg C, only 80% of organic in a raw material can be oxidized, and 20% of it will remain in the liquid mainly as acetic acid, which is virtually noncombustible. Furthermore, nitrogen is transformed to ammonium ions which normally cannot be absorbed by plants. To resolve these problems, it becomes necessary to use catalysts. Noble metals such as Ru, Rh and so on have proved to be partially effective as these catalysts. That is, oxidation does not occur completely, and the unexpected denitrification, instead of the expected nitrification, occurs. So, it is essential to develop the catalysts which are able to realize the complete oxidation and the nitrification.

Takahashi, Y.↗
NASA NTRS1987

Simultaneous field measurements of biogenic emissions of nitric oxide and nitrous oxide

Seasonal and diurnal emissions of NO and N2O from agricultural sites in Jamestown, Virginia and Boulder, Colorado are estimated in terms of soil temperature; percent moisture; and exchangeable nitrate, nitrite, and ammonium concentrations. The techniques and procedures used to analyze the soil parameters are described. The spatial and temporal variability of the NO and N2O emissions is studied. A correlation between NO fluxes in the Virginia sample and nitrate concentration, temperature, and percent moisture is detected, and NO fluxes for the Colorado site correspond with temperature and moisture. It is observed that the N2O emissions are only present when percent moisture approaches or exceeds the field capacity of the soil. The data suggest that NO is produced primarily by nitrification in aerobic soils, and N2O is formed by denitrification in anaerobic soils.

Anderson, Iris Cofman↗
NASA NTRS1987

N-15/N-14 variations in Cretaceous Atlantic sedimentary sequences - Implication for past changes in marine nitrogen biogeochemistry

Unusually low delta N-15 found in early to middle Cretaceous beds rich in marine organic matter from two separate eastern Atlantic Ocean basins is reported. These findings constitute unambiguous evidence that the N contained in these strata is the end result of biogeochemical processes that differed substantially from those that operated on the N contained in intervening organic carbon-poor strata and younger marine sediments. The data indicate that the low N-15 relative abundance is the consequence of pelagic rather than postdepositional processes. Reduced ocean circulation, increased denitrification, and hence, reduced euphotic zone nitrate availability may have led to Cretaceous phytoplankton assemblages that were periodically dominated by N2-fixing blue-green algae, a possible source of the sedimentary N-15 depletion.

Rau, Greg H.↗
NASA NTRS1987

Nitrogen transformations following tropical forest felling and burning on a volcanic soil

Nitrogen transformations and loss were measured following forest clearing in a relatively fertile tropical forest site. Nitrogen mineralization, nitrification, and amounts of ammonium and nitrate increased substantially in surface soils during the 6 mo following burning, then returned to background levels. The nitrogen content of microbial biomass declined to half its original value 6 mo after clearing and remained low in the cleared sites. Plant uptake of nitrogen was substantial on cleared plots (50 g/sq m), but it accounted for only 18 percent of N-15 label added to field plots. MIcrobial immobilization of N-15 was small relative to that in a cleared temperate site, and measurements of denitrification potentials suggested that relatively little mineralized nitrogen was lost to the atmosphere. Substantial amounts of nitrogen (40-70 g/sq m) were retained as exchangeably bound nitrate deep in the soils of a cleared plot on which revegetation was prevented; this process accounted for 12 percent of the N-15 label added to field plots.

Matson, Pamela A.↗
NASA NTRS1988

Nitrous oxide flux and nitrogen transformations across a landscape gradient in Amazonia

Nitrous oxide flux and nitrogen turnover were measured in three types of Amazonian forest ecosystems within Reserva Florestal Ducke near Manaus, Brazil. Nitrogen mineralization and nitrate production measured during 10-day laboratory incubations were 3-4 times higher in clay soils associated with 'terra firme' forests on ridge-top and slope positions than in 'campinarana' forests on bottomland sand soils. In contrast, nitrous oxide fluxes did not differ significantly among sites, but were highly variable in space and time. The observed frequency distribution of flux was positively skewed, with a mean overall sites and all sampling times of 1.3 ng N2O-N/sq cm per hr. Overall, the flux estimates were comparable to or greater than those of temperature forests, but less than others reported for Amazoonia. Results from a field fertilization experiment suggest that most nitrous oxide flux was associated with denitrification of soil nitrate.

Livingston, Gerald P.↗
NASA NTRS1988

Heterogeneous physicochemistry of the winter polar stratosphere

Present chemical theories of the Antarctic ozone hole assume that heterogeneous reactions involving polar stratospheric clouds (PSCs) are the precursor of springtime ozone depletions. However, none of the theories quantify the rates of proposed heterogeneous processed, and none utilize the extensive data base on PSC's. Thus, all of the theories must be considered incomplete until the heterogeneous mechanisms are properly defined. A unified treatment developed of the cloud related processes, both physical and chemical, and the importance of these processes using observation data is calibrated. The rates are compared competitive heterogeneous processes to place reasonable limits on critical mechanisms such as the denitrification and dechlorination of the polar winter stratosphere. Among the subjects addressed here are the physical/chemical properties of PSC's including their relevant microphysical, optical and compositional characteristics, mass transfer rates of gaseous constituents to cloud particles, adsorption, accommodation and sticking coefficients on cloud particles, time constants for condensation, absorption and other microphysical processes, effects of solubility and vapor pressure on cloud composition, the statistics of cloud processing of chemically active condensible species, rate limiting steps in heterogeneous chemical reactions, and the nonlinear dependence of ozone loss on physical and chemical parameters.

Turco, R. P.↗
NASA NTRS1988

The evolution of nitrogen cycling

The energetics of nitrogen transformation reactions and the evolution of nitrogen cycling are examined. It is suggested that meteor impact-produced fixed nitrogen could have caused the entire reservoir of the earth's N2 to convert into fixed nitrogen at the end of accretion. The abiotic fixation rate on the early earth by lightning is estimated at about 1-3 X 10 to the 16th molecules of NO/J. It is found that biological nitrogen fixation may have evolved after the development of an aerobic atmosphere. It is shown that HNO could eventually become NO2(-) and NO3(-) after reaching the earth's surface. It is concluded that the evolutionary sequence for the biological transformation of nitrogen compounds is ammonification - denitrification - nitrification - nitrogen fixation.

Mancinelli, Rocco L.↗
NASA NTRS1989

Measurements of nitric oxide and total reactive nitrogen in the Antarctic stratosphere - Observations and chemical implications

Results are presented on measurements of NO and the sum of reactive nitrogen species, NO(y), which include NO, NO2, NO3, N2O5, HNO3, and ClONO2 (in addition to ClO, O3, H2O, and N2O measurements), obtained aboard the NASA ER-2 aircraft flying over the Antarctica between the latitudes of 53 and 72 deg S during the Airborne Antarctic Ozone Experiment. The boundary of the chemically perturbed region (CPR), as indicated by a sharp increase in the level of ClO, occurred near 66 deg S; outside or equatorward of the CPR, the NO(y) mixing ratios ranged between 6 and 12 ppbv, with values decreasing poleward and reaching total NO(y) levels of 4 ppbv or less within 5-deg poleward of the boundary. Data presented in this paper clearly associate the Antarctic ozone decrease with perturbed conditions of ClO, NO(y), and H2O, which are in turn associated with processes defined as nonstandard heterogeneous chemistry, denitrification, and dehydration, respectively.

Fahey, D. W.↗
NASA NTRS1990

Redistribution of reactive odd nitrogen in the lower arctic stratosphere

In-situ measurements of total reactive odd nitrogen NO(y), were made from the NASA DC-8 aircraft in the lower arctic stratosphere during the 1989 Airborne Arctic Stratospheric Expedition. Throughout January and February, NO(y) mixing ratios were typically between 0.5 and 3 parts per billion by volume (ppbv) at altitudes between 10 and 12.5 km. During several flights late in the mission, events of unusually light NO(y) occurred with mixing ratios up to 12 ppbv at these altitudes. Simultaneous measurements of N2O, O3, and H2O during these events suggest that large changes in NO(y) are not expected. The elevated NO(y) values are interpreted as a vertical redistribution of NO(y) in the lower stratosphere resulting from gravitational sedimentation of aerosol particles containing HNO3. No evidence of the redistribution of H2O is noted, consistent with observations of denitrification without dehydration higher in the stratosphere.

Huebler, G.↗
NASA NTRS1990

Simulating the evolution of the chemical composition of the 1988/89 winter vortex

During the 1988/89 Airborne Arctic Stratospheric Expedition (AASE) observations of the chemical composition and aerosol characteristics of the winter vortex were obtained from a NASA ER-2 aircraft. In this paper we present interpretations of observations obtained on three ER-2 flights using a Lagrangian coupled photochemical-microphysical model. It is argued that observations obtained on Jaunary 16 and 19, and February 10, represent different stages of the chemical evolution of the vortex, from the early stages of chlorine release, the onset of denitrification and the intensively processed state.

Jones, R. L.↗
NASA NTRS1990

Emission of nitric oxide (NO) from tropical forest soils and exchange of NO between the forest canopy and atmospheric boundary layers

Emissions of NO from soils in the Amazon rain forest were measured at 66 locations using an enclosure technique, and continuous vertical profiles of NO and O3 were measured between the ground and 41-m altitude. Fluxes of NO averaged 8.9 (+ or - 1.5) x 10 to the 9th molecules/sq cm per sec from the dominant (yellow clay) soils of the region, with larger fluxes observed from adjacent white sand soils. Fluxes from clay soils were lower by more than a factor of 5 than fluxes observed during the dry season at a nearby site. Low soil emission rates were reflected in lower concentrations of NO at the top of the forest canopy in the wet season, only 30-50 parts per trillion by volume during the daytime. The measured fluxes are consistent with chemical mass balances for NO within the forest canopy, calculated from the NO and O3 profiles taken at night, and with observations of NO between 150 and 5000 m altitude. Measurements of NO emission rates from soil plots fertilized using NaNO3, NH4Cl, or sucrose indicated that a reductive pathway (denitrification) may have been primarily responsible for production of the NO released by both clay and sand soils.

Bakwin, Peter S.↗
NASA NTRS1991

Measurements in polar stratospheric clouds over Antarctica in September 1989

The results of six balloon flights at McMurdo Station, Antarctica, under varying temperature conditions, are used in a study of polar stratospheric clouds during Sept. 1989. A particle counter, with size resolution in the 0.5 micron radius region, indicates that cloud size distributions are always bimodal. Mode radii ranging from 0.05 to 0.10 microns were observed for the small particle mode, representing the sulfate layer or condensational growth enhancements of it. The data are not inconsistent with the expected increase in size with decreasing temperature of the small particle mode in the sulfate layer owing to deliquescence although this phenomenon is often masked by nitric acid trihydrate (NAT) condensation when temperatures are sufficiently low. Mode radii generally ranged from 1.5 to 3.5 micron for the large particle mode at concentrations 3 to 4 orders of magnitude lower than the small particle mode. The large particle mode, which normally comprises most of the mass, is presumably caused by NAT condensation on larger particles of the sulfate layer and indicates HNO3 mixing ratios of 1 to 5 ppbv for most of the cloud layers observed, suggesting substantial denitrification. On several occasions, distributions were observed with mode radii as high as 7 microns, and correspondingly large inferred mass, indicating water ice clouds in the 12 to 15 km region. On other occasions, absence of such clouds at very low temperatures indicated water vapor mixing ratios of less than 3 ppmv suggesting dehydration. Generally, the inferred HNO3 mixing ratios were higher in the lower stratosphere, suggesting redistribution through particle sedimentation.

Deshler, Terry↗
NASA NTRS1990

Fourier transform infrared studies of model polar stratospheric cloud surfaces - Growth and evaporation of ice and nitric acid/ice

Fourier-transform infrared surface studies are used to probe the microphysical properties of nitric acid trihydrate (NAT) and ice films representative of type I and II polar stratospheric clouds (PSC). Experiments indicate that, on initial exposure to 1.8 microtorr of HNO3, a layer of ice is quantitatively converted to NAT. However, conversion of ice to NAT does not proceed indefinitely, but rather the system reaches saturation. For longer exposures or higher HNO3 pressures, NAM becomes the dominant nitric acid containing species on the surface. Evaporation studies were performed to test the feasibility of a recent denitrification mechanism. The results indicate that ice coated with 0.20 micron of NAT evaporates at a temperature of about 4 C higher than uncoated ice.

Tolbert, Margaret A.↗
NASA NTRS1991

Biospheric-atmospheric coupling on the early Earth

Theoretical calculations performed with a one-dimensional photochemical model have been performed to assess the biospheric-atmospheric transfer of gases. Ozone reached levels to shield the Earth from biologically lethal solar ultraviolet radiation (220-300 nm) when atmospheric oxygen reached about 1/10 of its present atmospheric level. In the present atmosphere, about 90 percent of atmospheric nitrous oxide is destroyed via solar photolysis in the stratosphere with about 10 percent destroyed via reaction with excited oxygen atoms. The reaction between nitrous oxide and excited oxygen atoms leads to the production of nitric oxide in the stratosphere, which is responsible for about 70 percent of the global destruction of oxygen in the stratosphere. In the oxygen/ozone deficient atmosphere, solar photolysis destroyed about 100 percent of the atmospheric nitrous oxide, relegating the production of nitric oxide via reaction with excited oxygen to zero. Our laboratory and field measurements indicate that atmospheric oxygen promotes the biogenic production of N2O and NO via denitrification and the biogenic production of methane by methanogenesis.

Levine, J. S.↗
NASA NTRS1990

ATLAS: Airborne Tunable Laser Absorption Spectrometer for stratospheric trace gas measurements

The ATLAS instrument is an advanced technology diode laser based absorption spectrometer designed specifically for stratospheric tracer studies. This technique was used in the acquisition of N2O tracer data sets on the Airborne Antarctic Ozone Experiment and the Airborne Arctic Stratospheric Expedition. These data sets have proved valuable for comparison with atmospheric models, as well as in assisting in the interpretation of the entire ensemble of chemical and meteorological data acquired on these two field studies. The N2O dynamical tracer data set analysis revealed several ramifications concerning the polar atmosphere: the N2O/NO(y) correlation, which is used as a tool to study denitrification in the polar vertex; the N2O Southern Hemisphere morphology, showing subsidence in the winter polar vortex; and the value of the N2O measurements in the interpretation of ClO, O3, and NO(y) measurements and of the derived dynamical tracer, potential vorticity. Field studies also led to improved characterization of the instrument and to improved accuracy.

Loewenstein, Max↗