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Impacts of Fires on Photochemistry: Observations of Peroxyacetyl Nitrate (PAN) from CrIS and AIRS
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Towards the Harmonization of Nitrate Aerosol Simulations within the NASA Goddard Earth Observing System (GEOS) Model
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Changes to Peroxyacyl Nitrates (PANs) Over Megacities in Response to COVID‐19 Tropospheric NO 2 Reductions Observed by the Cross‐Track Infrared Sounder (CrIS)
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Examining Relationships Between Groundwater Nitrate Concentrations in Drinking Water and Landscape Characteristics to Understand Health Risks
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An integrated framework to model nitrate contaminants with interactions of agriculture, groundwater, and surface water at regional scales: The STICS–EauDyssée coupled models applied over the Seine River Basin
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Limitations in Representation of Physical Processes Prevents Successful Simulation of PM2.5 During KORUS-AQ
High levels of fine particulate matter (PM2.5) pollution in East Asia often exceed local air quality standards. Observations from the Korea United States-Air Quality (KORUS-AQ) field campaign in May and June 2016 showed that development of extreme pollution (haze) occurred through a combination of long-range transport and favorable meteorological conditions that enhanced local production of PM2.5. Atmospheric models often have difficulty simulating PM2.5 chemical composition during haze, which is of concern for the development of successful control measures. We use observations from KORUS-AQ to examine the ability of the GEOS-Chem chemical transport model to simulate PM2.5 composition throughout the campaign and identify the mechanisms driving the pollution event. At the surface, the model underestimates sulfate by -64% but overestimates nitrate by +36%. The largest underestimate in sulfate occurs during the pollution event, where models typically struggle to generate elevated sulfate concentrations due to missing heterogeneous chemistry in aerosol liquid water in the polluted boundary layer. Hourly surface observations show that the model nitrate bias is driven by an overestimation of the nighttime peak. In the model, nitrate formation is limited by the supply of nitric acid, which is biased by +100% against aircraft observations. We hypothesize that this is due to a large missing sink, which we implement here as a factor of five increase in dry deposition. We show that the resulting increased deposition velocity is consistent with observations of total nitrate as a function of photochemical age. The model does not account for factors such as the urban heat island effect or the heterogeneity of the built-up urban landscape resulting in insufficient model turbulence and surface area over the study area that likely results in insufficient dry deposition. Other species such as NH3 could be similarly affected but were not measured during the campaign. Nighttime production of nitrate is driven by NO2 hydrolysis in the model, while observations show that unexpectedly elevated nighttime ozone (not present in the model) should result in N2O5 hydrolysis as the primary pathway. The model is unable to represent nighttime ozone due to an overly rapid collapse of the afternoon mixed layer and excessive titration by NO. We attribute this to missing nighttime heating driving deeper nocturnal mixing that would be expected to occur in a city like Seoul. This urban heating is not considered in air quality models run at large enough scales to treat both local chemistry and long-range transport. Key model failures in simulating nitrate, mainly overestimated daytime nitric acid, incorrect representation of nighttime chemistry, and an overly shallow and insufficiently turbulent nighttime mixed layer, exacerbate the model’s inability to simulate the buildup of PM2.5 during haze pollution. To address the underestimate in sulfate most evident during the haze event, heterogeneous aerosol uptake of SO2 is added to the model which previously only considered aqueous production of sulfate from SO2 in cloud water. Implementing a simple parameterization of this chemistry improves the model abundance of sulfate but degrades the SO2 simulation implying that emissions are underestimated. We find that improving model simulations of sulfate has direct relevance to determining local vs. transboundary contributions to PM2.5. During the haze pollution event, the inclusion of heterogeneous aerosol uptake of SO2 decreases the fraction of PM2.5 attributable to long-range transport from 66% to 54%. Locally-produced sulfate increased from 1% to 25% of locally-produced PM2.5, implying that local emissions controls would have a larger effect than previously thought. However, this additional uptake of SO2 is coupled to the model nitrate prediction which affects the aerosol liquid water abundance and chemistry driving sulfate-nitrate-ammonium partitioning. An additional simulation of the haze pollution with heterogeneous uptake of SO2 to aerosol and simple improvements to the model nitrate simulation results in 30% less sulfate due to 40% less nitrate and aerosol water, and results in an underestimate of sulfate during the haze event. Future studies need to better consider the impact of model physical processes such as dry deposition and nighttime boundary layer mixing on the simulation of nitrate and the effect of improved nitrate simulations on the overall simulation of secondary inorganic aerosol (sulfate+nitrate+ammonium) in East Asia. Foreign emissions are rapidly changing, increasing the need to understand the impact of local emissions on PM2.5 in South Korea to ensure continued air quality improvements.
Physiology and enzymology involved in denitrification by Shewanella putrefaciens
Nitrate reduction to N2O was investigated in batch cultures of Shewanella putrefaciens MR-1, MR-4, and MR-7. All three strains reduced nitrate to nitrite to N2O, and this reduction was coupled to growth, whereas ammonium accumulation was very low (0 to 1 micromol liter-1). All S. putrefaciens isolates were also capable of reducing nitrate aerobically; under anaerobic conditions, nitrite levels were three- to sixfold higher than those found under oxic conditions. Nitrate reductase activities (31 to 60 micromol of nitrite min-1 mg of protein-1) detected in intact cells of S. putrefaciens were equal to or higher than those seen in Escherichia coli LE 392. Km values for nitrate reduction ranged from 12 mM for MR-1 to 1.3 mM for MR-4 with benzyl viologen as an artifical electron donor. Nitrate and nitrite reductase activities in cell-free preparations were demonstrated in native gels by using reduced benzyl viologen. Detergent treatment of crude and membrane extracts suggested that the nitrate reductases of MR-1 and MR-4 are membrane bound. When the nitrate reductase in MR-1 was partially purified, three subunits (90, 70, and 55 kDa) were detected in denaturing gels. The nitrite reductase of MR-1 is also membrane bound and appeared as a 60-kDa band in sodium dodecyl sulfate-polyacrylamide gels after partial purification.
Filter measurements of chemical composition during the airborne Antarctic ozone experiment
During the Airborne Antarctic Ozone Experiment campaign, a filter sampler was flown to measure the bulk composition of aerosol and gas phases. The background sulfate aerosol was measured in regions inside and outside of the chemically perturbed region (CPR) of the polar vortex. The mass ratio of sulfate outside to inside was 2.8. This is indicative of a cleansing mechanism effecting the CPR or of a different air mass inside versus outside. The absolute value of the sulfate mixing ratio shows that the background aerosol has not been influenced by recent volcanic eruptions. The sulfate measured on the ferry flight returning to NASA Ames shows a decrease towards the equator with increasing concentrations in the northern hemisphere. Nitrate in the aerosol phase was observed on two flights. The largest amount of nitrate measured in the aerosol was 44 percent of the total amount of nitrate observed. Other samples on the same flights show no nitrate in the aerosol phase. The presence of nitrate in the aerosol is correlated with the coldest temperatures observed on a given flight. Total nitrate (aerosol plus acidic vapor nitrate) concentrations were observed to increase at flight altitude with increasing latitude north and south of the equator. Total nitrate was lower inside the CPR than outside. Chloride and flouride were not detected in the aerosol phase. From the concentrations of acidic chloride vapor, the ratio of acidic vapor Cl to acidic vapor F and a summing of the individual chloride containing species to yield a total chloride concentration, there is a suggestion that some of the air sampled was dechlorinated. Acidic vapor phase fluoride was observed to increase at flight altitude with increasing latitude both north and south of the equator. The acidic vapor phase fluoride was the only compound measured with the filter technique that exhibited larger concentrations inside the CPR than outside.
Annual and interannual variations of phytoplankton pigment concentration and upwelling along the Pacific equator
The following variables along the Pacific equator from 145 deg E to 95 deg W were employed: surface layer phytoplankton pigment concentrations derived from Nimbus 7 coastal zone color scanner (CZCS) measurements of ocean color radiances; vertical velocities simulated at the 90-m bottom of the euphotic layer from a wind-driven ocean general circulation model; and nitrate concentrations estimated from model-simulated temperature. The upward flux of nitrate into the euphotic layer was calculated from the simulated vertical motion and nitrate concentration. The CZCS-derived phytoplankton pigment concentration was uniform from 175 deg to 95 deg W. Longitudinal profiles of upwelling, phytoplankton biomass, and 90-m nitrate flux were of different shapes. The small annual cycles of the phytoplankton pigment and nitrate flux were in phase: increased phytoplankton biomass was associated with increased upward nitrate flux, but the phase was not consistent with the annual cycles of the easterly wind or of the upwelling intensity. Variation of phytoplankton pigment concentration was greater during El Nino than during the annual cycle. The substantially reduced phytoplankton pigment concentration observed during El Nino was associated with smaller upward nitrate flux. Phytoplankton biomass during non-El Nino conditions was not related to nitrate flux into the euphotic layer.
Estimating new production in the equatorial Pacific Ocean at 150 deg W
A major goal of the WEC88 cruise of the R/V Wecoma to the equatorial Pacific (made in February-March 1988) was to establish rates of new production along a meridional section at 150 deg W and to compare these measured rates with the relatively high values for the equatorial Pacific that had been reported previously using indirect methods and models. Production values were obtained from the traditional approach using N-15 labeled nitrate uptake, and by using C-14 fixation values multiplied by f (proportion of new production) from various sources: from N-15 data, from a C-14 fixation-versus-f relationship, or from a nitrate-versus-f relationship. The ratios of directly measured nitrate and carbon uptake and the ratios of nitrate to nitrate plus ammonium uptake, i.e., values of f, agree well; values of f calculated from carbon uptake or from nitrate concentration are overestimates for the equatorial upwelling region. Carbon-to-nitrogen uptake ratios measured with C-14 and N-15, respectively, approximate the Redfield molar ratio, 6.6 C:N. The overall mean value of f (0.17) helps confirm the view that the low primary production in the enriched eastern equatorial Pacific is due to failure of the nitrate-uptake system.
New production in the warm waters of the tropical Pacific Ocean
The average depth-integrated rate of new production in the tropical Pacific Ocean was estimated from a calculation of horizontal and vertical nitrate balance over the region enclosed by the climatological 26 C isotherm. The net turbulent flux of nitrate into the region was computed in terms of the climatological net surface heat flux and the nitrate-temperature relationship at the base of the 26 C isotherm. The net advective transport of nitrate into the region was estimated using the mean nitrate distribution obtained from the analysis of historical data and previous results of a general circulation model of the tropical Pacific. The rate of new production resulting from vertical turbulent fluxes of nitrate was found to be similar in magnitude to that due to advective transport. Most (about 75%) of the advective input of nitrate was due to the horizontal transport of nutrient-rich water from the eastern equatorial region rather than from equatorial upwelling. An average rate of new production of 14.5 - 16 g C/sq m/yr was found for the warm waters of the tropical Pacific region. These values are in good agreement with previous estimates for this region and are almost five times less than is estimated for the eastern equatorial Pacific, where most of the nutrient upwelling occurs.
Chemical Characterization and Reactivity of Fuel-Oxidizer Reaction Product
Fuel-oxidizer reaction product (FORP), the product of incomplete reaction of monomethylhydrazine and nitrogen tetroxide propellants prepared under laboratory conditions and from firings of Shuttle Reaction Control System thrusters, has been characterized by chemical and thermal analysis. The composition of FORP is variable but falls within a limited range of compositions that depend on three factors: the fuel-oxidizer ratio at the time of formation; whether the composition of the post-formation atmosphere is reducing or oxidizing; and the reaction or post-reaction temperature. A typical composition contains methylhydrazinium nitrate, ammonium nitrate, methylammonium nitrate, and trace amounts of hydrazinium nitrate and 1,1-dimethylhydrazinium nitrate. Thermal decomposition reactions of the FORP compositions used in this study were unremarkable. Neither the various compositions of FORP, the pure major components of FORP, nor mixtures of FORP with propellant system corrosion products showed any unusual thermal activity when decomposed under laboratory conditions. Off-limit thruster operations were simulated by rapid mixing of liquid monomethylhydrazine and liquid nitrogen tetroxide in a confined space. These tests demonstrated that monomethylhydrazine, methylhydrazinium nitrate, ammonium nitrate, or Inconel corrosion products can induce a mixture of monomethylhydrazine and nitrogen tetroxide to produce component-damaging energies. Damaging events required FORP or metal salts to be present at the initial mixing of monomethylhydrazine and nitrogen tetroxide.
STABILITY TESTS OF MONOPROPELLANTS EXPOSED TO FLAMES AND RIFLE FIRE
Tests of the stability of several monopropellants under the effects of impact and heat were conducted in order to assess the potential hazard in a propellant storage area from major fires and enemy attack. Hydrazine, hydrazine nitrate solution, n-propyl nitrate, and ethylene oxide were all tested in one-gallon aluminum containers (half of them filled to 25% and half to 95% capacity) by being subjected to oil bonfires and wood bonfires, and 20-mm incendiary, 20mm high explosive incendiary, and .30-caliber rifle fire. Aviation gasoline was tested in the same manner, for comparison. In the bonfire tests, all four monopropellants generally gave explosion intensities equivalent to one another regardless of the type of bonfire (oil or wood) or the amount of liquid in the test container. Occasionally, however, with hydrazine, hydrazine nitrate solution, and n-propyl nitrate, anomalous results occurred: there was either (a) no explosion or (b) an explosion of above average intensity. Ethylene oxide more nearly approximated the behavior of aviation gasoline than did the other monopropellants. In the rifle-fire tests, n-propyl nitrate appeared to be most shock- sensitive since it was exploded by all three types of ammunition. Hydrazine and hydrazine nitrate solution were exploded by the high-explosive ammunition, but not by the incendiary or .30-dber ammunition. Ethylene oxide was not exploded by any of the gunfire, but the liquid was ignited by both incendiary and high-explosive incendiary ammunition.
Measurements of nitrogen productivity in the equatorial Pacific
During the R/V Wecoma WEC88 cruise that sampled a meridional transect along 150 deg W from 15 deg N to 15 deg S, uptake of nitrate and ammonium by phytoplankton was measured using the stable isotope N-15 with simulated in-situ bottle incubations and shipboard mass spectrometry. A set of 25 daily productivity stations showed the influence of equatorial upwelling on nitrate distribution and N-15 uptake in a band from 6 deg N to 7.5 deg S compared with the oligotrophic waters to the north and south, with the highest values of nitrate uptake occurring at the equator. During a 5-day time series at the equator, there was an increase in nitrate accompanied by increased nitrate uptake. Interestingly, nitrate uptake rates (equivalent to new production rates) at the equator were lower than those predicted by previous investigators. Holdover experiments and uptake versus irradiance curves showed that the phytoplankton was in an early stage of metabolic adaptation and that can be a contributing factor.
Energetic Charged Particle Component or the NO(y) Budget of the Polar Middle Atmosphere
Analysis of nitrates measured in polar ice cap snow at a high resolution shows large variations in the nitrates. It has been shown that the nitrate signal may contain a signature of solar activity [Zeller and Dreschhoff, 19951. Reactive odd nitrogen production associated with solar particle events (SPEs) and auroral activity may be a source of some of the nitrate anomalies observed in the polar ice caps. Periods of large SPEs can lead to a production of polar atmospheric odd nitrogen in excess of the ambient sources in the polar stratosphere and mesosphere, and may leave a large nitrate signal stratified in the polar ice cap. Auroral electrons and photoelectrons produce odd nitrogen in the thermosphere, some of which may be transported to the polar (>50 degrees) mesosphere and stratosphere. Sources of odd nitrogen in the polar middle atmosphere associated with SPEs, galactic cosmic rays, and auroral electron precipitation have been quantified. The relative contributions by the energetic particles sources to the Noy budget of the polar middle atmosphere (from tropopause to 50 km, from 50 degrees to 90 degrees latitude) are compared with the nitrates observed in the polar ice sheets.
A Simulated High CO 2 Spaceflight Environment Increases Plant Preference for Ammonium as a Nitrogen Source.
Future long-duration missions will require a sustainable supply of food to support human crews. The spaceflight cabin environment often contains very high concentrations of CO 2 due to release of CO 2 by astronauts that is not completely scrubbed from the cabin, and it is therefore crucial to understand plant responses to elevated CO 2 (eCO 2 ) environments. Much focus has been given to changes in plant photosynthetic and performance parameters in response to eCO 2 , but the effects of eCO 2 on nitrogen (N) uptake are poorly understood. Shoot nitrate reduction may be reduced at eCO 2 , likely due to less reductant available for nitrate reduction because of reduced photorespiration and increased carbon fixation 1. Relative growth rate can be reduced at eCO 2 when N is provided only as nitrate and can be unaffected when N is supplied as ammonium 1. However, N uptake in response to eCO 2 has, to our knowledge, not yet been studied. An increased ‘preference’ for plants to take up N as ammonium at eCO 2 could have important implications for growth in the space environment, where N is currently only supplied as nitrate. In this study, novel stable isotope approaches were used in conjunction with hydroponics and isotope ratio mass spectrometry to determine the effect of eCO 2 on N preference for ammonium or nitrate in spring barley and lettuce when both N forms are provided equally. Several varieties of spring barley displayed increased ammonium preference at eCO 2 (720 ppm) compared to ambient CO 2 (410 ppm), though this was not true for all varieties 2. In most cases, increases in ammonium preference were driven by increases in ammonium uptake at eCO 2 and not decreases in nitrate uptake. Current research is assessing whether similar responses are observed in the candidate space crop lettuce, at levels of CO 2 like those observed on ISS (3000 ppm), and these results will also be presented. This work will enable the development of optimized nutrient regimes for candidate crops in space environments and the selection of crop varieties adapted to eCO 2 environments. Plants adapted to ammonium nutrition may play a role in future plant-based bioregenerative life support systems with higher ammonium concentrations due to waste recycling 3. Moreover, this research will further our understanding of plant responses to the eCO 2 environment brought about by climate change, allowing the development of future-proof crops that will help to maintain food security. References: 1. Bloom (2015). The increasing importance of distinguishing among plant nitrogen sources. Current Opinion in Plant Biology 25, 10-16. 2. Fountain (2023). Understanding interactions of barley (Hordeum vulgare) with soil nitrogen cycling activity and links to plant nitrogen preference. Ph.D. Thesis, The University of Sheffield. 3. Schiefloe et al. (2023). From urine to food and oxygen: effects of high and low NH4+:NO3- ratio on lettuce cultivated in a gas-tight hydroponic facility. Frontiers in Plant Science 14:1229476.
A Simulated High CO 2 Spaceflight Environment Increases Plant Preference for Ammonium as a Nitrogen Source.
Future long-duration missions will require a sustainable supply of food to support human crews. The spaceflight cabin environment often contains very high concentrations of CO 2 due to release of CO 2 by astronauts that is not completely scrubbed from the cabin, and it is therefore crucial to understand plant responses to elevated CO 2 (eCO 2 ) environments. Much focus has been given to changes in plant photosynthetic and performance parameters in response to eCO 2 , but the effects of eCO 2 on nitrogen (N) uptake are poorly understood. Shoot nitrate reduction may be reduced at eCO 2 , likely due to less reductant available for nitrate reduction because of reduced photorespiration and increased carbon fixation 1. Relative growth rate can be reduced at eCO 2 when N is provided only as nitrate and can be unaffected when N is supplied as ammonium. However, N uptake in response to eCO 2 has, to our knowledge, not yet been studied. An increased ‘preference’ for plants to take up N as ammonium at eCO 2 could have important implications for growth in the space environment, where N is currently only supplied as nitrate. In this study, novel stable isotope approaches were used in conjunction with hydroponics and isotope ratio mass spectrometry to determine the effect of eCO 2 on N preference for ammonium or nitrate in spring barley and lettuce when both N forms are provided equally. Several varieties of spring barley displayed increased ammonium preference at eCO 2 (720 ppm) compared to ambient CO 2 (410 ppm), though this was not true for all varieties. In most cases, increases in ammonium preference were driven by increases in ammonium uptake at eCO 2 and not decreases in nitrate uptake. Current research is assessing whether similar responses are observed in the candidate space crop lettuce, at levels of CO 2 like those observed on ISS (3000 ppm), and these results will also be presented. This work will enable the development of optimized nutrient regimes for candidate crops in space environments and the selection of crop varieties adapted to eCO 2 environments. Plants adapted to ammonium nutrition may play a role in future plant-based bioregenerative life support systems with higher ammonium concentrations due to waste recycling. Moreover, this research will further our understanding of plant responses to the eCO 2 environment brought about by climate change, allowing the development of future-proof crops that will help to maintain food security.