Paul A. Roelle

Atmospheric nitrogen compounds II: emissions, transport, transformation, deposition and assessment

Abstract The Atmospheric Nitrogen Compounds II: Emissions, Transport, Transformation, Deposition and Assessment workshop was held in Chapel Hill, NC from 7 to 9 June 1999. This international conference, which served as a follow-up to the workshop held in March 1997, was sponsored by: North Carolina Department of Environment and Natural Resources; North Carolina Department of Health and Human Services, North Carolina Office of the State Health Director; Mid-Atlantic Regional Air Management Association; North Carolina Water Resources Research Institute; Air and Waste Management Association, RTP Chapter; the US Environmental Protection Agency and the North Carolina State University (College of Physical and Mathematical Sciences, and North Carolina Agricultural Research Service). The workshop was structured as an open forum at which scientists, policy makers, industry representatives and others could freely share current knowledge and ideas, and included international perspectives. The workshop commenced with international perspectives from the United States, Canada, United Kingdom, the Netherlands, and Denmark. This article summarizes the findings of the workshop and articulates future research needs and ways to address nitrogen/ammonia from intensively managed animal agriculture. The need for developing sustainable solutions for managing the animal waste problem is vital for shaping the future of North Carolina. As part of that process, all aspects of environmental issues (air, water, soil) must be addressed as part of a comprehensive and long-term strategy. There is an urgent need for North Carolina policy makers to create a new, independent organization that will build consensus and mobilize resources to find technologically and economically feasible solutions to this aspect of the animal waste problem.

Measurements and analysis of criteria pollutants in New Delhi, India

Ambient concentrations of carbon monoxide (CO), nitrogen oxides (NOx), sulfur dioxide (SO2), and total suspended particulates (TSP) were measured from January 1997 to November 1998 in the center of downtown [the Income Tax Office (ITO) located on B.S.G. Marg] New Delhi, India. The data consist of 24-h averages of SO2, NOx, and TSP as well as 8 and 24-h averages of CO. The measurements were made in an effort to characterize air pollution in the urban environment of New Delhi and assist in the development of an air quality index. The yearly average CO, NOx, SO2, and TSP concentrations for 1997 and 1998 were found to be 4810+/-2287 and 5772+/-2116 microg/m3, 83+/-35 and 64+/-22 microg/m3, 20+/-8 and 23+/-7 microg/m3, and 409+/-110 and 365+/-100 microg/m3, respectively. In general, the maximum CO, SO2, NOx, and TSP values occurred during the winter with minimum values occurring during the summer, which can be attributed to a combination of meteorological conditions and photochemical activity in the region. The ratio of CO/NOx (approximately 50) indicates that mobile sources are the predominant contributors for these two compounds in the urban air pollution problem in New Delhi. The ratio of SO2/NOx (approximately 0.6) indicates that point sources are contributing to SO2 pollution in the city. The averaged background CO concentrations in New Delhi were also calculated (approximately 1939 microg/m3) which exceed those for Eastern USA (approximately 500 microg/m3). Further, all measured concentrations exceeded the US National Ambient Air Quality Standards (NAAQS) except for SO2. TSP was identified as exceeding the standard on the most frequent basis.

Measurement of nitrogen oxide emissions from an agricultural soil with a dynamic chamber system

Biogenic soil emissions of nitric oxide (NO) were measured from an intensively managed agricultural row crop (corn, Zea mays) during a 4 week period (May 15 through June 9, 1995). The site was located in Washington County, near the town of Plymouth, which is in the Lower Coastal Plain of North Carolina. Soil NO flux was determined using a dynamic flowthrough chamber technique. The measurement period was characterized by two distinguishing features: an application of nitrogen (N) fertilizer at the midpoint of the experiment and a nontypical rainfall pattern. Average NO flux prior to the application of N fertilizer was 31.5 ± 10.1 ng N m−2 s−1, and more than doubled (77.7 ± 63.7 ng N m−2 s−1) after the application of a side-dressing of N fertilizer. Average soil extractable nitrogen values did not change significantly following application of the side-dressing of N fertilizer. We attribute this failure to detect a significant difference in soil extractable nitrogen following N fertilization to the method in which the fertilizer was applied, the subsequent rainfall pattern, and the technique of soil sampling. NO flux followed the same diurnal trend as soil temperature, with maximum NO emissions coinciding with maximum soil temperature, and minimum NO emissions coinciding with minimum soil temperature. NO flux was found to increase exponentially with soil temperature, but only after fertilization. Due to subsurface irrigation practices employed by the farmer, changes in soil water content were minimal, and no relation could be drawn between soil water content and NO flux. Simultaneous measurements of NOy, NO2, and NO emissions revealed that NO and NO2 emissions represent 86 and 8.7%, respectively, of NOy emissions leaving the soil. Simultaneous NO flux measurements made by a closed box flux technique, at the same site, revealed no statistically significant differences between the two different methodologies for measuring NO flux.

Nitric oxide emission from intensively managed agricultural soil in North Carolina

Emissions of nitric oxide (NO) were determined from an intensively managed agricultural soil near Plymouth, in the coastal plain of North Carolina, using the dynamic chamber technique. The measurements were made over a soybean field from July 15 to August 15, 1996, as part of the project Natural Emissions of Oxidant Precursors: Validation of Techniques and Assessment (NOVA). A N-containing fertilizer was applied at the middle of the experiment in order to investigate the effect of N-fertilizers on NO emissions and to test the response of instruments. Soil water content was high during the experimental period, with water-filled pore space ranging from 49% to 67%. NO emission during this period ranged between 0.28 and 18.45 ng N m -2 s -1 , with an overall average of 5.01 ± 3.03 ng N m -2 s -1 . A normal diurnal pattern with low values at nighttime and high values during the day was observed during the prefertilization period, but a reverse diurnal pattern (high at nighttime, low in daytime) of NO emission variation was found during the postfertilization, closed-canopy period, implying that interaction among canopy development, application of fertilization, and soil parameters may affect the diurnal variation of NO emission from soils. The emissions of NO were related to soil temperature, water-filled pore space, and extractable nitrogen. Application of fertilizer at the middle of the experiment was found to disrupt the normal relations between NO emission and soil temperature and water content seen during the prefertilization period but to enhance the positive relation between NO emission and extractable N. An intercomparison of the dynamic chamber technique with the eddy-correlation technique in this experiment indicates that in spite of large differences in the magnitudes of soil NO emission and the NO flux at 5 m, the two fluxes show similar variations with time and are strongly correlated.

Nitric oxide emissions from soils amended with municipal waste biosolids

Land spreading nitrogen-rich municipal waste biosolids (NO3 -No256 mg N kg � 1 dry weight, NH3-NB23,080 mg Nk g � 1 dry weight, Total Kjeldahl NB41,700 mg N kg � 1 dry weight) to human food and non-food chain land is a practice followed throughout the US. This practice may lead to the recovery and utilization of the nitrogen by vegetation, but it may also lead to emissions of biogenic nitric oxide (NO), which may enhance ozone pollution in the lower levels of the troposphere. Recent global estimates of biogenic NO emissions from soils are cited in the literature, which are based on field measurements of NO emissions from various agricultural and non-agricultural fields. However, biogenic emissions of NO from soils amended with biosolids are lacking. Utilizing a state-of-the-art mobile laboratory and a dynamic flow-through chamber system, in-situ concentrations of nitric oxide (NO) were measured during the spring/summer of 1999 and winter/spring of 2000 from an agricultural soil which is routinely amended with municipal waste biosolids. The average NO flux for the late spring/summer time period (10 June 1999–5 August 1999) was 69.4734.9 ng N m � 2 s � 1 . Biosolids were applied during September 1999 and the field site was sampled again during winter/spring 2000 (28 February 2000–9 March 2000), during which the average flux was 3.671.7 ng N m � 2 s � 1 . The same field site was sampled again in late spring (2–9 June 2000) and the average flux was 64.8741.0 ng N m � 2 s � 1 .A n observationally based model, developed as part of this study, found that summer accounted for 60% of the yearly emission while fall, winter and spring accounted for 20%, 4% and 16% respectively. Field experiments were conducted which indicated that the application of biosolids increases the emissions of NO and that techniques to estimate biogenic NO emissions would, on a yearly average, underestimate the NO flux from this field by a factor of 26. Soil temperature and % water filled pore space (%WFPS) were observed to be significant variables for predicting NO emissions, however %WFPS was found to be most significant during high soil temperature conditions. In the range of pH values found at this site (5.870.3), pH was not observed to be a significant parameter in predicting NO emissions. r 2002 Elsevier Science Ltd. All rights reserved.

Contribution of biogenic nitric oxide in urban ozone: Raleigh, NC, as a case study

Anthropogenic emissions from industrial and automotive sources within the confines of the city of Raleigh, NC have been documented by the North Carolina Department of Environment, Health and Natural Resources, Division of Environmental Management, but no direct biogenic emissions of nitric oxide (NO) from soils has yet been measured. In this study, emissions of NO were measured in Raleigh, NC, and its surrounding suburbs, in an attempt to determine the portion of the total NO, ( = NO + NO,) budget which can be attributed to biogenic sources. Residential and commercial lawns, and golf courses receiving normal fertilizer applications were chosen as the primary biogenic source of NO. Soil NO fluxes were measured using a dynamic chamber technique from 11 sites and ranged in value (hourly averages calculated from 15 min readings) from 1.24 to 23.7 ng N m -s-l. These hour averages were then combined with estimates of lawn acreage within the city proper, and in the surrounding suburbs, in order to develop a budget for biogenic NO emissions in Raleigh. This budget was then compared to the budget used in the Environmental Protection Agencys (EPA) Regional Oxidant Model (ROM) for photochemical modeling. Results from this comparison suggest that less than 1% of the total NO, budget for Raleigh, NC is emitted by natural processes, and that approximately 1.2% of the nitrogen applied as fertilizer is lost via soil NO emissions. Thus, the effects of biogenic NO may be neglected in the development of a reliable plan for reducing ozone in the urban atmosphere. 0 1997 Elsevier Science Ltd. All rights reserved.

Characterization of biogenic nitric oxide source strength in the southeast United States

Emissions of nitric oxide (NO) were measured during the summer of 1995 from 4 crops, located at three different sites throughout North Carolina. These sites were chosen to represent major physiographic regions of the Southeast US, in an effort to compare fluxes from different agriculturally managed soils. Emission rates were determined using a dynamic flow-through chamber system. In order to understand the NO flux from the different soil and crop types, measurements were made on corn and soybean crops in the coastal region, tobacco in the Piedmont region, and corn in the upper Piedmont region of North Carolina. Average NO fluxes were 5.5 f 2.2 ng N me2 s-‘, 20.7 + 19.2 ng N me2 s-‘, 4.1 + 1.4 ng N m-2s-1, and 8.5 2 4.9 ng N me2 s-l respectively for corn and soybean in the coastal region, tobacco in the Piedmont region, and corn in the upper Piedmont region. We were only able to detect an exponential dependence of NO flux on soil temperature at two of the locations. Tbe composite data of all the research sites revealed a general trend of increasing NO flux with soil water content or increasing extractable nitrogen in the soil, however, the day to day variations within each site did not reveal the same trends. We feel that acquisition of a soil NO flux data set in this fashion, which consists of observations collected over different points in both space and time, makes attempts to model soil NO flux in terms of different soil parameters difficult.

An ozone climatology: relationship between meteorology and ozone in the Southeast USA

A statistical analysis of ozone (O3) concentrations and meteorological parameters was performed to determine the relationship between meteorological changes and ambient O3 concentrations in the Southeast United States. The correlation between average daily maximum O3 concentration and various meteorological variables was analysed on a monthly basis from April through October during 1980-1994. The correlations were strongest during the summer months, particularly June, July, and August. Analysis of long term O3 concentration trends indicates increasing trends during the 1980s and decreasing trends during the early 1990s.

Modeling nitric oxide emissions from biosolid amended soils

Abstract Utilizing a state-of-the-art mobile laboratory in conjunction with a dynamic flow-through chamber system, nitric oxide concentrations [NO] were measured and NO fluxes were calculated during the summer, winter and spring of 1999/2000. The field site where these measurements were conducted was an agricultural soil amended with biosolids from a municipal wastewater treatment facility. These NO flux values were then used to assess the impact of including biosolid amended soils as a land-use class in an air quality model. The average NO flux from this biosolid amended soil was found to be exponentially dependent on soil temperature [NO Flux ( ng N m −2 s −1 )=1.07 exp (0.14 T soil ) ; R2=0.81—NO Flux =71.3 ng N m −2 s −1 at 30°C]. Comparing this relationship to results of the widely applied biogenic emissions inventory system (BEIS2) model revealed that for this field site, if the BEIS2 model was used, the NO emissions would have been underestimated by a factor of 26. Using this newly developed NO flux algorithm, combined with North Carolina Division of Water Quality statistics on how many biosolid amended acres are permitted per county, county-based NO inventories from these biosolid amended soils were calculated. Results from this study indicate that county-level biogenic NO emissions can increase by as much as 18% when biosolid amended soils are included as a land-use class. The multiscale air quality simulation platform (MAQSIP) was then used to determine differences in ozone (O3) and odd-reactive nitrogen compounds (NOy) between models run with and without the biosolid amended acreages included in the inventory. Results showed that during the daytime, when atmospheric mixing heights are typically at their greatest, any increase in O3 or NOy concentrations predicted by the model were small (

Soil Nitric Oxide Emissions: Lab and Field Measurements and Comparison

Equipment and procedures are developed and implemented to measure nitric oxide (NO) emissions from unamended and municipal wastewater treatment plant biosolids-amended soil in controlled laboratory...