Numerical Investigation of the Effects of Boundary-Layer Evolution on the Predictions of Ozone and the Efficacy of Emission Control Options in the Northeastern United States

This paper examines the effects of two different planetary boundary-layer (PBL) parameterization schemes – Blackadar and Gayno–Seaman – on the predicted ozone (O₃) concentration fields using the MM5 (Version 3.3) meteorological model and the MODELS-3 photochemical model. The meteorological fields obtained from the two boundary-layer schemes have been used to drive the photochemical model to simulate O₃ concentrations in the northeastern United States for a three-day O₃ episodic period. In addition to large differences in the predicted O₃ levels at individual grid cells, the simulated daily maximum 1-h O₃ concentrations appear at different regions of the modeling domain in these simulations, due to the differences in the vertical exchange formulations in these two PBL schemes. Using process analysis, we compared the differences between the different simulations in terms of the relative importance of chemical and physical processes to O₃ formation and destruction over the diurnal cycle. Finally, examination of the photochemical model's response to reductions in emissions reveals that the choice of equally valid boundary-layer parameterizations can significantly influence the efficacy of emission control strategies.     

Numerical Investigation of Boundary-Layer Evolution and Nocturnal Low-Level Jets: Local versus Non-Local PBL Schemes

Numerical simulations of the evolution of the planetary boundary layer (PBL) and nocturnal low-level jets (LLJ) have been carried out using MM5 (version 3.3) with four-dimensional data assimilation (FDDA) for a high pollution episode in the northeastern United States during July 15–20, 1999. In this paper, we assess the impact of different parameterizations on the PBL evolution with two schemes: the Blackadar PBL, a hybrid local (stable regime) and non-local (convective regime) mixing scheme; and the Gayno–Seaman PBL, a turbulent kinetic energy (TKE)-based eddy diffusion scheme. No FDDA was applied within the PBL to evaluate the ability of the two schemes to reproduce the PBL structure and its temporal variation. The restriction of the application of FDDA to the atmosphere above the PBL or the lowest 8 model levels, whichever is higher, has significantly improved the predicted strength and timing of the LLJ during the night. A systematic analysis of the PBL evolution has been performed for the primary meteorological fields (temperature, specific humidity, horizontal winds) and for the derived parameters such as the PBL height, virtual potential temperature, relative humidity, and cloud cover fraction. There are substantial differences between the PBL structures and evolutions simulated by these two different schemes. The model results were compared with independent observations (that were not used in FDDA) measured by aircraft, RASS and wind profiler, lidar, and tethered balloon platforms during the summer of 1999 as part of the NorthEast Oxidant and Particle Study (NE-OPS). The observations tend to support the non-local mixing mechanism better than the layer-to-layer eddy diffusion in the convective PBL.     

Relationship between air pollutants emission patterns and concentrations

Emission patterns of NO_x and S‐compounds are analyzed to study their influence on the concentrations of SO₂, NO_x, sulphate and nitrate in the air. Air mass trajectories, emission inventories and cluster analysis are used to define the emission patterns.

The scheme that characterized most of the days is defined by low emissions from 48 hours until 18 hours before the measurements and it produces average concentrations. High concentrations are due to emission peaks. The time between these emission peaks and the measurement determines the importance of the emission peak on the concentration.     

Boundary Layer Evolution and its Influence on Ground-Level Ozone Concentrations

Accurate determination of the planetary boundary layer (PBL) height (i.e., mixing height (MH)) is critical to properly simulating pollutant levels with the grid-based photochemical models. In this study, the daytime mixing heights based on the parcel and bulk Richardson number methods are compared with those obtained directly from a numerical mesoscale meteorological model in an effort to evaluate the uncertainties in the estimation of the PBL evolution. Mixing heights are estimated from hourly outputs of meteorological variables of the Penn State/NCAR Mesoscale Model Version 3.3 (MM5V3) with two PBL schemes (Blackadar and Gayno-Seaman) during July 1999 over Philadelphia, PA. An analysis of the diurnal variation in the urban PBL and its influence on ground-level ozone (O₃) levels is presented in this paper. The results indicate that on average, the MHs determined from the bulk Richardson number were larger than those estimated from the parcel method. The MHs from the MM5V3 output were much smaller than those derived from the parcel and bulk Richardson number methods, especially for the Gayno-Seaman scheme that is based on turbulent kinetic energy. The MH and ground-level O₃ concentration have been found to be twice as much on episode days than on non-episode days. The average hourly MH growth rate and O₃ tendency (i.e. rate of change in O₃) were largest during the morning hours (0700 to 1000 eastern standard time (EST)), suggesting that vertical mixing contributes significantly to the accumulation of ground-level O₃ in urban areas in the morning hours.     

Transport and Diffusion of Ozone in the Nocturnal and Morning Planetary Boundary Layer of the Phoenix Valley

The evolution of ozone (O ₃) in the nocturnal and morning-transitional planetary boundary layer (PBL) of the Phoenix valley was measured as a part of the `Phoenix Sunrise Experiment 2001' of the U.S. Department of Energy conducted in June 2001. The goal of the field program was to study the transport, distribution and storage of ozone and its precursors in the urban boundary layer over a diurnal cycle. The ground level O <sub>3</sub> as well as mean meteorological variables and turbulence were measured over the entire period, and vertical profiling (using a tethered balloon) was made during the morning transition period. Approximately half of the observational days showed the usual diurnal cycle of high O <sub>3</sub> during the day and low O <sub>3</sub> at night, with nitrogen oxides (NO <sub>x</sub> = NO <sub>2</sub> + NO) showing an out of phase relationship with O <sub>3</sub>. The rest of the days were signified by an anomalous increase of O <sub>3</sub> in the late evening ( 2200 LST), concomitant with a sudden drop of temperature, an enhancement of wind speed and Reynolds stresses, a positive heat flux and a change of wind direction. NO <sub>x</sub> measurements indicated the simultaneous arrival of an `aged' air mass, which was corroborated by the wind predictions of a mesoscale numerical model. In all, the results indicate that the recirculation of O ₃ rich air masses is responsible for the said high-O ₃ events. Such air masses are produced during the transport of O ₃ precursors by the upslope flow toward mountainous suburbs during the day, and they return back to the city at night via downslope winds (i.e. mountain breeze). The corresponding flow patterns, and hence the high-O ₃ events, are determined by background meteorological conditions. The vertical profiling of O ₃ and flow variables during the morning transition points to a myriad of transport, mixing and chemical processes that determine the fate of tropospheric O ₃. How well such processes are incorporated and resolved in predictive O ₃ models should determine the accuracy of their predictions.     

Analysis of air pollution at Shuaiba industrial area in Kuwait

A study has been conducted over a period of one year on measurements of air pollution in the Shuaiba Industrial Area (SIA) of Kuwait. The study included analysis of pollutant behaviour relative to the wind speed and direction. SIA comprises several large scale industries including three petroleum refineries, two power plants, two fertilizer plants, a cement plant, a chlorine and soda plant, a commercial harbour and two large oil loading terminals. Measurements of 15 parameters have been carried out every 5 minutes using a mobile laboratory fitted with an automatic calibrator and a data storage system. The pollutants studied include methane, non‐methane hydrocarbons (NMHC), carbon monoxide, carbon dioxide, nitrogen oxides (NO, NO₂, and NO _x ), sulphur dioxide, ozone and suspended dust. Meteorological parameters monitored simultaneously include wind speed and direction, air temperature, relative humidity, solar radiation, and barometric pressure. The air quality data collected using the mobile laboratory have been used to calculate the diurnal and monthly variations in the major primary and secondary pollutants. Distribution levels of these pollutants relative to wind direction and speed have also been used in the analysis. The results show large diurnal variations in some pollutant concentrations. Generally, two types of concentration variations have been found, depending on whether the species is a primary or a secondary pollutant. Diurnal variations with two maxima were observed in the concentrations of primary pollutants including NO, SO₂, NMHC, CO and suspended dust, whereas a single maximum was observed for secondary pollutants such as O₃and NO₂. The monthly variations of SO₂and NO _x showed maximum values during the warm months. However, ozone showed a quite marked seasonal variation with maxima during spring and late summer and a minimum during the early summer. The results also indicated a common source for NO _x , SO₂, NMHC, CO and suspended dust to the North‐West (NW) of the monitoring station. Moreover for NO _x and SO₂, another less significant source is to the South‐South‐West (SSW) and South‐West (SW) of the monitoring station.     

Assessment of the chemical components of Famenin groundwater,western Iran

The Faminin area in the semi-arid Hamadan state, western Iran is facing a serious deficiency in groundwater resources due to an increasing demand associated with rapid population growth and agricultural development. The chemical composition of 78 well samples throughout the Faminin area was determined with the aim of evaluating the concentration of the background ions and identifying the major hydrogeochemical processes that control the groundwater chemistry. The similarity between rock and groundwater chemistries in the recharge area indicates a significant rock-water interaction. The hydrochemical types Na–HCO₃ and Na–SO₄ are the predominate forms in the groundwater, followed by water types Ca–HCO₃ and Na–Cl. The high values of electrical conductivity and high concentrations of Na⁺, Cl⁻, SO₄²⁻ and NO₃⁻ in the groundwater appeared to be caused by the dissolution of mineral phases and would appeared to be caused by anthropogenic activities, such as intense agricultural practices (application of fertilizers, irrigation practice), urban and industrial waste discharge, among others.     

Impact of consistent boundary layer mixing approaches between NAM and CMAQ

Discrepancies in grid structure, dynamics and physics packages in the offline coupled NWS/NCEP NAM meteorological model with the U.S. Environmental Protection Agency Community Multiscale Air Quality (CMAQ) model can give rise to inconsistencies. This study investigates the use of three vertical mixing schemes to drive chemistry tracers in the National Air Quality Forecast Capability (NAQFC). The three schemes evaluated in this study represent various degrees of coupling to improve the commonality in turbulence parameterization between the meteorological and chemistry models. The methods tested include: (1) using NAM predicted TKE-based planetary boundary height, h, as the prime parameter to derive CMAQ vertical diffusivity; (2) using the NAM mixed layer depth to determine h and then proceeding as in (1); and (3) using NAM predicted vertical diffusivity directly to parameterize turbulence mixing within CMAQ. A two week period with elevated surface O₃ concentrations during the summer 2006 has been selected to test these schemes in a sensitivity study. The study results are verified and evaluated using the EPA AIRNow monitoring network and other ozonesonde data. The third method is preferred a priori as it represents the tightest coupling option studied in this work for turbulent mixing processes between the meteorological and air quality models. It was found to accurately reproduce the upper bounds of turbulent mixing and provide the best agreement between predicted h and ozonesonde observed relative humidity profile inferred h for sites investigated in this study. However, this did not translate into the best agreement in surface O₃ concentrations. Overall verification results during the test period of two weeks in August 2006, did not show superiority of this method over the other 2 methods in all regions of the continental U.S. Further efforts in model improvement for the parameterizations of turbulent mixing and other surface O₃ forecast related processes are warranted.     

Analysis and prediction of the influence of energy utilization on air quality in Beijing

This work evaluates the influence of energy consumption on the future air quality in Beijing, using 2000 as the base year and 2008 as the target year. It establishes the emission inventory of primary PM₁₀, SO₂ and NO_x related to energy utilization in eight areas of Beijing. The air quality model was adopted to simulate the temporal and spatial distribution of each pollutant concentration in the eight urban areas. Their emission, concentration distribution, and sectoral share responsibility rate were analyzed, and air quality in 2008 was predicted. The industrial sector contributed above 40% of primary PM₁₀ and SO₂ resulting from energy consumption, while vehicles accounted for about 65% of NO_x. According to the current policy and development trend, air quality in the eight urban areas could become better in 2008 when the average concentrations of primary PM₁₀, SO₂ and NO₂ related to energy utilization at each monitored site are predicted to be about 25, 50 and 51 μg/m³, respectively.     

Acute associations between air pollution on premature rupture of membranes in Hefei,China

Numerous studies had focused on the association between air pollution and health outcomes in recent years. However, little evidence is available on associations between air pollutants and premature rupture of membranes (PROM). Therefore, we performed time-series analysis to evaluate the association between PROM and air pollution. The daily average concentrations of PM_2.5, SO₂ and NO₂ were 54.58 μg/m³, 13.06 μg/m³ and 46.09 μg/m³, respectively, and daily maximum 8-h average O₃ concentration was 95.67 μg/m³. The strongest effects of SO₂, NO₂ and O₃ were found in lag4, lag06 and lag09, and an increase of 10 μg/m³ in SO₂, NO₂ and O₃ was corresponding to increase in incidence of PROM of 8.74% (95% CI 2.12–15.79%), 3.09% (95% CI 0.64–5.59%) and 1.68% (95% CI 0.28–3.09%), respectively. There were no significant effects of PM_2.5 on PROM. Season-specific analyses found that the effects of PM_2.5, SO₂ and O₃ on PROM were more obvious in cold season, but the statistically significant effect of NO₂ was observed in warm season. We also found the modifying effects by maternal age on PROM, and we found that the effects of SO₂ and NO₂ on PROM were higher among younger mothers (<?35 years) than advanced age mothers (≥?35 years); however,?≥?35 years group were more vulnerable to O₃ than?<?35 years group. This study indicates that air pollution exposure is an important risk factor for PROM and we wish this study could provide evidence to local government to take rigid approaches to control emissions of air pollutants.

     

Primary NO2 emissions and their impact on air quality in traffic environments in Germany

Background

The decreasing NO_X concentrations at urban measurement stations in Germany are in agreement with the reduction of NO_X emissions from vehicular traffic. However, the measured NO₂ concentrations are stagnating nationwide. In 2010, at more than the half of the urban measurement stations in Germany, annual mean values for NO₂ exceeded the new Europe-wide limit value of 40 μg/m³ (20 ppbv) NO₂. Similar findings are reported from many other member states of the European Union.

Results

The observed trend of the airborne NO₂ concentrations has different reasons. Firstly, the NO₂/NO_x emission ratio has increased significantly during the last two decades. Furthermore, secondary NO₂, caused by the titration reactions of NO with ozone (O₃) and peroxy radicals (RO₂), is responsible for the major fraction (approximately 70%) of the measured NO₂. However, secondary NO₂ shows a highly nonlinear dependency on NO_x and thus, is decreasing much more slowly than expected from the decreasing NO_x levels. Based on the results from the present study, the increased NO₂/NO_X emission ratio can only explain a minor fraction of the observed high airborne NO₂ concentration in the city center.

Conclusions

A further reduction of primary NO₂ emissions, due to improved exhaust gas treatment, will not have a strong influence on urban NO₂ levels, and a further significant reduction of the NO_X emissions, in particular from vehicular traffic, is necessary in order to meet the annual mean limit value for NO₂ of about 20 ppb in the future.     

Selective catalytic reduction of NO x from exhaust of lean-burn engine over Ag-Al2O3/cordierite catalyst

A highly effective Ag-Al₂O₃ catalyst was prepared using the in-situ sol-gel method, and characterized by surface area using nitrogen adsorption, scanning electron microscopy (SEM), and transmission electron microscopy (TEM) techniques. The catalyst performance was tested on a real lean-burn gasoline engine. Only unburned hydrocarbons and carbon monoxide in the exhaust were directly used as reductant (without any external reductant), the maximum NO _x conversion could only reach 40% at 450°C. When an external reductant, ethanol was added, the average NO _x conversion was greater than 60%. At exhaust gas temperature range of 350–500°C, the maximum NO _x conversion reached about 90%. CO and HC could be efficiently oxidized with Pt-Al₂O₃ oxidation catalyst placed at the end of SCR converter. However, NO _x conversion drastically decreased because of the oxidation of some intermediates to NO _x again. The possible reaction mechanism was proposed as two typical processes, nitration, and reduction in HC-SCR over Ag-Al₂O₃.     

Permitted emissions of major air pollutants from coal-fired power plants in China based on best available control technology

Based on the activity level and technical information of coal-fired power-generating units (CFPGU) obtained in China from 2011 to 2015, we, 1) analyzed the time and spatial distribution of SO₂ and NO_x emission performance of CFPGUs in China; 2) studied the impact of installed capacity, sulfur content of coal combustion, and unit operation starting time on CFPGUs’ pollutant emission performance; and 3) proposed the SO₂ and NO_x emission performance standards for coal-fired power plants based on the best available control technology. Our results show that: 1) the larger the capacity of a CFPGU, the higher the control level and the faster the improvement; 2) the CFPGUs in the developed eastern regions had significantly lower SO₂ and NO_x emission performance values than those in other provinces due to better economic and technological development and higher environmental management levels; 3) the SO₂ and NO_x emission performance of the Chinese thermal power industry was significantly affected by the single-unit capacity, coal sulfur content, and unit operation starting time; and 4) based on the achievability analysis of best available pollution control technology, we believe that the CFPGUs’ SO₂ emission performance reference values should be 0.34 g/kWh for active units in general areas, 0.8 g/kWh for active units in high-sulfur coal areas, and 0.13 g/kWh for newly built units and active units in key areas. In addition, the NO_x emission performance reference values should be 0.35 g/kWh for active units in general areas and 0.175 g/kWh for new units and active units in key areas.

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Photochemical indicators of ozone sensitivity: application in the Pearl River Delta,China

Surface O₃ production has a highly nonlinear relationship with its precursors. The spatial and temporal heterogeneity of O₃-NO _x -VOC-sensitivity regimes complicates the control-decision making. In this paper, the indicator method was used to establish the relationship between O₃ sensitivity and assessment indicators. Six popular ratios indicating ozone-precursor sensitivity, HCHO/NO _y , H₂O₂/ HNO₃, O₃/NO _y , O₃/NO _z , O₃/HNO₃, and H₂O₂/NO _z , were evaluated based on the distribution of NO_x- and VOC-sensitive regimes. WRF-Chem was used to study a serious ozone episode in fall over the Pearl River Delta (PRD). It was found that the south-west of the PRD is characterized by a VOCsensitive regime, while its north-east is NO _x -sensitive, with a sharp transition area between the two regimes. All indicators produced good representations of the elevated ozone hours in the episode on 6 November 2009, with H₂O₂/HNO₃ being the best indicator. The threshold sensitivity levels for HCHO/NO_y, H₂O₂/HNO₃, O₃/NO _y , O₃/NO _z , O₃/HNO₃, and H₂O₂/NO _z were estimated to be 0.41, 0.55, 10.2, 14.0, 19.1, and 0.38, respectively. Threshold intervals for the indicators H₂O₂/HNO₃, O₃/NO _y , O₃/NO _z , O₃/HNO₃, and H₂O₂/NO _z were able to identify more than 95% of VOC- and NO _x -sensitive grids. The ozone episode on 16 November 16 2008 was used to independently verify the results, and it was found that only H₂O₂/HNO₃ and H₂O₂/NO _z were able to differentiate the ozone sensitivity regime well. Hence, these two ratios are suggested as the most appropriate indicators for identifying fall ozone sensitivity in the PRD. Since the species used for indicators have seasonal variation, the utility of those indicators for other seasons should be investigated in the future work.

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Miscanthus × Giganteus straw and pellets as sustainable fuels

In this paper we present, for the first time, data on the combustion of Miscanthus × Giganteus straw and pellets. We found that the heating value of Miscanthus is 17.744 MJ/kg. The gaseous emission indices of SO₂, NO _x and total organic carbon (TOC) in the exhaust are reported and compared with the European standards for biomass boilers. On the basis of our results, it is possible to evaluate a net energy yield between 152 and 326 MJ/hectare/year for the cultivation of Miscanthus with an energy balance estimated to be in the range of 7.7–15.4. According to the presented results, it seems reasonable to consider Miscanthus as a promising candidate as alternative fuel.     

Chemical poison and regeneration of SCR catalysts for NO<Subscript><Emphasis Type="Italic">x</Emphasis></Subscript> removal from stationary sources

Selective catalytic reduction (SCR) of NO _x with NH₃ is an effective technique to remove NO _x from stationary sources, such as coal-fired power plant and industrial boilers. Some of elements in the fly ash deactivate the catalyst due to strong chemisorptions on the active sites. The poisons may act by simply blocking active sites or alter the adsorption behaviors of reactants and products by an electronic interaction. This review is mainly focused on the chemical poisoning on V₂O₅-based catalysts, environmental-benign catalysts and low temperature catalysts. Several common poisons including alkali/alkaline earth metals, SO₂ and heavy metals etc. are referred and their poisoning mechanisms on catalysts are discussed. The regeneration methods of poisoned catalysts and the development of poison-resistance catalysts are also compared and analyzed. Finally, future research directions in developing poisoning resistance catalysts and facile efficient regeneration methods for SCR catalysts are proposed.     

Improving simulations of sulfate aerosols during winter haze over Northern China: the impacts of heterogeneous oxidation by NO<Subscript>2</Subscript>

We implemented the online coupled WRF-Chem model to reproduce the 2013 January haze event in North China, and evaluated simulated meteorological and chemical fields using multiple observations. The comparisons suggest that temperature and relative humidity (RH) were simulated well (mean biases are–0.2K and 2.7%, respectively), but wind speeds were overestimated (mean bias is 0.5 m?s^–1). At the Beijing station, sulfur dioxide (SO₂) concentrations were overpredicted and sulfate concentrations were largely underpredicted, which may result from uncertainties in SO₂ emissions and missing heterogeneous oxidation in current model. We conducted three parallel experiments to examine the impacts of doubling SO₂ emissions and incorporating heterogeneous oxidation of dissolved SO₂ by nitrogen dioxide (NO₂) on sulfate formation during winter haze. The results suggest that doubling SO₂ emissions do not significantly affect sulfate concentrations, but adding heterogeneous oxidation of dissolved SO₂ by NO₂ substantially improve simulations of sulfate and other inorganic aerosols. Although the enhanced SO₂ to sulfate conversion in the HetS (heterogeneous oxidation by NO₂) case reduces SO₂ concentrations, it is still largely overestimated by the model, indicating the overestimations of SO₂ concentrations in the North China Plain (NCP) are mostly due to errors in SO₂ emission inventory.

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Diapycnal Mixing in the Thermocline of Lakes: Estimations by Different Methods

In order to evaluate the performance of different methods for estimation of the vertical eddy diffusivity in thermally stratified lakes, two field studies were conducted in Lake Biwa, Japan and Lake Kinneret, Israel. Lake Biwa experienced three typhoons during the campaign while Lake Kinneret experienced high winds in the afternoons. Microstructure profiles were collected by a portable flux profiler (PFP) during calm and disturbed periods. Then, the vertical eddy diffusivity was estimated by three indirect methods. The estimated vertical eddy diffusivities varied more than one order of magnitude, from 4.7× 10⁻⁷ to 7.7× 10⁻⁶ m² s⁻¹. The comparison of results with previous buoyancy flux measurements and scaling arguments showed that the Dillon–Park’s method is not appropriate and Osborn–Cox method performs better than Osborn method in the studied case. Furthermore, the low value of vertical eddy diffusivity within the thermocline suggests that within the thermocline of these lakes, diffusive vertical transport can be neglected.     

The effect of preparation conditions of Pt/Al2O3 on its catalytic performance for the H2-SCR in the presence of oxygen

Selective catalytic reduction of NO _x by H₂ in the presence of oxygen has been investigated over Pt/ Al₂O₃ catalysts pre-treated under different conditions. Catalyst preparation conditions exert significant influence on the catalytic performance, and the catalyst pre-treated by H₂ or H₂ then followed by O₂ is much more active than that pre-treated by air. The higher surface area and the presence of metallic Pt over Pt/Al₂O₃ pre-treated by H₂ or pretreated by H₂ then followed by O₂ can contribute to the formation of NO₂, which then promotes the reaction to proceed at low temperatures.     

Distribution of nitrogen species in groundwater aquifers of an industrial area in alluvial Indo-Gangetic Plains—a case study

The groundwater samples collected from the shallow and deep groundwater aquifers of an industrial area of the Kanpur city (Uttar Pradesh, India) were analyzed for the concentration levels and distribution pattern of nitrogenous species, such as nitrate-nitrogen (NO₃-N), nitrite-nitrogen (NO₂-N), ammonical-nitrogen (NH₄-N), organic-nitrogen (Org-N) and total Kjeldahl-nitrogen (TKN) to identify the possible contamination source. Geo-statistical approach was adopted to determine the distribution and extent of the contaminant plume. In the groundwater aquifers NO₃-N, NO₂-N, NH₄-N, TKN, Org-N and Total-N ranged from 0.10 to 64.10, BDL (below detection limit)-6.57, BDL-39.00, 7.84–202.16, 1.39–198.97 and 8.89–219.43 mg l⁻¹, respectively. About 42% and 26% of the groundwater samples of the shallow and deep groundwater aquifers, respectively, exceeded the BIS (Bureau of Indian Standards) guideline value of 10 mg l⁻¹ for NO₃-N and may pose serious health hazards to the people of the area. The results of the study revealed that the groundwater aquifers of the study area are highly contaminated with the nitrate and indicates point source pollution of nitrate in the study area.