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A publication of

CHEMICAL ENGINEERING TRANSACTIONS VOL. 30, 2012


Guest Editors: Renato Del Rosso Copyright 2012, AIDIC Servizi S.r.l., ISBN 978-88-95608-21-1; ISSN 1974-9791 The Italian Association of Chemical Engineering Online at: www.aidic.it/cet

Impact assessment of odorant sulphur compounds emitted by a fugitive industrial source located in an urban area
Jane M. Santos*a, Neyval C. Reis Jra, Harerton Douradoa, b and Edilson L. Nascimentoa
a b

Universidade Federal do Esprito Santo, Av. Fernando Ferrari 514, Goiabeiras, Vitria, ES, 29.060-970 Brazil Faculdade de Aracruz, R. Professor Berilo Baslio dos Santos, 180, Centro, Aracruz, ES, 29.194-910, Brazil Jane.santos@pq.cnpq.br

The present work investigate the impact of total reduced sulphur compounds (TRS) emissions of coke production plant on a nearby community. TRS emissions from the different sources were estimated using the AP-42 model and through reverse CALPUFF modeling. The relative contribution of TRS emission from the quench tower was evaluated in relation to the other sources. Finally, different scenarios of TRS impact on the nearby population were identified considering the meteorological and operational conditions, peoples complaints and values of TRS measured in the ambient air.

1. Introduction
Metallurgical coke is produced by destructive distillation of coal in an oxygen-free oven until most volatile components are removed and a carbon mass, called coke, remains (Weitkamp et al., 2005). Metallurgical coke is used in iron and steel industry processes as a fuel to reduce iron ore to iron (Diez, Alvarez and Fernndes, 2012). Particles and gaseous (ammonia, volatile organic compounds, and other sulphur compounds) emissions to the atmosphere can be released during coke oven charging and pushing, oven door leakage and quenching (Diez, Alvarez and Barriocanal, 2002). Although, the coal that is charged to the ovens is generally low in sulphur, there are still significant amount of sulphur compounds released to the atmosphere. After thermal distillation, the coke is pushed out of the oven and carried to a quench tower where it can be deluged with water to prevent it from burning after exposure to air. During this process, a large amount of vapour is released to the atmosphere containing sulphur compounds that can cause odour complaints from the nearby population (Hernia, Vigneron and Slingeneijer, 1992). A quench tower is a fugitive volumetric source which releases gases and particles at high temperatures and humidity which makes it difficult to perform analytical measurements of its emission rate of pollutants including the odorant gases such as total reduced sulphur compounds (TRS). This work aims to (i) estimate the TRS emission rate by the quench tower; (ii) evaluate the relative contribution of the TRS emission from the quench tower in comparison with all other existing sources of TRS in the two coke production plants located in the same urban area; (iii) investigate the odour impact caused by the TRS emissions from these coke production industries on the nearby population and (iv) identify scenarios of TRS impact on the nearby population considering the meteorological and operational conditions, peoples complaints and values of TRS measured in the ambient air.

2. Methods
2.1 Sources identification In the urban area where the odour impact assessment is carried out, there are two different coke production plants that can be identified as non-recovery and byproduct plants, and only the nonrecovery plant uses water in the quench tower to deluged the coke after thermal distillation. The emission rates from all the sources releasing TRS from both plants were estimated by using the AP 42 model. However, the source of interest in this study is not contemplated in the AP 42 model due to the difficulties in determining its emission factor. Thus, in order to determine the emission rate of TRS associated to the wet quenching, the CALPUFF (Scire, Strimaitis and Yamartino, 1990) dispersion model was employed in reverse manner using measurements of TRS in the ambient air near the source and meteorological parameters (seventeen different scenarios were used to calculate this emission rate). Then, the CALPUFF model was used again to simulate the TRS plume considering all the existing sources to evaluate the impact on the nearby population. 2.2 Meteorological data Several meteorological data for the region of interest are available: (a) wind speed and direction (5 min average) obtained from a meteorological station located at the non-recovery plant at 30 m above sea level and at a 30 m height; (b) radiation, pressure, temperature, relative humidity, first cloud layer height and mixing layer height, obtained from an airport meteorological station located approximately 6 km from the non-recovery plant; (c) geopotential height, pressure, meridional and zonal wind velocities and wind direction for eight different stratification levels obtained twice a day from the Earth System Research Lab, Physical Sciences Division, NOAA (ESRL/PSD/NOAA), USA; (d) 2-year period (01/01/2008 to 12/31/2009) hourly averages of meteorological data obtained from the MM5 (Mesoscale Model version 5) for a 50 km x 50 km domain (12 km spatial resolution): surface data comprising wind speed and direction, temperature, cloud cover, cloud cover height, pressure, relative humidity and precipitation, as well as 18 level-vertical profiles of wind velocity, temperature and pressure. The prevailing wind direction is N-NE (45% of occurrence frequency), with wind speeds ranging from 2.0 m/s to 4.0 m/s. However, monthly data showed that between April and August, the prevailing wind direction is S-SE, where the population affected by the coke production plants is located. Figure 1 shows the non-recovery plant and the TRS plume affected by prevailing S-SE winds.

3. Results
3.1 Emission rates Among all the sources, the quench tower presented the highest emission rate of TRS (1.42 kg/h) followed by the oven pushing and leakage from the byproduct plant (1.19 kg/h). The other sources emission rates of TRS were much lower. However, the AP 42 showed that there is a significant emission of VOCs from the non-recovery and byproduct plants and ammonia emission from the byproduct plant. These results are summarized in Table 1. 3.2 TRS Concentration Figure 1 and 2 show the relation between wind direction (degrees) and TRS concentration (ppb) measured at the non-recovery plant meteorological station between May and October of 2010. Figure 1 is based on hourly averaged wind direction and concentration while Figure 2 employs 5-minute averages. Results indicate that the highest concentration levels is about 35 ppb (for hourly averages) when the wind direction is between 150 and 215 degrees, and about 95 ppb (5-minute averages) when the wind direction is between 150 and 215 degrees, favoring the occurrence of odour episodes in the affected population. However, it is important to note that for wind directions not favoring impact from the quench tower a TRS concentration of about 2.5 ppb (1-hour averages) and about 5 ppb (5-minute averages) is observed, suggesting the existence of a background TRS concentration; also, this data is related to wind speeds larger than 4.0 m/s (1-hour averages) and 3 m/s (5-minute averages). The use of the short averaging period (5 minutes) eliminates the influence of wind meandering. Figure 2 also shows two occurrences of peak concentration in excess of 10 ppb for a 50-degree wind direction (not favorable for quench tower impact).

Concentration peaks of 40 ppb (1-hour averages) and 95 ppb (5-minute averages) were observed inside the non-recovery plant boundaries. Table 1: TRS emission rate estimates Plant Source TRS emission rate (kg/h) 0,000267 0,00235 1,42 0,96 1,19 VOC emission rate (kg/h) 9.2205 0.698 18.00 8.70 Amonnia emission rate (kg/h) 1.86 0

Non-recovery plant Byproduct plant*

Ovens Stack Quench tower Ovens Stack

* Estimated values, since operational data was not available for evaluation 3.3 Odour complaints from the nearby population Odour complaints from the nearby population between March and April of 2010 are associated with wind direction and TRS concentration (Figure 3) and with wind direction and speed (Figure 4), measured at the non-recovering plant meteorological station. It is possible to note that the majority of complaints (except complaint number 4) occurred when the wind direction was favorable to quench tower impact 160 to 320 degrees, with most complaints between 180 to 200 degrees with wind speeds above 4 m/s. TRS concentrations observed during these complaints were between 1 and 2 ppb. Complaint number 4 was recorded between 23:00 and 08:00 and records showed the wind direction at that specific time and day was not favorable to impact from the quench tower. 3.4 Scenarios of odour impact Based on the available meteorological data, emission rates from AP42 and reverse application of the dispersion model, the scenarios which originated the odour complaints were simulated in CALPUFF in order to determine critical wind directions and TRS concentrations at the non-recovering plant meteorological station site. This information can be used along with operational parameters variation monitoring as a tool for odour management. CALPUFF results indicate concentrations ranging from 1.5 to 15 ppb at the affected area (5 minute concentration peaks). The estimated plume centerline concentration decay between the meteorological station (300 m from the source) and the nearby community (2 km from the source) range from 10 to 20 times so that measured concentrations of 10 ppb (about 6.1 ppb hourly average) are potentially annoying for the nearby community depending on wind direction. In all simulated complaint scenarios, TRS concentration at the meteorological station was higher than 10 ppb, exceeding 20 ppb most of the time, with peaks of 30 ppb. All complaints occurred with wind directions from 180 to 225 degrees with speeds higher than 4 m/s.

(a)

(b) Figure 1: wind direction versus TRS concentration considering wind speed between May and October, 2010, 1-hour averages (a) and 5-minute averages (b) The proposed critical scenarios of odour impact are listed in Table 2 according to wind direction and monitored concentration (5-minute average). Scenario 1 represents situations where, depending on wind direction, the contaminant plume impacting the nearby community is not directly over the monitoring station or just barely touching it. After implementation of the proposed scenarios it was observed that short (less than 5 minutes) concentration peaks over 20 ppb monitored at the meteorological station (which would cause TRS concentrations above the detection threshold at the community) were not perceived by or did not annoy the nearby community (Figure 5), indicating that the proposed scenarios are a conservative estimative and need constant evaluation.

Figure 2: Wind direction versus TRS concentration considering odour complaints. Hourly averages between March and April, 2010.

Figure 3: Wind direction versus Wind speed considering odour complaints. Hourly averages between March and April, 2010 Table 2: proposed scenarios of odour impact Scenario 1 2 3 4 Annoying potential Weak possibility of odour perception Moderate possibility of perception Possibility of odour perception Strong possibility of perception Wind direction 130 - 270 180 - 240 180 - 240 180 - 240 Monitored concentration 1 2 ppb above background 5 10 ppb 10 20 ppb Above 20 ppb

TRS Concentration

Concentration peaks higher


Concentration (ppb)

than 20 ppb did not generated community


complaints.

Figure 4: TRS concentration timeseries measured at the meteorological station between February and March, 2011

4. Conclusion
The present work estimated the emission rate from a non-recovery coke plant and evaluated its relative contribution to odour impact over a nearby community compared with all other sources of TRS in the two coke production plants located in the same urban area (one plant is non-recovery type and the other one is a byproduct type). Odour impact on the community caused by TRS emitted by the two coke plants was investigated and four scenarios of TRS impact on the nearby population were proposed based on meteorological and operational conditions, as well on recorded community complaints and ambient TRS monitoring. Analysis of meteorological records revealed the wind directions corresponding to odour nuisance, which occur between April and September. Emission rates from the two coke plants were estimated in accordance to AP 42 while the emission rate from the nonrecovering plant quench tower was estimated through reverse application of the CALPUFF model. AP 42 also revealed the emission of VOC and ammonia by both coke plants. Records of odour complaints by the affected community showed most complaints corresponded to a wind direction between 180 to 200 degrees and wind speeds above 4 m/s. CALPUFF simulations based on the available meteorological data, monitored TRS concentration and complaints records made possible the proposal of four different scenarios of odour impact to be used with meteorological and TRS concentration monitoring inside the non-recovery plant as a tool for odour management plan. The initial proposal may be conservative as short concentration peaks did not triggered complaints from the community. Further evaluation of monitored data and community complaints must be done as a continuous process in order to define the best scenarios of odour impact.

References Diez, M.; Alvarez, R. & Barriocanal, C. (2002), Coal for metallurgical coke production: predictions of coke quality and future requirements for cokemaking, International Journal of Coal Geology 50(1-4), 389-412. Diez, M.; Alvarez, R. & Fernndez, M. (2012), Biomass derived products as modifiers of the rheological properties of coking coals, Fuel 96(0), 306-313. Hermia, J.; Vigneron, S. & Slingeneijer, C. (1992), Odour Characterization and Control of Volatile Odoriferous Compounds in Coke and Steel Industries, in A.J. Dragt & J. van Ham, ed., Elsevier, , pp. 225--230. Scire, J.; Strimaitis, D. & Yamartino, R. (1990), Model Formulation and users guide for the CALPUFF dispersion model., Prepared for the California Air Resources Board by Sigma Research Corporation, Concord, MA. Weitkamp, E. A.; Lipsky, E. M.; Pancras, P. J.; Ondov, J. M.; Polidori, A.; Turpin, B. J. & Robinson, A. L. (2005), Fine particle emission profile for a large coke production facility based on highly timeresolved fence line measurements, Atmospheric Environment 39(36), 6719-6733.