Air emissions at large municipal wastewater treatment plants in Finland for national E-PRTR reporting register T. Fred *, M. Heinonen **, L. Sundell***, and S. Toivikko**** *Helsinki Water, P.O. Box 1100, FIN-00099, The City of Helsinki, Finland (E-mail: [email protected]) **Helsinki Water, P.O. Box 1100, FIN-00099, The City of Helsinki, Finland (E-mail: [email protected]) ***Helsinki Water, P.O. Box 1100, FIN-00099, The City of Helsinki, Finland (E-mail: [email protected]) ****Finnish Water and Waste Water Works Association, Asemapäällikönkatu 7, FIN-00520, Helsinki, Finland (E-mail: [email protected]) Abstract: EC regulation (166/2006) obligates all urban waste water treatment plants above 100.000 PE in European Union area to report their water and air emissions by PRTR protocol from year 2007. There were no general rules or correlations determined to calculate or measure air emissions of municipal wastewater plant. Due to fact that major part of the treatment plants is uncovered, individual air emission study was demanding to implement. In Finland a group of large wastewater treatment plants studied PRTR air emissions based on the samples of Viikinmäki WWTP (780.000 PE), the largest wastewater treatment plant in Finland. Since Viikinmäki WWTP is completely covered, underground plant, ventilation air analyses were possible to implement in full scale. Based on this study, air emissions of Viikinmäki WWTP has been determined and reported to fulfil the PRTR protocol demands. Air emission model was accepted by Finnish Environmental Authorities and the air emission model of Viikinmäki WWTP was used by other, large Finnish WWTPs. Keywords: Air emissions, emission correlation factor, E-PRTR register, NMVOC, PRTR reporting, VOC emissions INTRODUCTION E-PRTR (European Pollutant Release and Transfer Register) regulation (166/2006) of the European Commission obligates PRTR reporting of urban wastewater treatment plants when the capacity of the plant exceeds 100.000 population equivalents, PE. This demand considers both water and air emissions. Since there were no general rules or known methods to fulfil air emission reporting demand of E-PRTR regulation, the group of large Finnish wastewater plants decided to make a common study about this issue. Water and wastewater association of Finland (VVY) had an active role as a co-ordinator of both water and air related emissions in Finland. However, Viikinmäki WWTP of the Helsinki Water has had the leading role of the measuring, modelling and PRTRreporting of the air emissions for the group of large plants. In Finland 13 urban wastewater treatment plants are required to participate E-PRTR reporting system based on the PE size of the plant. Additionally two smaller plants have been involved in the study of the group. Plants of the group have been listed in Table 1. Air emissions at WWTP Normal biological process is developing greenhouse gases like carbon dioxide, methane and N2O. Volatile organic compounds – so called VOC compounds are easily released from the wastewater unit processes were mixing or aeration occurs. Air emission level depends on the evaporation characteristics and concentration of the compound. Carbon dioxide released from the biological process (STOWA, 2007) is not part of PRTR register, since it has no fossil origin. However, so called bio-origin CO2 is determined and shown in this paper. Most of the major Finnish urban wastewater treatment plants have in some level their own power or heat production, which means typically biogas for electricity production or oil usage for heating purposes. Thus typical power production air emissions like SOX, NOX and CO have to be considered what comes to PRTR reporting demands. When burning the biogas, some methane is considered to be released as well due to incomplete burning process. Especially greenhouse gas emissions are strongly depending on the process selection (Yasui et al., 2005; Keller et al., Water Practice & Technology Vol 4 No 2 © IWA Publishing 2009 doi: 10.2166/WPT.2009.029 2003).General background information about the power production of selected WWTP is given as well in Table 1. Table 1: General information of the plants (based on year 2006 statistics) WWTP Helsinki Qave m3/d PE BOD7 Ninfluent Neffluent t/d t/d t/d Digestion Y/N Biogas Mm3/a Heating oil Heating oil Y/N t/a 260 000 820 000 57,4 11,5 1,3 Y 10,0 Y 85 Espoo 90 000 260 000 18,2 4,8 1,2 Y 2,9 Y 295 Turku Jyväskylä Tampere Oulu Lahti Kuopio Pori Kotka Seinäjoki Rovaniemi Lappeenranta Riihimäki Rauma 67 000 42 000 63 000 39 000 20 000 20 000 20 000 12 000 17 000 16 000 16 000 13 000 13 000 200 000 191 000 172 000 137 000 117 000 113 000 112 000 97 000 93 000 90 000 81 000 60 000 26 000 14,0 13,4 12,1 9,6 8,2 7,9 7,9 6,8 6,5 6,3 5,7 4,2 1,8 2,8 2,8 2,7 2,1 0,9 1,2 0,9 0,9 0,7 1,0 1,1 0,7 0,4 0,9 2,0 1,9 1,6 0,2 0,8 0,5 0,2 0,3 0,8 0,4 0,2 0,4 N Y Y N Y Y N N N N N Y N 1,2 1,7 1,5 1,2 0,5 N N N N N Y Y Y Y Y N N N 18 81 18 61 140 Viikinmäki WWTP Viikinmäki WWTP treats the wastewater of 780,000 people in addition to the industry in the areas of Helsinki and neighbouring municipalities. The average wastewater flow rate is 280 000 m3/d and the peak flow as much as 800 000 m3/d. Treatment process is including primary settling, activated sludge system and tertiary denitrification filter. All the sludge is unaerobically digested and dewatered before transport. The process facilities for wastewater and sludge treatment have been excavated into bedrock. Underground areas are 14 hectares and aboveground areas only 3 hectares. Ventilation air flow is more than 100m3/s and all underground ventilation air of the plant is collected into the one point. This makes measurement and calculation of air emissions more accurate (Fred et al., 2008). Figure 1: Viikinmäki WWTP 2 MATERIAL AND METHODS Water phase concentrations of various VOC compounds are generally below detection limit at sewage water (Fred et al., 2008; Wicht, 1996; Wild et al., 1995; Zheng et al., 1994). Therefore it may be impossible to use models, which are based on water phase concentrations for air emission estimation. Air emission mechanisms are divided in the pre-studies into five groups; power production, biological formation in anaerobic conditions, combustion of gas or oil, denitrification process and general volatilization from wastewater surface (Fred et al., submitted; Tchobanoglous et al., 2003). All PRTR compounds were studied based on this emission mechanism idea. In some cases only one phenomena could be found and in case of some other compounds, like methane, CO2 and NMVOC, more than one mechanism occurs simultaneously (Fred et al., submitted). Most of the waste water treatment plants in Finland are uncovered, open-air plants, which makes air emission studies very demanding. At the pre-study phase, most of the compounds had been measured directly in the air phase at the chimney of Viikinmäki WWTP (Fred et al., 2008). Analyses were made in the pre-phase of the project by accepted analyse methods, like TD-GC/MSD-method and FT-IR-gas analyzer, for gases (Fred et al., 2008). Based on these measurements at Viikinmäki WWTP, correlation factors for each compound have been determined and used for estimation of the PRTR emissions of studied plants. Emission correlation factors have been collected in Table 2. Table 2: Emission correlation factors (Fred et al., 2008) Compound CASnumber Methane 74-82-8 Carbon monoxide 630-08-0 Carbon dioxide (bio) 124-38-9 Carbon dioxide (fossil) 124-38-9 Nitrous oxide (N2O) 10024-97-2 Ammonia (NH3) 7664-41-7 Waste water kg/m3 BOD7 kg/kg Nitrogen kg/kg 1,31E-02 Biogas kg/m3 Heating oil kg/kg 7,31E-03 7,33E-03 8,78E-01 1,70E-02 1,79 3,13 1,62E-02 2,47E-5 NMVOC 3,23E-05 Nitrogen oxides (NOx) 6,72E-05 4,35E-03 6,72E-08 Sulphuric oxides (SOx) 5,28E-08 8,76E-05 1,12E-04 1,2-dichloroethane (EDC) 107-06-2 6,77E-09 Dichloromethane (DCM) 75-09-2 2,68E-08 Hexachlorobentzene (HCB) Pentachlorobentzene 118-74-1 8,33E-11 608-93-5 8,38E-11 Tetrachloroethylene (PER) Tetrachloromethane (TCM) 1,1,1-trichloroethane 127-18-4 2,09E-07 56-23-5 6,76E-09 71-55-6 7,88E-09 Trichlorothene 79-01-6 1,78E-07 Trichloromethane 67-66-3 2,18E-08 Benzene 71-55-6 1,15E-07 2,03E-02 3 Data collection After the preliminary phase of measurements and laboratory tests, operational data of each plant was collected and processed by a common data collection sheets. Common and simple data sheet ensures equal data format. Common calculation sheet is also easy to revise when future studies increase the accuracy of the method. Based on correlation factors represented in Table 2, emissions of each wastewater treatment plant have been calculated. RESULTS AND DISCUSSION Wastewater quality at Finnish municipal wastewater treatment plants is very similar as it is shown by some examples in Table 3. Level of PRTR compounds is also generally relatively low in Finnish municipal wastewaters. In most of the cases concentrations were below analyze limit accuracy. Table 3: Wastewater effluent quality of PRTR compounds in Finnish urban WWTPs (2006) Compound 1,2-dichloroethane (EDC) Dichloromethane (DCM) Hexachlorobenzene (HCB) Pentachlorophenol (PCP) Tetrachloroethylene (PER) Trichloroethylene Trichloromethane Benzene Median, µg/l < 0,30 < 0,3 < 0,05 < 0,1 < 0,5 < 0,5 < 0,3 < 0,5 Max,µg/l Environmental Quality Environmental Quality WHO limitation for Standard*, Sea water, drinking water, µg/l Standard*, Surface µg/l water, µg/l <1 10 10 30 2 20 < 0,25 0.03 0.03 < 0,1 2 2 9 <1 10 10 40 <1 10 10 20 < 0,5 12 12 300 <1 10 * Government Decree 1022/2006 Based on this fact the method of one large reference plant, Viikinmäki, was selected for air emission calculations and statistical quality of the correlation factors shown in Table 2 is considered acceptable by Finnish Environmental Authorities. Based on described pre-studies correlation factors were used for all 13 wastewater treatment plants operational data to be able to check the reporting obligation. Modelling of the greenhouse gases and ammonia emissions shows that methane and nitrous oxide exceed the reporting limits what comes to the case of three large wastewater treatment plants of the group. On the other hand carbon dioxide and ammonia emission levels were far below of the reporting limits. Figure 2 shows as an example calculated greenhouse gas and ammonia emissions of the studied plants. NMVOC emissions are based on either usage of heating oil (Tata et al. 2003) or normal release of the VOC from the waste water. Figure 3 shows the emissions of the power production. Nitrous oxide (NOX) emission of the Viikinmäki WWTP is 50 % of the reporting limit and other WWTP has approximately 10 % emissions of the reporting limit. All other NMVOC emissions are marginal compared to limits given by PRTR guidance of EU regulation. In case of CVOC compounds and benzenes calculation shows similar results giving approximately 0 - 10 % fraction of the reported emission level. 4 ri tka nk Es i po o Tu r k Jy vä u s T a kylä m pe re Ou lu La ht Ku i op io Po ri Ko S e tk a in R o ä jo k v La a n i pp ie m ee nr i a R i nta ih im ä R a ki um a He lsi Se inä j R o oki va ni La em pp i ee nr an ta Ko Po o ht i op i La lu re Ou t/a Ku u ylä rk pe sk m vä Ta Jy Tu po o nk i nk Es i po o Tu J y rk u vä sk T a ylä m pe re Ou lu La ht Ku i op io Po ri Ko S e tk a in ä R o jo k i La van p p ie m ee i nr a R i nta ih im äk Ra i um a He l si nk Es i po o Tu J y rk u vä sk T a ylä m pe re Ou lu La ht Ku i op io Po ri Ko S e tk a in R o ä jok i v La an p p iem ee nr i a R i nta ih im äk Ra i um a He l si t/a nk Es i po o Tu r ku Jy vä sk y T a lä m pe re Ou lu La ht Ku i op io Po ri Ko tka Se inä R o jok i v La an pp iem ee i nr a R i nta ih im äk Ra i um a 1000 Es He lsi nk Es i po o Tu r k Jy u vä sk T a ylä m pe re Ou lu La ht Ku i op io Po ri Ko tka Se in ä R o jo k va i La n p p iem ee i nr a R i nta ih im äk Ra i um a He lsi nk Es i po o Tu r k Jy vä u sk y T a lä m pe re Ou lu La ht Ku i op io Po ri Ko t S e ka in ä R o jo k i L a van p p ie m ee i nr a R i n ta ih im äk Ra i um a He lsi 200 150 He lsi nk Es i po o Tu r k Jy vä u sk T a ylä m pe re Ou lu La ht Ku i op io Po ri Ko S e tka in ä R o jo k i L a van p p ie m ee nr i a R i nta ih im äk Ra i um a He lsi t/a Methane, CH4 t/a 400 70 350 60 300 50 250 40 Reporting limit 100 t/a 100 50 0 Carbon dioxide, CO2 Reporting limit 100 000 t/a 100 000 90 000 80 000 70 000 60 000 50 000 40 000 30 000 20 000 10 000 0 Reporting limit 100 t/a 100 90 80 70 60 50 40 30 20 10 0 t/a Reporting limit 500 t/a 0 5 Nitrous oxide, N2O 30 20 10 Reporting limit 10 t/a 0 t/a Ammonia, NH3 10,0 Reporting limit 10 t/a 1,0 0,1 0,0 Figure 2: Calculated greenhouse gas and ammonia emissions Nitrogen oxides, NOX t/a Sulphuric oxides, SOX 1000,000 Carbon monoxide, CO Reporting limit 150 t/a 100,000 10,000 1,000 0,100 0,010 0,001 0,000 kg/a NMVOC 100 Figure 3: Calculated emissions of power production and NMVOC emissions Reporting limit 100 t/a 100 10 10 1 1 0 Modeling of the PRTR emissions shows that three largest municipal wastewater plants – Helsinki, Espoo and Turku, exceed reporting level in case of methane and nitrous oxide. All other WWTP are far behind and probability to achieve reporting limit in any compounds is very small. However the future improvements in nitrogen removal level might cause reporting responsibility of nitrous oxide in case of Tampere and Jyväskylä. Reported compounds and treatment plants in Finland are collected in Table 4. Table 4: Reported PRTR compounds in Finland, reporting year 2007 WWTP Reported WWTP compound compound Helsinki CH4, N2O Pori Espoo CH4, N2O Kotka Turku Jyväskylä Tampere Oulu Lahti Kuopio N2O - Reported - - Seinäjoki Rovaniemi Lappeenranta Riihimäki Rauma - CONCLUSIONS The study shows that the reliable measurements for air emissions for complete ventilated WWTP can be conducted. Possibility to make measurements in ventilation air stream at a single point makes emission estimations very accurate compared to the other estimation methods. Accuracy is high enough if the results are used for the evaluation whether the reporting limits of the PRTR compounds are exceeded or not at some other WWTP’s. By using generated simplified model, the demands of the reporting of the PRTR can be fulfilled also in the uncovered urban waste water treatment plants, where the air emission analysing is very difficult to arrange in a proper way. From the perspective of the PRTR reporting limits, it seems that the greenhouse gas emissions of urban wastewater treatment plant can be significant at reporting point of view. In case of Finland reporting limit is exceeded with nitrous oxide (N2O) and methane (CH4) emissions in Helsinki and Espoo. Nitrous oxide emissions caused reporting responsibilities at the Turku WWTP. Volatile organic compounds (VOC) emissions are low due to very strict control of industrial discharges to municipal sewer based on the measurements and models made for this study. 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