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THE APPLICATION OF MODELLING TO DESIGN AND OPERATION OF ACTIVATED SLUDGE PROCESSES

B Chambers, J Dudley, WRc, Frankland Road, Swindon, SN5 8YF

ABSTRACT Dynamic process models for wastewater treatment have developed rapidly in recent years and their use for design and optimisation of operation is now widespread in the Water Industry. Most of the available models are centred on activated sludge processes but a few can represent most of the processes used in wastewater and sludge treatment. The main differences between the models are related to the way in which the organic material in wastewater is characterised. The alternatives are COD and BOD-based models and the available evidence would support that either gives acceptable results. Experience of using these models indicates that one of the main problems is acquiring sufficient data for calibration and validation. The requirement for calibration and validation is usually less severe for activated sludge modelling than is the case for biofilm modelling.

INTRODUCTION Traditional process design procedures for wastewater treatment plants were built up empirically over many years by observation of full-scale plant performance. In activated sludge systems, for example, the concepts of sewage retention time, sludge loading rates and final tank upward flow velocities became widely understood and values for each of these parameters were established commensurate with the effluent quality required. The extreme complexity of the microbiological reactions which occur in wastewater treatment made it very difficult to develop design procedures based on reaction kinetics. Process models were developed but the resulting equations were either too simple to be useful or too complex for manual solution. Dynamic process modelling began in the 1970s when computing power became available for solution of the model equations. Initially, modelling activity was largely confined to variations of the activated sludge process but recently the range of available models has increased to cover virtually all the processes proposed for wastewater treatment. The increasing availability, and processing power, of PC equipment has led to the widespread use of modelling for process design and optimisation. In the late 1980s, the UK Water Industry funded the development of the STOAT wastewater treatment simulator as part of the requirement for suitable models to assess the impact of

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storm events on receiving waters and sewerage operation (Foundation for Water Research, 1994; Dudley and Chambers, 1996). In Canada the Wastewater Technology Centre supported the development of GPS-X as a teaching and training tool (Patry and Chapman, 1989). Germany, meanwhile, saw the development of SIMBA, with an initial remit similar to that of STOAT. These models have all increased in capability to support teaching, training, design, operation and process trouble-shooting. Part of the driving force behind this has been the availability of cheap computing power. A modern Intel Pentium computer has greater numerical processing power than a 1970s super-computer. The process models can be split into two types: those addressing single processes, most commonly activated sludge, such as SSSP, EFOR and UCTASP, and those that can be described as whole-works models such as STOAT and GPS-X. There are also models that are centred around activated sludge, with the ability to model multiple lanes but with limited support for other processes, such as SIMBA, EDAR and BioWin. Most of these models rely on similar assumptions about the following: Process solids are described in terms of a few fractions, typically settleable and nonsettleable and volatile and non-volatile suspended solids. The exact specification of these fractions frequently depends on the individual process being modelled (e.g. they might be different for an activated sludge process and a biological filter). The organic fractions in wastewater are described as either BOD or COD and in some cases there is further sub-division into biodegradable and non-biodegradable and soluble and particulate. Obviously, neither BOD nor COD are true components since they both are measures of complex mixtures of individual substances (lumped components). The modelling literature contains extensive discussions about the advantages of either COD or BOD as a lumped parameter but practical experience shows that satisfactory results can be obtained with either. The COD-based IAWQ activated sludge models rely on BOD measurements to estimate the readily biodegradable COD fraction. The reaction mechanisms are modelled by Monod-type equations, or by simple extensions of these equations. The IAWQ activated sludge model popularised the view of the Monod saturation function as a mechanism to switch reactions on and off under anaerobic, anoxic and aerobic environments. The Monod saturation function was originally developed for modelling enzyme receptor sites. Thus, the Monod model approaches the saturation constants as measurable parameters, while the switching function approach treats them as parameters that will take whatever value is required to force the model to match the data. Basic 1-dimensional representations of the flow pattern through the process tanks. Some 2-dimensional models are used, mainly for final settling tanks, but these often use grid meshes simplified to the point where it is arguable that the flow patterns are not being correctly resolved. An improvement in computing power is likely to see an increase in the use of 2-dimensional models and an increase in the grid resolution.

DEVELOPMENT OF ACTIVATED SLUDGE MODELS Activated sludge has been the focus of most modelling research and reliable models now exist of most of the process variants used in full-scale applications such as nitrogen and phosphorus removal systems, sequencing batch reactors, deep-shaft processes etc. Useful

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and accurate activated sludge models contain descriptions of the reactions which occur in aeration tanks and the settlement processes which take place in final tanks. Aeration Tank Models Most of the commercially available dynamic modelling packages use the IAWQ COD-based models to describe activated sludge reaction kinetics. In addition, the STOAT package also contains a BOD-based model. The IAWQ activated sludge models are still under development and most existing software contains what have become known as IAWQ models 1 and 2 (Henze et al, 1986, 1995). Some of the important features of these models are: COD is used as the measure of concentration of organic material in wastewater. The COD is divided into four fractions: soluble and particulate, degradable and nondegradable. The soluble degradable material can be utilised directly by bacteria. The particulate degradable material must first be broken down (hydrolysed) into soluble degradable material. Biomass is lost by decay. Decay is assumed to result in the biomass splitting into two fractions - nondegradable particulate COD and degradable particulate COD. The degradable COD can be utilised for further biomass growth. This allows the IAWQ model to handle endogenous respiration and the effect of COD accumulation through cell death when there is insufficient oxygen available to consume the death products. This mechanism is called the death-regeneration cycle. Nitrogenous material is also divided into soluble and particulate organic nitrogen fractions, and these in turn are further divided into degradable and nondegradable fractions. There is a further fraction, ammoniacal nitrogen. Only ammoniacal nitrogen can be utilised directly by the biomass, so that there is a conversion chain where particulate degradable organic nitrogen is broken down into soluble degradable organic nitrogen, and this is then converted into ammoniacal nitrogen.

Although the bulk of activated sludge modelling world-wide makes use of the IAWQ CODbased model, WRc has developed an alternative BOD-based model (Jones, 1978). Apart from BOD and COD the main difference between the IAWQ and Jones models is the handling of viability. In the IAWQ model bacteria exist in two states: viable bacteria, which utilise COD for growth, and nonviable bacteria, which are dead. COD removal is therefore a growth-related process. The Jones approach was based on earlier research (Wooldridge and Standfast, 1936) that indicated that only a small proportion of respiring bacteria are actually viable. Jones therefore modelled the biomass as being in three states. Viable bacteria, as in the IAWQ model, utilise BOD for growth-related processes. This is modelled using the Monod equation. Nonviable bacteria are unable to take part in growth, but continue to have a residual enzyme activity. This activity is lower than that of viable bacteria, because the dominant means of substrate transport through the cell to the enzyme sites is passive rather than active. The Michaelis-Menten equation is used to model this behaviour. The third state is dead biomass, with no biological activity. Jones model thus decoupled BOD removal from growth. Because of the death-regeneration approach used in the IAWQ model the difference between the two models in practice is less clear cut. Unpublished WRc comparisons between the two models, using data from UK sewage works, indicated that the two models will give

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similar predictions for effluent quality and oxygen demand, providing that both models have been appropriately calibrated. The Jones model in WRc usage is rarely recalibrated, the defaults having been set in 1974. The IAWQ model is commonly recalibrated. The Jones model therefore appears to be more robust. This difference between the two models is not a feature of the use of BOD or COD, but of the choice of representation of bacterial activity. COD models are often described as intrinsically superior to BOD models, because COD can be treated as a conserved substance: COD removal is balanced by COD uptake as new biomass or by oxygen demand. It is therefore possible to do a mass balance on COD in a similar manner to mass balances on (say) carbon. This is not the case with BOD, where typically BOD is calculated as the equivalent of COD oxidised, and there is an additional BOD created that is the equivalent of COD uptake in the biomass. However, the COD models require an estimate of the biodegradable fraction of total COD. This value is commonly estimated through BOD5 or BOD20 tests and where this is done the COD mass balance is weakened. Another common approach has been to measure only total COD and to estimate the degradable fraction as whatever value is required to calibrate the model. This approach then creates uncertainty in the modelling as to where the appropriate effects on effluent quality lie - degradable COD, reaction kinetic parameters, or oxygen transfer limitations. BOD-based modelling has a practical advantage in that there are no adjustments made to the biodegradable amounts of BOD. The progress in activated sludge modelling is splitting into two camps. The first is the baroque approach, exemplified by the IAWQ Activated Sludge Model No. 2. This takes the basis of the IAWQ Activated Sludge Model No. 1 and adds additional processes, with more switching functions, to produce a parameter-rich model. Unfortunately there is often no justification for these parameters, as they are sometimes added for numerical reasons and many of them are therefore defined as having any value that permits the model to match the data. Final Settling Tanks The development of accurate models of final settling tank behaviour has also been the subject of much research. Some of the earlier activated sludge models (Gujer and Henze, 1991) ignored the effects of sedimentation and treated settling tanks as perfect splitters. This is obviously a limitation and most commercially available simulation packages now contain more realistic final settling tank models. The most common approach is to use the Takacs model (Takacs et al, 1991) which models the effects of thickening and clarification but assumes the internal hydraulics are those of a perfect settlement tank. This model is based on the limiting flux theory which was originally developed for steady-state operation, with simple rules to extend the model for dynamic modelling. The basis of the limiting flux method is that if the rate at which solids enter the sludge blanket exceeds the rate at which solids leave then the sludge blanket must grow. Solids are partitioned into two fractions, settleable and non-settleable and only the settleable fraction is used in calculating the settling velocity. The model has been recently reviewed (Jeppsson and Diehl, 1996) and shown to fail to correctly resolve rapid changes in the sludge blanket. Despite this theoretical weakness, the Takacs model is widely used because it does provide predictions that are a reasonable match with measured data. Most of the current models use a one-dimensional flow field, where the flow is either vertically up or down (clarification and thickening) and therefore is an idealisation of the actual flow

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pattern. The alternative is to use two- and three-dimensional models based on computational fluid dynamics (CFD), which describe the real flow field within the tank, including shortcircuiting and recirculation currents. A fine numerical mesh is required to correctly resolve the flow behaviour; using a coarse mesh will provide numerical answers, but may not calculate the correct flow field. The CFD approach is becoming more common but places a large computational burden on the model. As an example, a typical one-dimensional model will use 10 cells to represent the settling tank; a typical two-dimensional CFD model will use 10,000 or more cells to correctly resolve the flow field. Although 2-D final settlement tank models are theoretically more accurate, they are not currently at a stage where they can be used for routine dynamic modelling with a sufficiently fine grid. With accurate calibration, the Takacs model is adequate for most users requirements. MODELLING PRACTICE There are many ways to approach the modelling of an activated sludge process and it is important to commence a new project in a systematic and defined way. The main stages in this approach are discussed below. Data Acquisition All relevant historical flow and compositional data should be collected and analysed for suitability of use in the modelling exercise. In some situations the historical flow and compositional data are either inaccurate or inadequate and there is often no substitute for a short-term intensive survey to characterise the diurnal variation in the wastewater. Flows and compositional data ideally need to be monitored every time they are altered in the environment encompassed by the model. Monitoring should be carried out at the points where flow streams enter and leave the modelled environment. Flows should be recorded every 2 minutes and averaged over 15 to 120 minutes. Ensure that the flowmeter used is suitable for the position where it is being used and that the meters are accurately calibrated. Composition: Each parameter should be monitored upstream and downstream of each modelled process. The parameters that need to be measured depend on whether the model used is COD or BOD based. The following table sets out the parameters that need to be measured in each case.

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IAWQ Model #1 (COD) Soluble BOD5 Particulate BOD5 Soluble biodegradable COD Soluble non-biodegradable COD Particulate non-biodegradable COD Particulate biodegradable COD Volatile suspended solids Non-volatile suspended solids Ammoniacal nitrogen Soluble biodegradable organic nitrogen Particulate biodegradable organic nitrogen Soluble non-biodegradable organic nitrogen Particulate non-biodegradable organic nitrogen Filtered BOD20 (a) Total BOD20 - Filtered BOD20 (b) Note #1 (c) Total COD - (a+b+c)

Jones Model (BOD) Filtered BOD5 Total BOD5 - Filtered BOD5

Ammoniacal Nitrogen Filtered TKN - Ammonia Total TKN - Filtered TKN set to zero set to zero

Volatile SS Total SS - volatile SS Ammoniacal Nitrogen

Note #1: Remove an aliquot of reactor contents from a completely mixed reactor treating the wastewater at an SRT in excess of 10 days and aerate it in a batch reactor. Remove samples periodically and measure for COD until no change occurs in the analysis.

A sampling period of 72 hours duration is recommended (or at least three times the sewage retention time, whichever is the greater), with spot samples taken every one or two hours. The sampling survey should be carried out under dry weather conditions with separate sampling required for unusual events such as storm flows etc. The 72 hour duration should allow the modeller sufficient data to derive a typical 24 hours diurnal pattern. Calibration The model must now be calibrated against the actual data collected from the plant. The model should be run, with all other parameters set to the default values, for at least three sludge ages or hydraulic retention times to allow dynamic equilibrium to be achieved. The model predictions should be compared with the actual results and the modeller must decide which are the appropriate parameters to change to achieve a better fit. If required, certain measured parameters should be remeasured before adjustment within the model. This process can quickly become being very expensive and the modeller must review the cost effectiveness of continuing the calibration. There are many numerical methods for comparing predicted data against actual data, e.g. minimising sum of squares, t-tests etc. which can be used but a graphical comparison, although subjective, is often the best way of carrying out this procedure, because of the relatively limited data that are normally available. It is usual for settling properties to be the parameters which vary most from site to site and the default values in the settling models will usually have to be changed. However, most settling models are relatively easy to calibrate. Activated sludge kinetics are also readily

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calibrated. With the Jones BOD model it is unusual to have to change any of the calibration parameters, while with the COD model, the IAWQ recommendations emphasise the need to examine principally the biomass growth rates and yields. Validation The results from the calibrated model should now be compared against a new set of independent data. If the comparison is unacceptable, the validation data can be used to further calibrate the model and a new set of data must be used to validate the newly calibrated model. CASE STUDIES AND EXAMPLES The following case studies are typical examples of the use of dynamic modelling in process design and optimisation of activated sludge systems. Bellozanne STW, Jersey, Channel Islands This project involved a review of the process strategies to uprate Bellozanne STW to treat additional flow. The sewage works at Bellozanne includes a screening plant, a grit-grease separator, primary treatment and a diffused air activated sludge process followed by a UV disinfection plant. Two 24-hour periods of intensive sampling took place. The data from one survey was used to calibrate the works and from the second survey to validate the model. Figure 1 shows the calibration curves achieved for BOD, solids and ammonia.

Figure 1

Calibration curves for Bellozanne STW

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The curves show a good fit with respect to all three parameters but especially with respect to ammonia. The calibrated model was then used to assess the effect of higher flows through the plant with the following results. The maximum flow rate of 1200 l/s could be treated by the existing primary tanks but caused hydraulic overloading of the activated sludge settlement tanks. The maximum throughput of the activated sludge plant was determined by the maximum effluent suspended solids which permitted adequate disinfection in the downstream UV plant. A new biological treatment plant would be required to operate in parallel to the existing activated sludge plant. Some preliminary sizing of a BAF plant was also carried out. Retrofitting anoxic zones into the existing activated sludge plant would enable better nitrogen removal to be achieved.

Daldowie STW, Glasgow Daldowie STW is a large activated sludge plant to the East of Glasgow, which is owned and operated by West of Scotland Water (WoSW) and treats a DWF of 85,512 m3/d. It consists of a primary sedimentation plant followed by a surface aeration activated sludge plant. The Scottish Environmental Protection Agency (SEPA) indicated that the consent would be changed to require the production of a fully nitrified effluent while receiving higher flows and loads because of the closure of other works. Many simulations were carried out to assess the future ability of the plant to achieve its nitrification consent. Figure 2 shows a STOAT output which demonstrates the effect of a storm event on the existing plant effluent. As can be seen from the summary statistics in this figure the plant would fail the consents for all three main parameters. Further simulations were carried out to assess the effect of the same storm with extra aeration capacity and extra final settlement tank capacity with the results shown in Figure 3. It can be seen that the modified plant would be able to accept the storm load without contravening the consent. This case study showed the ability of modelling to expand the boundaries of design parameters and assess the effect of shock loads on the plant. The project concluded that extra aeration and final settlement capacity would be needed to allow Daldowie STW to accept and treat all the flow that is due to pass to the works in the near future.

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Figure 2

A simulated storm event at Daldowie

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Figure 3

Modified plant receiving storm event

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Phosphorus Removal System The treatment plant in this project used a combination of chemical and biological processes for phosphorus removal. Data for model calibration and validation were provided as COD and hence, COD-based models were used in the exercise. The results from the initial COD calibration are shown in Figure 4. The IAWQ Activated Sludge Model #2 was then used to model phosphorus removal. A simple black box model was developed to correlate phosphorus in and out of the primary tank. The results from this correlation are shown in Figure 5, which demonstrates that a reasonable match was obtained. Chemical processes can often be reasonably correlated by simple steady-state equations, because of the speed of the reactions involved.

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Correlation results for settled sewage phosphorus

A model of the activated sludge process was then developed. The aeration tanks were not designed to promote biological phosphorus removal but the effluent clearly demonstrates that there is such a removal. This removal is associated with the normal phosphorus requirements for biological growth, and this behaviour is included in the IAWQ Activated Sludge Model #2. The results using the default parameter values for that model are shown in Figure 6, which demonstrates that both the magnitude and dynamics of the removal have been matched.
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Model predictions for final effluent phosphorus

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The standard activated sludge models, such as the IAWQ Activated Sludge Model #1, do not include phosphorus removal as a normal growth-related process and therefore predict that the effluent quality is unchanged from the settled sewage. This demonstrates that an appropriate model must be chosen for the modelling requirements. Because of the large number of parameters available in the Model #2, required for the biological phosphorus removal sub-model, it would not be appropriate to use this model where phosphorus removal was not a required part of the study. Design of Aeration Systems for Activated Sludge Plants This area represents one of the first applications of process modelling in the UK. The traditional conservative approach to this design problem involved calculating the maximum flow and load which the plant would receive and then installing aeration capacity to meet this peak demand, often without any means of adjusting air supply downwards during periods of reduced load. Typically the result was good effluent quality but excessive energy costs for aeration. In the 1980s, the UK Water Industry became increasingly concerned about the cost of energy used in activated sludge aeration - typically 70-80% of the energy cost of wastewater treatment, and design procedures for more efficient aeration systems were developed based on the use of process modelling. The main difficulty in designing an aeration system for an activated sludge process lies in matching the oxygen supply to the oxygen demand exerted by the process. Oxygen demand varies spatially, as a function of aeration tank geometry and operating conditions, and also with time, as a result of diurnal and seasonal variations in wastewater flow and load. Ideally, matching oxygen supply and demand results in a constant aeration tank dissolved oxygen concentration under all conditions of operation (typically about 2 mg/l). Process modelling allows the maximum and minimum aeration capacities at various points in an aeration tank to be determined and these values can in turn be used to develop specifications for aeration equipment and dissolved oxygen control systems. The results obtained can be compared with predictions of effluent quality, also obtained by modelling, and an overall design can be established for any given range of influent conditions. Examples of large activated sludge plants designed using process modelling with emphasis on aeration energy saving include Blackburn Meadows (Yorkshire Water), Whitlingham (Anglian Water) and Wanlip (Severn Trent Water). Blackburn Meadows and Whitlingham were among the first plants where energy use in aeration was included in the performance guarantee along with effluent quality. Effluent quality obtained at the Whitlingham site during a performance test lasting for 365 consecutive days is summarised in Table 1.

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Table 1

Effluent quality at Whitlingham during performance tests BOD (mg/l) SS (mg/l) 8.0 16.1 1.0 37.0 40 NH3-N (mg/l) 0.24 1.3 0.02 6.8 7

Mean 95%-ile Minimum Maximum Consent

4.8 10.1 2.0 21.0 2.0

During the performance test, the average oxygen demand satisfied was about 17,700 kg/d for an average energy use of 13,700 kWh/d. This is equivalent to an aeration efficiency of about 1.3 kg/kWh. Aeration efficiency, expressed as described above, or in some equivalent format, is now routinely specified in tender documents. It is difficult, without unacceptable risk, to design a treatment plant which conforms to both effluent quality and energy use specifications without the use of process modelling. Process Modelling as an Aid to Process Selection Following privatisation of the UK Water Industry, there has been an enormous capital investment in new treatment plants. In some Water Utilities, a considerable proportion of this investment has related to the provision of improved treatment facilities at coastal sites. The nature of the catchments at such sites often results in the need to build a plant in a restricted area and it is sometimes found that conventional plants cannot fit into the available space. New processes, such as deep shaft, biological aerated filters (BAF) and sequencing batch reactors (SBRs) have been proposed for such sites. Many of these processes are proprietary and several variants exist. Design and performance information are commercially sensitive and have not been released into the public domain. As a result there is often a lack of independent information available to the end user of such processes, and it can be difficult to select a treatment system for a particular site. Process modelling can be used to identify differences in performance between competing processes and confidence can be placed in the results since the same influent wastewater characteristics can be used for each process. Comparisons can be made in terms of effluent quality, energy use, susceptibility to various process failures and response to catchmentspecific rainfall events. As an example, in the past few years a large number of papers have been published about the advantages of various forms of SBR technology and such processes are now either in operation or under construction at several sites in the UK. SBRs are a variant of the activated sludge process which operate in the same way as the original designs first developed by Arden & Lockett about 80 years ago. A sequence of timed events allows the same process tank to be used for different purposes. A typical sequence might be filling, aeration, settling and decanting. Obviously a number of tanks in parallel are required so that the continuous inflow of sewage can be accepted - thus one tank could be filling while another is being aerated and yet another is undergoing settling.

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The multiple use of the process tanks can result in a substantial area saving compared with conventional plant and this feature translates into a capital cost advantage for similar effluent quality. Parameters such as sludge loading rate and sludge age are not easily calculated for SBR systems and it is difficult to make true performance comparisons with conventional plant. These difficulties can be overcome by process modelling. It is relatively easy to develop process models of SBR systems since the kinetics are identical to conventional activated sludge plants. Model predictions can be used to determine aeration capacities - since several units might be operating in parallel at various stages of the process sequence, the overall peak demand for air does not usually occur at an obvious point in the cycle. It is difficult to understand how an accurate value of peak air demand could be determined without process modelling. The use of process modelling as an aid to process selection has been relatively uncommon. This has probably been caused by the timetables for capital investment which are usually very short and result in a tendency to transfer risk to process plant suppliers. There is some evidence that new processes have not always performed as claimed at some sites - in particular operating costs are often higher than expected. More recently the use of process modelling for evaluating designs in tenders for PFI schemes has become more widespread. CONCLUSIONS 1. 2. 3. 4. Computer modelling of the activated sludge process is an important part of both the design of these facilities and the optimisation of existing plants. Data collection is an important part of modelling which allows the model to be accurately calibrated and validated for all conditions. Given sufficient data, the activated sludge process can be accurately modelled in either COD or BOD. Future developments in models will embrace the more mechanistic approach of structured models rather than the switching function approach. However, the latter approach will remain popular due to the fact that it is relatively easy to understand and calibrate the models and it provides predictions that are adequate for engineering use. Computational fluid dynamics will be used in the future to more accurately model the flow behaviour of final settlement tanks.

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REFERENCES 1. 2. 3. 4. Foundation for Water Research, 1994. Urban Pollution Management, FR/CL 0002. Dudley, J and Chambers, B, 1996. Dynamic Modelling of Wastewater Treatment Processes Using STOAT. WaPUG User Note No. 3. Gujer, W and Henze, W, 1991. Activated sludge modelling and simulation, Water Science and Technology 23(4/6). Henze, M, Grady, C P L, Gujer, W, Marais Gv R and Matsui, T, 1987. Activated Sludge Model No. 1, IAWQ.

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5. 6. 7.

Henze, M, Gujer, W, Mino, T, Matsuo, T, Wentzel, M C and Marais, Gv R, 1995. Activated Sludge Model No. 2, IAWQ. Jeppsson, U and Diehl, S, 1995. Validation of a robust dynamic model of continuous sedimentation. Med Fac Landbouw Univ Gent 60/4b. Jones, G L, 1978. A mathematical model for bacterial growth and substrate utilisation in the activated sludge process, in A James (ed) Mathematical Models in Water Pollution Control, Wiley. Patry, G G and Chapman, D, 1989. Dynamic Modelling and Expert Systems in Wastewater Engineering. Lewis Publishers, Chelsea, MI, USA. Takacs, I, Patry, G G and Nolasco, D, 1991. A dynamic model of the clarificationthickening process, Water Research 25(10).

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10. Wooldridge, W R and Standfast, A F B, 1936. The role of enzymes in activated sludge and sewage oxidation. Biochemical Journal 30(9), 1542-1543.

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