United States Prevention, Pesticides EPA712-C-08-004 Environmental Protection And Toxic Substances October 2008 Agency (7101) 4>EPA Fate, Transport and Transformation Test Guidelines OPPTS 835.3240 Simulation Test—Aerobic Sewage Treatment: A. Activated Sludge Units ------- INTRODUCTION This guideline is one of a series of test guidelines that have been developed by the Office of Prevention, Pesticides and Toxic Substances (OPPTS), United States Environmental Protection Agency for use in the testing of pesticides and toxic substances, and the development of test data to meet the data requirements of the Agency under the Toxic Substances Control Act (TSCA) (15 U.S.C. 2601), the Federal Insecticide, Fungicide and Rodenticide Act (FIFRA) (7 U.S.C. 136, et seq.), and section 408 of the Federal Food, Drug and Cosmetic (FFDCA) (21 U.S.C. 346a). OPPTS developed this guideline through a process of harmonization of the testing guidance and requirements that existed for the Office of Pollution Prevention and Toxics (OPPT) in Title 40, Chapter I, Subchapter R of the Code of Federal Regulations (CFR), the Office of Pesticide Programs (OPP) in publications of the National Technical Information Service (NTIS) and in the guidelines published by the Organization for Economic Cooperation and Development (OECD). For additional information about OPPTS harmonized guidelines and to access this and other guidelines, please go to http://www.epa.gov/oppts and select "Test Methods & Guidelines" on the left side menu. ------- OPPTS 835.3240: Simulation test—aerobic sewage treatment: A. activated sludge units (a) Scope—(1) Applicability. This guideline is intended for use in testing pursuant to the Toxic Substances Control Act (TSCA) (15 U.S.C. 2601). (2) Background. The source material used in developing this harmonized OPPTS guideline is Organization for Economic Cooperation and Development (OECD) test guideline 303 (adopted 22 January 2001), available from Source OECD at http ://masetto. sourceoecd.org/. (b) Purpose. The test method described in this guideline is designed to determine the elimination and primary and/or ultimate biodegradation of water-soluble organic substances by aerobic microorganisms in a continuously operated test system simulating the activated sludge process. The method is designed to ascertain whether the substances tested (usually those known to be inherently but not readily biodegradable) can be biodegraded within the limits imposed in typical wastewater treatment plants. The results are expressed in terms of percentage removal and percentage biodegradation. Because this is a simulation test, it is assumed that results can be extrapolated to predict elimination in full-scale treatment plants, provided that critical parameters such as temperature, sludge retention time (SRT) and initial test substance concentration are in the same range. Normally tests are performed at only one nominal concentration of sludge solids or one nominal SRT. However, variants of the principle test method are also described in which test substance is present at low concentrations (e.g. ng/1) considered more typical of wastewaters; and in which the SRT is controlled within much narrower limits as happens in full-scale treatment plants. (c) Overview—(1) General Concepts. In the 1950s it was realized that the newly introduced surfactants caused excessive foaming in wastewater treatment plants and in rivers. They were not fully removed in aerobic treatment and in some cases limited the removal of other organic matter. This instigated many investigations into how surfactants could be removed from wastewaters and whether new substances produced by industry were amenable to wastewater treatment. Because it would have been impractical and very costly to distribute each new material and to monitor large-scale treatment plants, model units have been developed that represent the two main types of aerobic biological wastewater treatment (activated sludge and percolating, or trickling, filtration). (2) Activated sludge units, (i) Model activated sludge units have been described ranging in size from 300 ml up to about 2000 ml. Some closely mimic full-scale plants, having sludge settlement tanks with settled sludge being pumped back to the aeration tank, while others provide no settlement facilities; e.g. Swisher (see paragraph (p)(l) of this guideline). The size of the apparatus is a compromise. On the one hand, it must be large enough for successful mechanical operation and for the provision of sufficient volume of samples without affecting the operation, while on the other hand it should not be so large that it demands excessive space and materials. (ii) Two forms of apparatus that have been extensively and satisfactorily used are 1 ------- the Husmann units (see paragraph (p)(2) of this guideline) and porous pot units (see paragraphs (p)(3) and (p)(4) of this guideline), first used in the study of surfactants; these are described in this guideline. Others have also been used satisfactorily, e.g. Eckenfelder (see paragraph (p)(5) of this guideline). Because of the relatively high cost and effort of applying this test, simpler and cheaper screening tests, now embodied in 301 A-F, were investigated in parallel. Experience with many surfactants and other chemical substances have shown that substances that passed the screening tests (i.e. were readily biodegradable) also degraded in the activated sludge simulation test. Some of those failing the screening tests passed the inherent biodegradability tests (302 A, B) but only some of this latter group were degraded in the activated sludge test, while those substances that failed tests for inherent biodegradability did not degrade in the activated sludge test (see paragraphs(p)(6), (p)(7) and (p)(8) of this guideline). (iii) For some purposes simulation tests carried out under a single set of operating conditions are sufficient. The results are expressed as a percentage removal of the test substance or of dissolved organic carbon (DOC). A description of such a test is given in this guideline. However, unlike the previous 303A (see paragraph (a)(2) of this guideline), which described only one type of apparatus treating synthetic sewage in the coupled mode using a relatively crude method of sludge wastage, this text offers several variations. Alternatives to the type of apparatus, mode of operation, sewage and sludge wastage removal are described. This text closely follows that of the ISO Standard 11733 (see paragraph (p)(9) of this guideline), which was carefully scrutinized during its preparation, though the method has not been subject to a ring test. (iv) For other purposes the concentration of the test substance in the effluent needs to be known more accurately and for this a more extensive method is needed. For example, the sludge wastage rate must be more precisely controlled throughout each day and throughout the period of the test, and units have to be run at several wastage rates. For a fully comprehensive method, tests should also be run at two or three different temperatures: such a method is described by Birch (see paragraphs (p)(10) and (p)(ll) of this guideline) and summarized in paragraph (n) of this guideline. However, present knowledge is insufficient to decide which of the kinetic models is (are) most appropriate for describing the biodegradation of substances in wastewater treatment and in the aquatic environment generally. The application of Monod kinetics, given in paragraph (n) as an example, is limited to substances present at 1 mg/1 and above, but in the opinion of some, even this remains to be substantiated. Tests at concentrations more truly reflecting those found in wastewaters are described in paragraph (m) of this guideline. (3) Percolating (trickling) filters, (i) Much less attention has been given to model percolating filters, perhaps because they are more cumbersome and less compact than activated sludge plant models. Gerike et al (see paragraph (p)(12) of this guideline) developed trickling filter units and operated them in the coupled mode (see paragraphs (a)(2) and (p)(12) of this guideline). These filters were relatively large (height 2 m; volume 60 1) and each required as much as 2 1/h of sewage. Baumann et al (see paragraph (p)(13) of this guideline) simulated trickling filters by inserting polyester fleece strips into 1 m tubes (14 mm int. diameter) after the strips had been immersed in concentrated activated sludge for 30 min. The test substance as sole C source in a mineral salts solution 2 ------- was fed down the vertical tube and biodegradation was assessed from measurements of DOC in the effluent and CC>2 in the issuing gas. (ii) Biofilters have been simulated in another way (see paragraph (p)(14) of this guideline): the inner surfaces of rotating tubes, inclined at a small angle to the horizontal, were fed with sewage (250 ml/h) with and without the test substance, and the collected effluents were analyzed for DOC and/or the specific substance. This method is described in part B of OECD 303 (cited in paragraph (a)(2) of this guideline) and the corresponding U.S. EPA Fate, Transport and Transformation Test Guidelines no. 835.3260, on biofilms (cited in paragraph (p)(15) of this guideline). (d) Principle of the test. (1) This method is designed to determine the elimination and the primary and/or ultimate biodegradation of water-soluble organic substances by aerobic microorganisms in a continuously operated test system simulating the activated sludge process. An easily biodegradable organic medium and the organic test substance are the sources of carbon and energy for the microorganisms. (2) Two continuously operated test units are run in parallel under identical conditions that are chosen to suit the purpose of the test. Normally the mean hydraulic retention time (HRT) is 6 h and the mean sludge age (= sludge retention time or SRT) is 6 to 10 d. Sludge is wasted by one of two methods. The test substance is normally added at a concentration of between 10 mg/1 and 20 mg/1 as DOC to the influent (organic medium) of one of the units. The second unit is used as a control to determine the biodegradation of the organic medium. (3) In frequently taken samples of the effluents, the DOC (preferably) or chemical oxygen demand (COD) is determined, together with the concentration of the test substance (if required) by specific analysis, in the effluent from the unit receiving the test substance. The difference between the effluent concentrations of DOC or COD in the test and control units is assumed to be due to the test substance or its organic metabolites. This difference is compared with the influent concentration of DOC or COD due to the added test substance in order to determine the extent of its elimination. (4) Biodegradation normally can be distinguished from bioadsorption by careful examination of the elimination vs. time curve, and usually can be confirmed by applying a test for ready biodegradation using an acclimated inoculum taken from the activated sludge unit receiving test substance. (e) Applicable ASTM standards. Refer to the documents referenced in paragraph (p)(16) of this guideline for the standards in paragraphs (e)(l) through (e)(7) of this guideline: (1) Dl 129-90 Standard Terminology Relating to Water. (2) Dl 193-91 Standard Specifications for Reagent Water (Federal Test Method and Standard No. 7916). ------- (3) D1293-84 Standard Test Methods for pH of Water. (4) D2579-85 Standard Test Method for Total and Organic Carbon in Water. (5) D4375-90 Standard Terminology for Basic Statistics in Committee D-19 on Water. (6) D4839-88 Standard Test Method for Total Organic Carbon in Water by Ultraviolet, or Persulfate Oxidation or Both, and Infrared Detection. (7) E178-80 Standard Practice for Dealing with Outlying Observations. (f) Information on the test substance—(1) General. The purity, water solubility, volatility and sorption characteristics of the test substance should be known to enable correct interpretation of results. Normally, volatile and insoluble substances cannot be tested unless special precautions are taken. The chemical structure, or at least the empirical formula, should also be known in order to calculate theoretical values and/or check measured values of parameters; e.g. theoretical oxygen demand (ThOD), DOC and COD. (2) Poorly water-soluble substances, (i) Few reports seem to have been published on subjecting poorly water-soluble and insoluble substances to tests simulating wastewater treatment (see paragraphs (p)(17), (p)(18) and (p)(19) of this guideline). (ii) There is no single method of dispersal of the test material that is applicable to all insoluble substances. Two of the four methods described in ISO 10634 (see paragraph (p)(20) of this guideline) appear suitable for attempting to disperse test substances for activated sludge simulation testing; they are the methods using emulsifying agents and ultrasonic energy. The stability over at least a 24-h period of the resulting dispersion should be established. Suitably stabilized dispersions, contained in a constantly stirred reservoir, would then be dosed to the aeration tank separately from the domestic (or synthetic) sewage. (iii) If the dispersions are stable, investigate how the test substance concentration can be determined in the dispersed form. It is unlikely that DOC will be suitable, so that a specific analytical method for the test substance would have to be established that could be applied to effluents, effluent solids and activated sludge. The fate of the test substance in the simulation of the activated sludge process would then be determined for both liquid and solid phases. Thus, a mass balance would be established to decide whether the test substance had been biodegraded. However, this would indicate only primary biodegradation. Demonstration of ultimate biodegradation should be attempted by applying a respirometric test for ready biodegradability (301 B, C or F) using as the inoculum sludge exposed to the test substance in the simulation test. (3) Volatile substances—(i) Applicability. The application of wastewater treatment simulations to volatile substances is both debatable and problematic. As with poorly water-soluble test substances, very few reports seem to have been published describing simulation tests using volatile substances. A conventional type of complete- 4 ------- mixing apparatus is adapted by sealing the aeration and settling vessels, measuring and controlling the air flow using flowmeters, and passing the exit gas through traps to collect volatile organic matter. In some cases, a vacuum pump has been used to draw the exit gas through a cold trap or a purge-trap containing Tenax and silica gel for gas chromatographic analyses. The test substance present in the trap can be determined analytically. (ii) Stripping test. The test is carried out in two parts. The units are first operated without sludge but with the synthetic wastewater plus test substance being pumped into the aeration tank. Influent, effluent and exit gas samples are collected and analyzed for the test substance for a few days. From the data collected, the percentage (Rvs) of the test material stripped from the system may be calculated. (iii) Biological test. Then the biological (i.e. with sludge) test is performed under operating conditions identical to those in the stripping study. DOC or COD measurements are also made to check that the units are performing efficiently. Occasional analyses are made to determine the test substance in the influent, effluent and exit gas in the first part of the test; and after acclimation, more frequent analyses are made. Using the data obtained after steady-state removal is achieved, the percentage removal of the test substance from the liquid phase by all processes (Rx) (physical and biological) may be calculated, as well as the proportion (Rv) stripped from the system. (iv) Calculations. (A) In the non-biological (stripping) test, the percentage (Ryp) of the test material stripped from the system is %RVP = SVP/SIP xioo where RVP = removal of test substance by volatilization (%), SVP = test substance collected in trap expressed as equivalent concentration in liquid phase (mg/1), SIP = test substance concentration in influent (mg/1). (B) In the biological test, the percentage (Rv) of the test material stripped from the system is %Rv = Sv/Si x 100 where RV = removal of test substance by volatilization in biological test (%), Sv = test substance collected in trap in biological test, expressed as equivalent concentration in liquid influent (mg/1), Si = test substance concentration in influent (mg/1). (C) In the biological test, the percentage (Rx) of the test substance removed by all processes is given by: ------- %RT = (l-SE/Si) xlOO where SE = concentration of test substance in the (liquid) effluent (mg/1). (D) Thus, the percentage (RBA) removed by biodegradation plus adsorption can be calculated from: %RBA = (RT-RV) Separate tests should be carried out to determine whether the test substance is adsorbed; if it is, then a further correction may be made. (E) A comparison between the proportion of test substance stripped from the biological (Ry) and non-biological test (Ryp) systems indicates the overall effect that biological treatment has had on the emission of the test substance into the atmosphere. Example: Benzene Sludge retention time = 4 days A synthetic sewage; retention time = 8h SIP = Si = 150 mg/1 S Vp = 150 mg/1 ( SEP = 0) Sv = 22.5 mg/1 SE = 50 Thus, RVp = 1 00%, Rv = 15% RT = 100% and RBA = 85%. If benzene is assumed not to be adsorbed onto sludge, the results suggest that it is removed by a combination of stripping and (mostly) biodegradation. (4) Inhibitory substances — (i) Information on the toxicity of the test substance to microorganisms may be useful for selecting appropriate test concentrations and may be essential for the correct interpretation of low biodegradation values. (ii) A substance (or wastewater) may not be degraded or removed in the simulation test and may even have an inhibitory effect on the sludge microorganisms. Other substances may be biodegraded at low concentrations but inhibitory at higher concentration. Inhibitory effects may have been revealed at an earlier stage or may be determined by applying a toxicity test, using an inoculum similar or identical to that used in the simulation test (see paragraph (p)(21) of this guideline). Useful microbial toxicity tests include inhibition of oxygen uptake (OECD Guideline 209; ISO Standard 8192)(see paragraph (p)(22) of this guideline) and inhibition of growth of sludge organisms (ISO 15522)(see paragraph (n)(24) of this guideline). ------- (iii) In the activated sludge simulation test, if the test substance inhibits activity of the activated sludge, the percentage removal of DOC (and biochemical oxygen demand or BOD; COD; or NH4+ ) of the organic medium on treatment will be decreased by the presence of the test substance. If this occurs, the test should be repeated reducing the concentration of the test substance until a level is reached at which no inhibition occurs, and perhaps further reducing the concentration until the test substance is biodegraded. However, if the test substance (or wastewater) has adverse effects on the process at all concentrations tested, the indications are that the substance is difficult, if not impossible, to treat biologically. In this case it may be worth repeating the test with activated sludge from a different source and/or subjecting the sludge to a more gradual acclimation. (iv) Conversely, if the test substance is removed by biodegradation at the first attempt in this test, its concentration could be increased if it is considered useful to know whether the substance could be inhibitory at some higher level. It also should be remembered that the activated sludge population can change, so that with time the microorganisms may become more tolerant of an inhibitory substance. (v) The overall percentage removals RO, for BOD, DOC and COD for the test and control units are calculated as shown in this paragraph: where I = influent concentration of BOD, DOC or COD, for test or control vessels (mg/1) E = respective effluent concentrations (mg/1). I and E must be corrected for the DOC due to the test substance in the test units; otherwise the calculations of percentage inhibition will be incorrect. The degree of inhibition caused by the presence of the test material can be calculated from: % inhibition = 100 (Rc - Rt)/ Rc where RC = percentage removal in the control vessels Rt = percentage removal in the test vessels (g) Pass levels. (1) Because this test is intended to simulate activated sludge wastewater treatment rather than measure "ready" or "inherent" biodegradability, there are no pass or fail criteria. The levels of removal observed should approximate levels of removal expected in full-scale activated sludge treatment systems. (2) Percentage removal obtained in this test can therefore be used to calculate probable environmental concentration, for application in hazard assessment. Results tend to follow an all-or-nothing pattern. For example, in several studies of pure substances, the percentage removal of DOC was found to be >90% in more than three quarters and >80% in over 90% of substances that showed any significant degree of biodegradability. (3) Relatively few substances (e.g. surfactants) are present in sewage at the 7 ------- concentrations (about 10 mg C/l) used in this test. Some substances may be inhibitory at these concentrations, while the kinetics of removal of others may be different at low concentrations. A more accurate assessment of their biodegradation could be made by using modified methods, using realistically low concentrations of the test substance, and the data collected could be used to calculate kinetic constants. However, the necessary experimental techniques have not yet been fully validated and neither have kinetic models, which describe the biodegradation reactions, been established. (h) Reference substances. To ensure that the experimental procedure is being carried out correctly, it is useful to include one or more reference substances, i.e. a substance whose behavior is known, when test substances are investigated. Examples of such substances are adipic acid, 2-phenyl-phenol, 1-naphthol, diphenic acid and 1- naphthoic acid (see paragraphs (p)(6), (p)(7) and (p)(8) of this guideline). (i) Reproducibility of test results. (1) There have been far fewer reports of simulation tests than of tests for ready biodegradability. Reproducibility between (simultaneous) replicates is good (within 10-15%) for test substances degraded by 80% or more, but for less well-degraded substances, variability is greater. Also, with some borderline substances widely disparate results (e.g. 10% vs. 90%) have been recorded on different occasions within the 9 weeks allowed in the test. (2) Little difference has been found in results obtained with the two types of apparatus (see paragraph (c)(2)(ii) of this guideline), but some substances have been more extensively and consistently degraded in the presence of domestic sewage than with OECD synthetic sewage. (j) Description of the test method—(1) General. The test system for one test substance consists of a test unit and a control unit; but when only specific analyses are performed (i.e. primary biodegradation is determined), only a test unit is required. One control unit can be used for several test units receiving either the same or different test substances. In the case of coupling (see paragraph (1)(5) of this guideline) each test unit should have its own control unit. The test system may be either a Husmann unit (see Figure 1), or a porous pot (see Figures 2 and 3). In both cases, storage vessels of sufficient size for the influents and effluents are needed, as well as pumps to dose the influent, either mixed with solution of the test substance or separately. ------- Figure 1. Activated sludge treatment model test system: Husmann unit Air B \, 'Air I t H V C G D I F A. Storage vessel B. Dosing pump C. Aeration chamber (3 1 capacity) D. Settling vessel E. Air lift pump F. Collection vessel G. Aerator H. Air flow meter Figure 2. Activated sludge treatment model test system: porous pot A. Storage vessel B. Dosing pump C. Porous aeration vessel D. Outer impermeable vessel c F G Air E. Collection vessel F. Diffuser G. Air flow meter ------- Figure 3. Detailed diagram of typical porous pot aeration vessel Internal diameter of porous pot 14cm Internal diameter of outer pot 10.6cm Side of cone outer 9.9cm Side of cone inner 10 ------- (2) Activated sludge model system: Husmann unit. Each unit consists of an aeration vessel with a known capacity of about 3 1 of activated sludge and a separator (secondary clarifier) that holds about 1.5 1 (see Figure 1). To some extent the volumes can be changed by adjusting the height of the separator. Vessels of different sizes are permissible if they are operated with comparable hydraulic loads. If it is not possible to keep the temperature in the test room in the desired range, the use of water-jacketed vessels with temperature controlled water is recommended. An airlift pump or a dosing pump is used to recycle the activated sludge from the separator to the aeration vessel, either continuously or intermittently at regular intervals. (3) Activated sludge model system: porous pot. (i) The porous pot system (see Figures 2 and 3) consists of an inner, porous cylinder with a conical bottom held in a slightly larger vessel of the same shape, but made of an impervious plastic material. A suitable material for the porous vessel is porous polyethylene of maximum pore size 90 jim and 2 mm thickness. Separation of the sludge from the treated organic medium is effected by differential passage through the porous wall. Effluents collect in the annular space from where it overflows into the collecting vessel. No settlement occurs and hence there is no sludge return. The whole system may be mounted in a thermostatically controlled water bath. (ii) The feature that distinguishes this test from other activated sludge simulation tests is the retention of the activated sludge by the porous liner, which eliminates the need for a secondary clarifier and facilitates control of a critical parameter, the SRT. (iii) The porous pot system provides a laboratory-scale simulation of activated sludge wastewater treatment because settled domestic sewage is used as the feed and key control parameters are maintained in the ranges typical of such treatment. These parameters include temperature, dissolved oxygen (DO) concentration, HRT and SRT. Mixed liquor volatile suspended solids (MLVSS) are monitored but not controlled. The porous pots are allowed to attain steady state at an MLVSS level commensurate with the other key control parameters. (iv) Porous pots can be completely sealed and tests using 14C-labeled test substances are possible. Carbon dioxide in the exhaust gas and bicarbonate in the effluent can be used together to assess the extent of mineralization, and levels of radiolabel in the sludge and in the aqueous phase may also be determined. (4) Aeration, (i) For aeration of the sludge in the aeration vessels of both systems, suitable techniques are required, for example sintered cubes (diffuser stones) and compressed air. The air should be cleaned, if necessary, by passing it through a suitable filter and washing. Sufficient air should pass through the system to maintain aerobic conditions and to keep sludge floes in suspension at all times during the test. (ii) An oil-free compressor is needed for supplying compressed air to the aeration vessel. (5) Pumps. Suitable pumps are needed for dosing activated sludge units with test 11 ------- substance solutions and sewage at the correct rates (0-1.0 mL/min for test substance solutions, 5-20 mL/min for sewage). An additional pump is needed to waste sludge from the pot, unless sludge is wasted manually. Low rates of sludge wastage are attained using a pump set at a high flow rate but operating intermittently. The actual flow is calculated as shown in this paragraph: flow = [pump throw (mL/min) x pumping time (sec)1 timer cycle (sec) For example, when the pump is operating for 10 sec each minute, the timer cycle is 1 min (60 sec), and the pump throw is 3 mL/min, the wastage rate is 0.5 mL/min. (6) Filtration apparatus or centrifuge. A device is needed for filtering samples that uses membrane filters of suitable porosity (nominal aperture diameter 0.45 |im) and that adsorbs soluble organic substances and releases organic carbon to a minimum degree. If filters are used that release organic carbon, first wash the filters carefully with hot water to remove teachable organic carbon. Alternatively, a centrifuge capable of producing 40,000 m/s2 may be used. (7) Other equipment, (i) Analytical apparatus as needed, to determine (A) DOC and total organic carbon (TOC), or COD; (B) Specific substance; (C) Suspended solids, pH, oxygen concentration in water; (D) Temperature, acidity and alkalinity; (E) Ammonium, nitrite and nitrate, if the test is performed under nitrifying conditions. (ii) Additional apparatus (A) 1-L sample bottles to hold test substance dosing solutions. (B) Silicone rubber tubing: Bore = 0.5 mm ID. (C) Polypropylene transmission tubing. (D) Tube connectors. (E) Diffuser stones. (F) 25-mL measuring cylinders. (G) 1-mL graduated pipets. 12 ------- (H) Stopwatch. (I) 40-mL sample bottles for collection of samples for waste sludge and mixed liquor suspended solids determinations. (J) Thermometer having range 0 to 50°C. (K) 1- and 2-1 measuring cylinders for each pot to collect waste sludge. (L) Timer for sludge wastage pump allowing intermittent operation, unless sludge is wasted manually. (M) Right-angled plastic tube to fit on one end of the air line to ensure complete mixing of activated sludge. (N) If porous pots are operated in the sealed mode, plastic tubing to fit on the pot effluent port as shown in Figure 3 to balance the back pressure caused by the CO2 traps. (8) Water, (i) Tap water should contain less than 3 mg DOC/1. Determine the alkalinity if it is not already known. (ii) Deionized water should contain less than 2 mg DOC/1. See also paragraph (d) of this guideline, on applicable ASTM standards. (9) Organic medium—(i) General. Synthetic sewage, domestic sewage or a mixture of both can be used as the organic medium. It has been shown (see paragraphs (p)(8) and (p)(ll) of this guideline) that the use of domestic sewage alone often gives increased percentage DOC removal and even allows the removal and biodegradation of some substances that are not biodegraded when synthetic sewage is used. Also, the constant or intermittent addition of domestic sewage often stabilizes the activated sludge, including the crucial ability to settle well. Thus, use of domestic sewage is recommended. Measure the DOC or COD concentration in each new batch of organic medium. The acidity or alkalinity of the organic medium should be known. The organic medium may require the addition of a suitable buffer (sodium hydrogen carbonate or potassium dihydrogen phosphate) if it is of low acidity or alkalinity, to maintain a pH of about 7.5 ± 0.5 in the aeration vessel during the test. The amount of buffer to be added, and when to add it, has to be decided in each individual case. When mixtures are used either continuously or intermittently, the DOC (or COD) of the mixture must be kept at an approximately constant value, e.g. by dilution with water. (ii) Synthetic sewage. Dissolve in each liter of tap water peptone, 160 mg; meat extract, 110 mg; urea, 30 mg; anhydrous dipotassium hydrogen phosphate (K2HPO4), 28 mg; sodium chloride (NaCl), 7 mg; calcium chloride dihydrate (CaQ2-2H2O), 4 mg; magnesium sulfate heptahydrate (Mg2SO4'7H20), 2 mg. This OECD synthetic sewage is an example and gives a mean DOC concentration in the influent of about 100 mg/1. Alternatively, use another composition, with about the same DOC concentration that is 13 ------- closer to real sewage. If a less-concentrated influent is required, dilute the synthetic sewage with tap water (for example 1:1) to obtain a concentration of about 50 mg/1. Such a weaker influent will allow better growth of nitrifying organisms and this modification should be used if the simulation of nitrifying wastewater plants is to be investigated. Synthetic sewage may be prepared with distilled water in a concentrated form and stored at about 1°C for up to one week. When needed, dilute with tap water. This medium is not entirely satisfactory, e.g. the nitrogen concentration is very high and carbon content relatively low, but nothing better has been suggested. Some investigators add more phosphate as buffer and extra peptone. (iii) Domestic sewage. Use fresh settled sewage collected daily from a wastewater treatment plant receiving predominantly domestic sewage. It should be collected, prior to primary sedimentation, from the overflow channel of the primary sedimentation tank, or from the feed to the activated sludge plant, and be largely free of coarse particles. The sewage can be used after storage for several days (but storage time generally should not exceed 7 d) at about 4°C, if it is first established that the DOC (or COD) has not significantly decreased (i.e. <20%) during storage. In order to limit disturbances to the system, the DOC (or COD) of each new batch should be adjusted before use to an appropriate constant value, e.g. by dilution with tap water. (iv) Activated sludge. Collect activated sludge for inoculation from the aeration tank of a well operated wastewater treatment plant or from a laboratory-scale activated sludge unit, treating predominantly domestic sewage. (10) Stock solutions of test substance, (i) For substances of adequate solubility, prepare stock solutions at appropriate concentrations (e.g. 1 to 5 g/1) in deionized water, or use synthetic sewage without the organic nutrient portion (e.g. peptone or meat extract). For insoluble and volatile substances, see paragraphs (f)(2) and (f)(3) of this guideline. Determine the DOC and total organic carbon (TOC) of the stock solution and repeat the measurements for each new batch. If the difference between the DOC and TOC is greater than 20%, check the water-solubility of the test substance. Compare the DOC or the concentration of the test substance measured by specific analysis of the stock solution with the nominal value, to ascertain whether recovery is good enough (normally >90% can be expected). Ascertain, especially for dispersions, whether DOC can be used as an analytical parameter or an analytical technique specific for the test substance is required. Centrifugation of the samples is required for dispersions. For each new batch, measure the DOC, COD or the test substance by specific analysis. (ii) Determine the pH of the stock solution. Extreme values indicate that the addition of the substance may have an influence on the pH of the activated sludge in the test system. In this case neutralize the stock solution to obtain a pH of 7 ± 0.5 using small amounts of inorganic acid or base, but avoid precipitation of the test substance. (11) Other reagents and materials, (i) Compressed air (filtered for oil and water) for aeration of porous pots. (ii) Extraction apparatus and solvent for hydrophobic test substances. 14 ------- (iii) Glycerol for lubricating the rollers of the peristaltic pumps. (iv) Sodium hypochlorite solution. (k) Safety precautions. (1) This procedure involves the use of mixed liquor and natural sewage from a domestic wastewater treatment plant. Consequently, individuals performing this test may be exposed to microbial agents that are dangerous to human health. It is recommended that test units be operated in a separate room and that exhaust air be vented outside the building. (2) Personnel who work with sewage organisms may choose to keep current with pertinent immunizations such as typhoid, polio, hepatitis B, and tetanus. (3) Effluent from activated sludge units should be treated with a chemical disinfectant (chlorine bleach, 5%) or autoclaved prior to disposal. Safety glasses and protective gloves should be worn when using sodium hypochlorite to clean porous pot liners. (4) Unless shown to be nontoxic, all test substances should be treated as potentially harmful. (1) Procedure—(1) Preparation of the inoculum, (i) Inoculate the test system at the beginning of the test with either activated sludge or an inoculum containing a low concentration of microorganisms. Keep the inoculum aerated at room temperature until it is used, and use it within 24 h. In the first case, take a sample of activated sludge from the aeration tank of an efficiently operated biological wastewater treatment plant, or a laboratory treatment plant, that receives predominantly domestic sewage. If nitrifying conditions are to be simulated, take sludge from a nitrifying wastewater treatment plant. Determine the concentration of suspended solids and, if necessary, concentrate the sludge by settling so that the volume added to the test system is minimal. Ensure that the starting concentration of dry matter is about 2.5 g/1. (ii) In the second case, use 2 ml/1 to 10 ml/1 of an effluent from a domestic biological wastewater treatment plant as inoculum. To maximize microbial diversity, it may be helpful to add inocula from various other sources, for example surface water. In this case, the activated sludge will develop and grow in the test system. (2) Husmann unit procedure—(i) Dosage of organic medium. (A) Ensure that influent and effluent containers and tubing between influent and effluent vessels are thoroughly cleaned, to remove microbial growth initially and for the duration of the test. Assemble the test systems in a room where the temperature is controlled (normally in the range 20-25°C) or use water-jacketed test units. Prepare a sufficient volume of the required organic medium (see paragraph (j)(9) of this guideline). Initially fill the aeration vessel and the separator with the organic medium, then add the inoculum. Start the aeration such that the sludge is kept in suspension and in an aerobic state, and begin dosing the influent and recycling the settled sludge. Dose organic medium from storage vessels into the aeration 15 ------- vessels of the test and control units, and collect the respective effluents in similar storage vessels. To get the normal HRT of 6 h, the organic medium is pumped at 0.5 1/h. To confirm this rate, measure the daily amount of organic medium dosed by noting the reduction in volumes of the medium in the storage vessels. The dosing mode may need to be modified if, for example, the study objective is to determine the effects of intermittent release or shock loading of substances. (B) If the organic medium is prepared for use for a period >1 d, it should be cooled to about 4°C, or another appropriate method should be used to prevent microbial growth and biodegradation outside the test units. If synthetic sewage is used, it is possible to prepare, and store at about 4°C, a concentrated stock solution (e.g. lOx the normal concentration. This stock solution can be mixed with the appropriate volume of tap water immediately before use. Alternatively, it can be pumped directly while the appropriate amount of tap water is pumped separately. (ii) Dosage of test substance. (A) Add an appropriate volume of the stock solution of test substance to the storage vessel of the influent, or dose it directly with a separate pump into the aeration vessel. The normal mean test substance concentration in the influent should be between 10 and 20 mg/1 as DOC, with an upper concentration of no more than 50 mg/1. If the water solubility of the test substance is low (see paragraph (e)(2) of this guideline) or if toxic effects are considered likely (see paragraph (e)(4) of this guideline), reduce the concentration to 5 mg/1 as DOC or even less, but only if a suitable specific analytical method for test substance is available. Dispersed test substances that are poorly soluble in water may be added using special dosing techniques: see paragraph (e)(2) of this guideline. (B) Start adding the test substance after a period in which the system has stabilized and is removing DOC of the organic medium efficiently (i.e. by about 80%). It is important to check that all units are working equally efficiently before the addition of test substance; if they are not, it usually helps to mix the individual sludges and to re-dispense equal volumes to individual units. When an inoculum of (about) 2.5 g/1 (dry weight) activated sludge is used, the test substance may be added from the start of the test since directly adding increasing amounts from the beginning has the advantage that the activated sludge may be better able to adapt to the test substance. However test substance is added, it is recommended that the relevant flow rate and/or the volumes in the storage vessel(s) be measured at regular intervals. (iii) Handling of activated sludge. (A) The concentration of activated sludge solids normally stabilizes between limits during the test, independent of the inoculum used, in the range of 1 to 3 g/1 (dry weight) depending on the quality and concentration of the organic medium, operating conditions, the nature of the microorganisms present and the influence of the test substance. (B) Either determine the suspended solids in the aeration vessels at least weekly and discard surplus sludge to maintain the concentration at 1 g/1 to 3 g/1 (dry weight), or control the mean SRT at a constant value usually in the range 6 days to 10 days. If, for example, a sludge retention time of 8 days is selected, remove daily 1/8 of the volume of the activated 16 ------- sludge in the aeration vessel and discard it. Perform this action on a daily basis or, preferably, by means of an automatic intermittently operating pump. Maintaining the concentration of suspended solids at a constant level, or within narrow limits, does not ensure a constant SRT, which is the operating variable that determines the value of the concentration of test substance in the effluent. (C) Throughout the test, remove, at least daily, any sludge adhering to the walls of the aeration vessel and the separator so that it is resuspended. Check and clean regularly all tubes and tubing to prevent growth of biofilm. Recycle the settled sludge from the separator to the aeration vessel, preferably by intermittent pumping. (D) Poor settling and loss of sludge may occur in the Husmann units. These may be rectified by employing one or more of the actions listed in paragraphs (l)(2)(iii)(D)(7) through (l)(2)(iii)(D)(<5) of this guideline for both test and control units: (1) Fresh sludge or a flocculant (for example 2 ml/vessel of 50 g/1 Feds) can be added at regular intervals, e.g. weekly, but ascertain that no reaction or precipitation of the test substance occurs with (2) The air-lift pump can be replaced by a peristaltic pump, thus enabling a sludge recirculation flow that equals the influent flow to be used and allows development of an anaerobic zone in the settled sludge. The geometry of the air-lift pump limits the minimum flow rate of returned sludge to be about 12x that of the influent; (3) Sludge can be pumped intermittently from the separator to the aeration vessel (e.g. 5 min every 2.5 h to recycle 1 1/h to 1.5 1/h); (4) A nontoxic anti-foaming agent (e.g. silicone oil) at minimal concentration can be used to prevent loss by foaming; (5) Air can be passed through the sludge in the separator in short, shock bursts (e.g. 10 sec every hour); (6) The organic medium may be dosed at intervals into the aeration vessel (e.g. for 3 min to 10 min every hour). (3) Porous pot procedure, (i) Set up the number of pots required by the study plan. Each test should have at least one control pot (pot fed settled sewage and benzoate or other easily degradable reference substance) and it is recommended (but not required) that each test substance be tested in duplicate. (ii) Fill the aeration vessel with activated sludge to the level of the effluent overflow. The volume required is 3.8 1 for a typical porous pot (see Figure 3). The initial MLVSS should be 1.5 to 3.0 g/L, and this level should be maintained throughout the test. This may necessitate supplementation of the feed with synthetic sewage. (iii) Start the aeration and set the air flow. The air flow should be sufficient to 17 ------- maintain and thoroughly mix the solids in suspension and keep the concentration of DO above 2 mg/L at all times. In order to do this it is necessary to maintain an air to influent flow ratio of 5 to 10/1 on a volume basis. (iv) Place 1 1 of test/reference substance dosing solution in the dosing vessel. (v) Start the dosing pumps, lubricating the tubes with a small amount of glycerol. (vi) Start the sludge wastage pump at the rate required to give the desired SRT. The SRT (in days) is equal to the pot volume (1) divided by the sludge wastage rate (1/d). Alternatively, sludge may be wasted manually by periodically discarding the required volume. (vii) Set the sewage dosing rate to give the required HRT and the test/reference substance dosing rate at about 0.5 ± 0.05 ml/min. (viii) Daily measurements of sewage flow rates should be made using a 25-ml measuring buret and a stopwatch. The flow rates should be adjusted to within ± 0.05 mL/min of the required flow. (ix) Dosing solution flow rates should be calculated from measuring the volume left after 24 h of dosing. (x) The dosing rates should be recorded and corrected to the nominal value given in the study plan. The sewage flow should be adjusted if the measured flow differs by more than 0.5 ml/min from the nominal value. (xi) Sludge that gathers around the rim of the porous liner should be returned to the mixed liquor at least once per day by scraping with a large spatula. This should always be done before taking a sample of mixed liquor for MLVSS determination. (xii) The temperature, pH and DOC of the mixed liquor should be measured at least every other day. (xiii) Periodically remove a 40-ml sample of mixed liquor from the aeration vessel for MLVSS determination. Three times weekly is usually sufficient. (xiv) The volume of mixed liquor wasted from the porous pot should be measured and recorded daily. Remove a representative 40-ml sample from the sludge wastage bottle at least once per week and determine the MLVSS level. (xv) The porous pot liner should be changed at the first sign of blocking of the pores; i.e., when the mixed liquor rises above the effluent overflow. To change the liner, proceed as explained in this paragraph: siphon the mixed liquor into a suitable container and remove any solids from the inner surface of the outer vessel. Place a fresh liner in the outer vessel. Return the mixed liquor to the aeration vessel. Scrape off and transfer any sludge adhering to the sides of the blocked liner. The blocked liner should be thoroughly 18 ------- cleaned before reuse by immersion in a 20 percent solution of hypochlorite bleach for several hours. The liners should be thoroughly rinsed in clean tap and the deionized water before reuse. (xvi) Sewage and effluent samples should be taken twice weekly during the stabilization ("running-in") period for organic carbon analysis and specific compound analysis if required. If necessary, ammoniacal nitrogen, nitrate, nitrite, COD and 5-d BOD may also be determined. (xvii) When the pots have attained steady-state conditions, the effluents are analyzed periodically to determine the extent of biodegradation/removal of the test substance during treatment. (xviii) If information on the effects of various operating conditions on removal is required, e.g., temperature, SRT, HRT, etc., any changes should be made gradually. Operate the pot for a period of at least three SRT under the new conditions before collecting data to determine the effect of the new condition(s). (4) Sampling and analysis, (i) At regular intervals measure the DO concentration, temperature and pH of the activated sludge in the aeration vessels. Ensure that sufficient oxygen is always available (>2 mg/1) and that the temperature is kept in the required range (normally 20°C to 25°C). Keep the pH at 7.5 ± 0.5 by dosing small amounts of inorganic base or acid into the aeration vessel or into the influent, or by increasing the buffering capacity of the organic medium (see paragraph (j)(9)(i) of this guideline). When nitrification occurs acid is produced, the oxidation of 1 mg N producing the equivalent of about 7 mg COs"2. The frequency of measurement depends on the parameter to be measured and the stability of the system, and may vary between daily and weekly. (ii) Measure the DOC or COD in the influents to the control and test vessels. Measure the test substance concentration in the influent by specific analysis, or estimate it from the concentration in the stock solution (see paragraph (j)(10)(i) of this guideline), the volume used and the amount of sewage dosed into the test unit. It is recommended that the concentration of the test substance be calculated in order to reduce the variability of the concentration data. (iii) Take suitable samples from the collected effluent (e.g. 24-h composites) and filter through a membrane of pore size 0.45 jim, or centrifuge them at 40,000 m/s2 for 15 min. Centrifuging should be used if filtering is difficult. Determine DOC or COD at least in duplicate to measure ultimate biodegradation and, if required, primary biodegradation by an analysis method specific for the test substance. (iv) The use of COD may give rise to analytical problems at low concentrations and is therefore recommended only if a sufficiently high test concentration (about 30 mg/1) is used. Also, for strongly adsorbing substances, it is recommended that the amount of adsorbed substance in the sludge be measured using an analytical technique specific for the test substance. 19 ------- (v) The frequency of sampling depends on the expected duration of the test. A recommended frequency is three times per week. Once the units are operating efficiently, allow from 1 week to a maximum of 6 weeks after the test substance has been introduced, for adaptation to reach steady state. Preferably obtain at least 15 valid measurements during the plateau phase (see paragraph (m)(2)(iv) of this guideline), which normally lasts 3 weeks, for the proper evaluation of the test substance. The test may be terminated if a sufficient degree of elimination is reached (e.g. >90%) and these 15 values, which represent analyses carried out each weekday over 3 weeks, are available. Normally, the test duration should not exceed 12 weeks after addition of the test substance. (vi) If the sludge nitrifies and the effects of the test substance on nitrification are to be studied, analyze samples from the effluent of the test and control units at least once per week for ammonium and/or nitrite plus nitrate. (vii) All analyses, but especially the nitrogen determinations, should be performed as soon as possible. If analyses have to be postponed, store the samples at about 4°C in the dark in full, tightly closed bottles. If samples have to be stored for more than 48 h, preserve them by freezing, acidification (e.g. 10 ml/1 of a 400 g/1 solution of sulfuric acid), or addition of a suitable preservative (e.g. 20 ml/1 of a 10 g/1 solution of mercury(II) chloride). Ensure that the preservation technique does not influence results of analysis. (5) Coupling of test units, (i) If coupling is to be used, exchange daily the same amount of activated sludge (150 ml to 1500 ml for aeration vessels containing 3 1 of liquor) between the aeration vessels of the test unit and its control unit. If the test substance adsorbs strongly onto the sludge, change only the supernatant of the separators. In both cases use a correction factor to calculate the test results. (ii) In order to try to equalize the microbial populations in sludges in a test unit receiving organic medium plus a test substance, and in a control unit, receiving only organic medium, a daily interchange of sludge was introduced (see paragraph (p)(24) of this guideline). The procedure was called coupling and the method is referred to as the Coupled Units Test. Coupling was initially performed using Husmann activated sludge units but it has also been done with porous pot units (see paragraphs (p)(3) and (p)(8) of this guideline). No significant differences in results were found between noncoupled and coupled units, whether Husmann or porous pot, suggesting that there is no advantage in expending the time and energy needed in coupling the test units. (iii) Sludge exchanges can give the appearance of considerable removal, since some of the test substance in transferred and the concentrations of test substance in the test and control effluents become more nearly equal. Thus, correction factors have to be used which depend on the fraction exchanged and the mean HRT. More details of the calculation have been published (see paragraph (p)(24) of this guideline). (iv) Calculate the corrected DOC or COD elimination percentage using the formula in this paragraph: Dtc = (Dt- 100-a-r/12)/(l-a-r/12) 20 ------- where Dtc = corrected % DOC or COD elimination Dt = determined % DOC or COD elimination a = interchange fraction of the volume of the activated sludge units r = mean HRT (h) If, for example, half of the volume of the aeration tank is exchanged (a = 0.5) and the mean HRT is 6h, the correction formula is: Dtc = 4Dt- 100 3 (m) Data and reporting—(1) Treatment of results, (i) Calculate the percentage of DOC or COD elimination of the test substance for each time using the equation Dt = G. - (E -En) x 100 Cs where Dt = % elimination of DOC or COD at time t Ct = DOC or COD in the influent due to the test substance, preferably estimated from the stock solution (mg/1) E = measured DOC or COD value in the test effluent at time t (mg/1) E0 = measured DOC or COD value in the control effluent at time t (mg/1) (ii) The degree of DOC or COD elimination of the organic medium in the control unit is helpful information in assessing the activity of the activated sludge during the test. Calculate the percentage elimination from the equation DB = CM-En x 100 CM where DB = % elimination of DOC or COD of the organic medium in the control unit at time t CM = DOC or COD of the organic medium in the control influent (mg/1) Optionally, calculate the percentage elimination DOC or COD due to the organic medium plus test substance in the test unit from the equation DT = CT-E x 100 CT where DT = % elimination of total test influent DOC or COD CT = DOC or COD of total test influent or calculated from stock solutions (mg/1) (iii) Calculate the removal of the test substance if measured with a specific analytical method at each time assessment from the equation 21 ------- DST = Si-Se x 100 Si where DST = % primary elimination of test substance at time t S; = measured or estimated test substance concentration in the test influent (mg/1) Se = measured test substance concentration in test effluent at time t (mg/1) (iv) If the coupling mode has been used, compensate for the dilution of the test substance in the aeration vessel by the sludge exchange using a correction factor (see paragraph (l)(5)(iv) of this guideline). (2) Expression of test results—(i) Elimination curve. Plot the percentage elimination Dt (or Dtc) and Dst, if available, vs. time (see Figure 4). From the shape of the elimination curve of the test substance (as parent or as DOC), conclusions may be drawn about the removal process. Figure 4. Example of an elimination curve Polyethylene glycol 400 Test Concentration 20 mg/1 as DOC 120 0 0 10 15 20 Time (Day) 25 30 (ii) Adsorption. If high DOC elimination for the test substance is observed from the beginning of the test, the test substance is probably eliminated by adsorption onto the activated sludge solids. It is possible to prove this by determining the adsorbed test substance by specific analysis. It is not usual for the elimination of DOC of adsorbable substances to remain high throughout the test; normally, removal is high initially but 22 ------- gradually falls to a lower, equilibrium value. However, acclimation can occur over time, possibly encouraged by the sorption to sludge, such that removal could remain or increase to a high level by the end of the measurement period, and reflect some combination of sorption and biodegradation. (iii) Lag phase. As in static screening tests, many test substances exhibit a lag phase before biodegradation becomes evident. In the lag phase, acclimation or adaptation of the degrading bacteria takes place with little or no evident removal of the test substance. As growth of bacteria at the expense of the test substance occurs, its biodegradation becomes measurable. Normally, the lag phase is considered to end and the degradation phase begins when 10% of the initial amount of test substance is removed (after allowing for adsorption, if it occurs). This value is somewhat arbitrary but has become common practice. The lag phase is often highly variable and poorly reproducible. (iv) Plateau phase. The plateau phase of an elimination curve in a continuous test is defined as that phase in which the maximum degradation takes place. The plateau phase should last at least 3 weeks and have at least 15 measured removal values. (v) Mean degree of elimination of test substance. Calculate the mean value from the elimination values (Dt) of the test substance at the plateau phase. Rounded to the nearest whole number, it is the degree of elimination of the test substance. It is also recommended to calculate the 95% confidence interval of the mean value. (vi) Elimination of organic medium. Plot the elimination percentage of the DOC or COD of the organic medium in the control unit (DB) vs. time. Indicate the mean degree of elimination in the same way as for the test substance. (vii) Indication of biodegradation. If the test substance does not sorb significantly to activated sludge and the elimination vs. time curve has the typical shape of a biodegradation curve with lag period, then increasing percentage degradation and finally the plateau phase, the measured elimination can safely be attributed to biodegradation. If a high initial removal is observed, this test cannot differentiate between biological and abiotic elimination processes. In such cases, and in other cases where there is any doubt about biodegradation (e.g. if stripping takes place), analyze adsorbed test substances or perform additional static biodegradation tests based on parameters clearly indicative of biological processes. Such tests are the oxygen uptake methods (OECD 301C, 301D and 301F) or a test with measurement of carbon dioxide production (301B or 310), using a pre-exposed inoculum from the simulation test. If both DOC removal and specific substance removal have been measured, significant differences between the percentages removed (the former being lower than the latter) indicate the presence in the effluents of intermediate organic products, which may be more difficult to degrade than the parent substance. (3) Validity of test results, (i) Information on the normal biodegradation behavior of the inoculum is obtained from the degree of elimination of the organic medium in the control unit (see paragraph (m)(l)(ii) of this guideline). Consider the test to be valid if the degree of DOC or COD elimination in the control unit is >80% after two weeks and no 23 ------- unusual observations have been made. (ii) If a readily biodegradable (reference) substance has been used, the degree of biodegradation (Dt) should be >90%. (iii) If the test is performed under nitrifying conditions, the mean concentration in the effluents should be <1 mg/1 for ammonia-N and <2 mg/1 nitrite-N. (iv) If these criteria are not met, repeat the test using an inoculum from a different source, include a reference substance, and review all experimental procedures. (4) Quality assurance. To assure the integrity of data developed using this method and to comply with current regulatory requirements, a quality assurance program meeting EPA, FDA, or OECD guidelines should be followed. This may require replicates (three or more) to be run for good laboratory practice (GLP) compliance and assessment of variability. (5) Test report. The test report should include the information in paragraphs (m)(5)(i) through (m)(5)(iii) of this guideline: (i) Test substance (A) Identification data; (B) Physical state and, where relevant, physical/chemical properties. (ii) Test conditions (A) Type of test system; and any modifications for testing insoluble or volatile substances; (B) Type of organic medium; (C) Proportion and nature of industrial wastewaters in sewage, if known; (D) Inoculum, nature and sampling site(s), concentration and any pre-treatment; (E) Test substance stock solution: DOC and TOC content; how prepared, if a suspension; test concentration used; reasons if outside range of 10-20 mg DOC/1; method of addition; date first added; any changes; (F) Mean SRT and mean HRT; method of sludge wastage; methods of overcoming bulking, loss of sludge, etc.; (G) Analytical techniques employed; (H) Test temperature; 24 ------- (I) Sludge qualities: MLVSS, sludge volume index (SVI), bulking (if observed); (J) Any deviations from standard procedures and any circumstances that may have affected results. (iii) Test results (A) All measured data, including DOC, COD, specific analyses, pH, temperature, oxygen concentration, suspended solids, N compounds, as appropriate; (B) All calculated values of Dt (or Dtc), DB, DSt, in tabular form and as elimination curves; (C) Information on lag and plateau phases, test duration, degree of elimination of the test substance and reference substance (if included) and that of the organic medium in the control unit, together with statistical data and statements on biodegradability and validity of the test; (D) Discussion of results. (n) Tests At low (ug/1) concentration range—(1) Background. Many substances are normally present in the aquatic environment, even in wastewaters, at very low concentrations (ng/1). At such concentrations, they probably do not serve as primary substrates resulting in growth, but are more likely to degrade as nongrowth, secondary substrates, concurrent with a variety of naturally occurring carbon compounds. Consequently the degradation of such substances will not fit kinetics models for substrates that support growth (see paragraph (o) of this guideline). There are many models that could be applied and, under the conditions prevailing in wastewater treatment systems, more than one may be operative at a given time. (2) Procedure. Until research sheds more light on kinetics of biodegradation at low substrate concentrations in activated sludge treatment, the procedure given in the main text (see paragraph (1) of this guideline) can be followed, but only for primary biodegradability, using suitably low test substance concentrations (<100 |ig/l) and a validated analytical procedure. The percentage biodegradation may be calculated provided that abiotic processes (adsorption, volatility, etc.) are taken into account. Examples can be found in the studies cited in paragraphs (p)(25) and (p)(26) of this guideline, which used a fill-and-draw system with 4-h cycle. These studies reported pseudo first-order biodegradation rate constants for 5 substances in synthetic sewage initially at 5-100 |ig/l. For ultimate biodegradability, 14C-labeled test substance may be used. A description of this is beyond the scope of this guideline since there are as yet no agreed procedures, although a proposed method for ISO standard 14592 (see paragraph (p)(27) of this guideline) contains guidance on the use of 14C-labelled substances. (3) Two-stage test—(i) General. More recently a simpler two-stage test was proposed (see paragraphs (p)(28), (p)(29) and (p)(30) of this guideline), and is described below in paragraphs (n)(3)(ii) through (n)(3)(iv). In it, a semi-continuous activated sludge 25 ------- (SCAS) test is followed by short-term kinetic tests on samples withdrawn from the SCAS units. (ii) SCAS test. (A) The SCAS system is operated with known sludge wastage rates and is fed a modified OECD synthetic sewage or domestic sewage. The synthetic sewage was modified (because of changing pH value and poor sludge settleability) by addition of phosphate as buffer, yeast extract, iron (III) chloride and trace element salts, and its COD was increased to about 750 mg/1 by increasing the concentration of peptone and meat extract. The units are operated on a 24-h cycle: aeration for 23 h, wastage of sludge, settlement, and withdrawal of supernatant (effluent), followed by addition of synthetic sewage plus test substance at up to 100 jig/1. Once per week 10% of the total sludge is replaced by fresh sludge in order to maintain a balanced microbial population. (B) The concentrations of test substance initially and at the end of aeration are measured and the test is continued until a constant removal of test substance is attained; this takes from one week to several months. (iii) Short-term test. A short test (e.g. 8 hours) is applied to determine the (pseudo) first-order kinetic rate constant for the decay of the test substance in activated sludges of known but different origins and histories. In particular, sludge samples are taken from the SCAS reactors - at the end of an aeration period when the concentration of organic substrate is low - during the course of an acclimatization experiment (see paragraph (n)(3)(ii) of this guideline). Sludge may also be taken from a parallel SCAS unit not exposed to the test substance, for comparison. Mixtures of sludge and the test substance added at two or more test substance concentrations in the range 1-50 jig/1 are aerated, without the addition of synthetic sewage or other organic substrate. Test substance remaining in solution is determined at regular intervals, e.g. hourly, depending on the degradability of the substance, for a period not longer than 24 h. Samples are centrifuged before analysis. (iv) Calculations. (A) Data from the SCAS units are used to calculate the percentage removal of test substance (see paragraph (m)(l)(iii) of this guideline). Also, an average rate constant KI, normalized for concentration of suspended solids, can be calculated as shown in this paragraph: KI = 1/t • In (Ce / CO • 1/SS (1/g h) where t = aeration time (23 h) Ce = concentration at end of aeration period (|ig/l) C; = concentration at beginning of aeration (|ig/l) SS = concentration of activated sludge solids (jig/1) (B) In the short term test the log (% concentration remaining) is plotted against time and the slope of the initial part of the plot (i.e. at 10-50% degradation) is equivalent to KI, the (pseudo) first-order rate constant. The constant is normalized with respect to the concentration of sludge solids by dividing by the concentration of sludge solids. As reported, test results should also include details of initial concentrations of the test 26 ------- substance and suspended solids, sludge retention time, sludge loading and source, and details of pre-exposure (if any) to the test substance. (4) Variability of results. Variability and other facets of biodegradation kinetics were discussed at a 1996 workshop (see paragraph (p)(31) of this guideline). From such studies, reported and projected, a clearer view of kinetics operating in wastewater treatment plants should be forthcoming, to enable a better interpretation of existing data as well as suggest more relevant designs for future test guidelines. (o) Effects of SRT on treatability of substances—(1) Background. The method described in the main text (paragraphs (a) through (1) of this guideline) was designed to ascertain whether the substances tested (usually those known to be inherently but not readily biodegradable) can be biodegraded within the limits imposed in typical wastewater treatment plants. The results are expressed in terms of percentage removal and percentage biodegradation. The conditions of operation of the activated sludge units and choice of influent allow rather wide variations in concentration of the test substance in the effluent. Normally tests are performed at only one nominal concentration of sludge solids or one nominal SRT, and the sludge wastage regimes described can cause the value of SRT to vary considerably during the test, both from day to day and during a day. (2) General. In this variant (see paragraphs (p)(10) and (p)(ll) of this guideline) the SRT is controlled within much narrower limits throughout each 24-h period, as happens in full-scale treatment plants, which results in a more constant test substance concentration in effluents. Domestic sewage is recommended since it gives more consistent and higher percentage removals. Also, the effects of varying the SRT are investigated, and in a more detailed study, the effects of a range of temperature on effluent concentration may be determined. (3) Kinetic models. There is no general agreement yet on which kinetic models operate when substances biodegrade in wastewater treatment. The Monod model of bacterial growth and substrate utilization was selected for application here, since the method was intended for application only to substances produced in high tonnages, resulting in concentrations in sewage of above 1 mg/1. The validity of the simplified model and the assumptions made was established using a series of alcohol ethoxylates having varying degrees of primary biodegradability (see paragraphs (p)(ll) and (p)(32) of this guideline). (4) Principle of the test, (i) This variant method follows closely much of the text in paragraphs (a) through (1) of this guideline and only those details that differ are given hereafter. (ii) Activated sludge porous pot units, designed to facilitate the nearly continuous wastage of mixed liquor allowing very precise control of the SRT, are operated in the non- coupled mode over a range of SRT and, optionally, over a range of temperature. The retention time is usually 2 to 10 d and the temperature between 5 and 20°C. Sewage, preferably domestic, and a solution of the test substance, are dosed separately to the units at rates to give the required sewage retention time (3 to 6 h) and the required concentration of 27 ------- test substance in the influent. Control units receiving no test substance are operated in parallel for comparative purposes. (iii) Other types of apparatus can be used but great care should be exercised to ensure that good control of SRT is achieved. For example, when using a model test system that incorporates a settler, allowance for loss of solids via the effluent may be necessary. Further, special precautions to avoid errors due to variation in the quantity of sludge in the settler should also be taken. (iv) The units are operated at each selected set of conditions and, after steady state has been reached, the average steady-state concentrations in the effluents of test substance and, optionally, DOC, are obtained over a period of about three weeks. Besides assessing the percentage removal of test substance and, optionally, DOC, the relationship between operating conditions and the test substance concentration in the effluent is expressed in graphical form. From this, tentative kinetic constants may be calculated and the conditions under which the test substance can be treated may be predicted. (5) Apparatus, (i) A suitable unit is the modified porous pot system (see Figure 5). It consists of an inner vessel (or liner) constructed from porous polypropylene of 3.2 mm thickness and pore size of approximately 90 jim, the joint being butt-welded. This makes a more robust unit than the one shown in Figure 3 (see also paragraph (j)(3)(i) of this guideline). The liner is fitted into an impervious polyethylene outer vessel, which consists of two parts: a circular base in which holes are bored to accommodate two air lines and a sludge wastage line, and an upper cylinder that screws onto the base and that has an outlet placed so as to give a known volume (3 1) in the porous pot vessel. One of the air lines is fitted with a diffuser stone and the other is open-ended and set at right angle to the stone in the pot. This system produces the necessary turbulence to ensure that the contents of the pot are completely mixed, as well as providing concentrations of DO >2 mg/1. (ii) The appropriate number of units are maintained at controlled temperatures in the range of 5 to 20°C (+/- 1°C), either in a water bath or in a constant-temperature room. Pumps are required to dose to the aeration vessels the solution of test substance and settled sewage at the required rates (0-1.0 ml/min and 0-25 ml/min, respectively), as well as a third pump to remove waste sludge from the aeration vessels. The necessary very low flow rate of waste sludge is achieved by using a pump set at a higher rate and operated intermittently by the use of a timer switch, e.g. operating for 10 seconds per min, with a pump delivery rate of 3ml/min yielding a wastage rate of 0.5 ml/min. (6) Inoculum. Paragraph (l)(l)(i) of this guideline applies, but use only activated sludge at about 2.5 g/1. (7) Number of test units. For a simple test, i.e. to measure percentage removal, only a single SRT is required, but in order to acquire data necessary to calculate tentative kinetic constants, data for 4 or 5 SRT values are required. Values between 2 and 10 days are usually chosen. Practically, it is convenient to perform a test at 4 or 5 SRT values simultaneously at one temperature. In extended studies the same SRT values, or perhaps a different range of values, are used at other temperatures within the range 5 to 20°C. For 28 ------- primary biodegradation (the main use), only one test unit per set of conditions is normally required. However, for ultimate biodegradability a control unit is required, for each set of conditions, which receives sewage but not test substance. If the test substance is thought to be present in the sewage used in the test, it is necessary to use control units when assessing primary biodegradation, and to make the necessary correction in the calculations. (8) Dosage of organic medium and test substance. Paragraphs (l)(2)(i) and (l)(2)(ii) of this guideline apply generally, but note that the test substance solution is dosed separately and that various sludge wastage rates are used. Also, frequently (e.g. twice per day) monitor and adjust to within +/- 10%, if necessary, the flow rates of influent, effluent and sludge wastage. If difficulties are encountered in the analytical methods when domestic sewage is used, perform the test with synthetic sewage, but it must be assured that different media give comparable kinetic data. (9) Handling of activated sludge units. Paragraph (l)(2)(iii) of this guideline applies generally, but control SRT only by constant wastage of sludge. (10) Sampling and analysis. Paragraph (1)(4) of this guideline applies generally, except that the concentration of the test substance should be determined and DOC determined optionally; also, COD should not be used. (11) Calculation of kinetic constants—(i) It is more realistic to quote the mean steady-state concentration of the test substance in the effluent and to describe how this varies with operating conditions than to quote percentage removal due to primary biodegradation. This can be done by consideration of Equation [6] of this guideline, which can yield values for KS, |im and ©sc, the critical sludge retention time. (ii) Alternatively, approximate values of Ks and m may be obtained using a simple computer program to fit the theoretical curve calculated from Equation [2] of this guideline to the experimental values obtained. Although any given solution will not be unique, a reasonable approximation of Ks and |imcan be obtained. (iii) By assuming Monod kinetics apply and considering a mass balance of active solids and substrate across the activated sludge system (see paragraph (p)(10) of this guideline), the steady state expressions shown in this paragraph can be obtained: J_ = [% • S^ - Kd Equation [1] ©s Ks + Si Si = Ks-Q +KH-Q.) Equation [2] 0~ • (|im - Kd) -~1 where Si = concentration of substrate in effluent (mg/1) Ks = half-saturation constant, the concentration at which |i = |im/2 (mg/1) |i = specific growth rate (d"1) |im = maximum value of m (d"1) Kd = specific decay rate of active solids (d"1) 29 ------- 0s = mean SRT (d) Examination of this equation leads to the conclusions in paragraphs (o)(ll)(iii)(A) through (A) The effluent concentration is independent of that in the influent (S0); hence, the percentage biodegradation varies with the influent concentration, S0. (B) The only plant-control parameter affecting Si is the sludge retention time, S. (C) For a given concentration in the influent, S0, there will be a critical sludge retention time, such that: J_ = j±s_l_So_ - Kd Equation [3] 0SC KS + So where 0SC = critical sludge retention time, below which the competent microorganisms will be washed out of the plant. (D) Since the other parameters in equation [2] are associated with growth kinetics, temperature is likely to affect the effluent substrate level and the critical SRT, i.e. the sludge retention time needed to obtain a certain degree of treatment, will increase with decreasing temperature. (iv) From a mass balance of solids in the porous pot system, and assuming that the solids concentration in the plant effluent, X2, is low compared with that in the aeration vessel, Xi, 0S = V-Xi _ Equation [4] (Qo - Qi) • X2 + Qi • Xi and 0S = v-x, = V Qi • Xi Qi where 0s = mean SRT (d) V = volume of the aeration vessel (1) Xi = concentration of solids in aeration vessel (mg/1) X2 = concentration of solids in effluent (mg/1) Qo = fl ow rate of influent (1/d) Qi = flow rate of waste sludge (1/d) Thus, it is possible to control the sludge retention time at any preselected value by the control of the waste sludge flow rate, Qi. (v) The main purpose of the test is thus to allow the effluent concentration, and hence the levels of test substance in the receiving waters, to be estimated. By plotting Si, 30 ------- vs. 0s, the critical sludge retention time, 0sc, can sometimes be readily evaluated; e.g. curve 3 in Figure 6. When this is not possible, 0sc may be calculated, together with approximate values of |im and Ks, by plotting Si, vs. Si -0s. Rearrangement of equation (1) gives 0s = K£ + Si 0S • Kd Hm Hm Equation [5] If Kd is small, then 1 + 0S 1 and [5] becomes Si • 0S = Kj, + Si Urn Urn Equation [6] Thus, the plot should be a straight line (see Figure 7) of slope l/|im and intercept Ks/|im; also 0S ~l/Hm- Figure 5. Modified porous pot for SRT control Test substance Influent Plastic outer vessel Porous polypropylene liner Seal Screw thread Solid plastic base Diffuse? stone rzu Effluent Jr supply Water sludge 31 ------- Figure 6. Effluent concentration vs. SRT for three temperatures and five SRT values CURVE3:5°C CURVE 2: 10°C CURVE 1: 15°C .^ 0 4 6 SRT - Days 32 ------- Figure 7. Regression line for SRT • Si vs Si at T= 5° C 30 — 25^ U3 2°- H * Wi *z ij ? d> S io- cs O O 1 5- S §* 0 x X'" MMax: 0.3 Ks; 1 / xx" x"k m l ' 1 1 1 02468 1 Effluent concentration (81) (mg/l) 33 ------- (12) Variability of results, (i) It is common experience that variable values of kinetic parameters for individual substances are obtained. It is thought that the conditions under which the sludge has been grown, as well as the conditions prevailing in the type of test system used (e.g. see paragraph (o)(4)(iii) of this guideline), have a large effect on the resulting values. One aspect of this variability has been discussed by Grady et al. (see paragraph (p)(33) of this guideline), who have suggested that the terms extant and intrinsic should be applied to two extreme conditions representing the limits of physiological state that a culture may attain during a kinetics experiment. If this physiological state is not allowed to change during the test, the kinetic parameter values reflect the conditions in the environment from which the microorganisms were taken; these values are called extant or currently existing. At the other extreme, if conditions in the test are such as to permit the full development of the protein synthesizing system allowing the maximum possible growth rate, the kinetic parameters obtained are said to be intrinsic, and are dependent only on the nature of the substrate and the types of bacteria in the culture. As a guide, extant values will be obtained by keeping the ratio of concentration of substrate to competent microorganisms (S0/X0) low, e.g. 0.025, and intrinsic values arise when the ratio is high, e.g. at least 20. In both cases, S0 should equal or exceed the relevant value of Ks, the half- saturation constant. (ii) Variability and other facets of biodegradation kinetics were discussed at a 1996 workshop (see paragraph (p)(31) of this guideline). From such studies, reported and projected, a clearer view of kinetics that apply in wastewater treatment plants should eventually be forthcoming. This will enable a better interpretation of existing data, as well as suggest more relevant designs for future test guidelines. (p) References. (1) Swisher, R. D. (1987). Surfactant biodegradation, 2nd ed. Marcel Dekker, New York, NY. 1085pp. (2) German Government (1962). Ordinance of the degradability of detergents in washing and cleaning agents. Bundesgesetzblatt, Pt.l, No. 49:698-706. (3) Painter, H. A. and E.F. King (1978). WRC porous pot method for assessing biodegradability. Technical Report No. 70, Water Research Centre, Medmenham, UK. (4) Painter, H. A. and E.F. King (1978). The effect of phosphate and temperature on growth of activated sludge and on biodegradation of surfactants. Wat. Res. 12, 909-915. (5) Eckenfelder, Jr., W.W. and R.R. Cardenas, Jr. (1966). Scale-up from laboratory activated sludge and trickling filter units to prototype design. Biotechnol. Bioengr. 8, 389- 404. (6) Gerike, P. and W.K. Fischer (1979). A correlation study of biodegradability determinations with various chemicals in various tests. Ecotox. Environ. Saf 3, 157-173. (7) Gerike, P. and W.K. Fischer (1981). A correlation study of biodegradability 34 ------- determinations with various chemicals in various tests. II. Additional results and conclusions. Ecotox. Environ. Saf. 5, 45-55. (8) Painter, H. A. and D. Bealing (1989). Experience and data from the OECD activated sludge simulation test. In (B.N. Jacobsen, H. Muntau, G. Angeletti, H.A. Painter and DJ. Bealing, eds.) Laboratory tests for simulation of water treatment processes, pp. 113-138. CEC Water Pollution Report 18. (9) ISO 11733 (1995). Evaluation of the elimination and biodegradability of organic substances in an aqueous medium - activated sludge simulation test. International Organization for Standardization, Geneva. (10) Birch, R. R. (1982). The biodegradability of alcohol ethoxylates. XIII Tornado Com. Espafiol. Deterg., 33-48. (11) Birch, R. R. (1984). Biodegradation of nonionic surfactants. J. Am. Oil. Chem. Soc. 61, 340-343. (12) Gerike, P., W.K. Fischer and W. Holtmann (1980). Biodegradability determinations in trickling filter units compared with the OECD confirmatory test. Wat. Res. 14, 753-758. (13) Baumann, U., G. Kuhn and M. Benz (1998). Einfache Versuchsanordnung zur Gewinnung gewasserokologisch relevanter Daten. UWSF - Z. Umweltchem. Okotox. 10, 214-220. (14) HMSO (1982). Methods for the examination of waters and associated materials. Assessment of biodegradability, 1981, pp. 91-98. Her Majesty's Stationery Office, London. (15) US EPA (2007). Simulation test - aerobic sewage treatment: B. Biofilms. Fate, Transport and Transformation Test Guidelines 835.3260, U.S. Environmental Protection Agency, Washington, DC. (16) ASTM (1993). Annual Book of ASTM Standards, Volumes 11.01 and 11.02 on Water and Environmental Technology, and Volume 14.02 on General Methods and Instrumentation. American Society for Testing and Materials, Philadelphia, PA. (17) Horn, J.A., I.E. Moyer and J.H. Hale (1970). Biological degradation of tertiary butyl alcohol. Proc. 25th Ind. Wastes Conf. Purdue Univ., 939-854. (18) Fitter P. and J. Chudoba (1990). Biodegradability of organic substances in the aquatic environment. CRC Press, Boston, MA. (19) Stover, E.L. and D.F. Kincannon (1983). Biological treatability of specific organic compounds found in chemical industry wastewaters. J. Wat. Pollut. Contr. Fed. 55, 97-109. 35 ------- (20) ISO 10634 (1995). Water quality-guidance for the preparation and treatment of poorly water-soluble organic compounds for the subsequent evaluation of their biodegradability in an aqueous medium. International Organization for Standardization, Geneva. (21) Reynolds, L., J. Blok, A. de Morsier, P. Gerike, H. Wellens and WJ. Bontinck (1987). Evaluation of the toxicity of substances to be assessed for biodegradability. Chemosphere 16, 2259-2277. (22) OECD (1984). Activated sludge, respiration inhibition test, no. 209, adopted 4 April 1984. Organization for Economic Cooperation and Development, Paris. (23) ISO 15522 (1999). Water quality-determination of the inhibitory effect of water constituents on activated sludge microorganisms. International Organization for Standardization, Geneva. (24) Fischer, W., P. Gerike and W. Holtmann (1975). Biodegradability determinations via unspecific analyses (chemical oxygen demand, DOC) in coupled units of the OECD confirmatory test. I. The test. Wat. Res. 9, 1131-1135. (25) Nyholm, N., B.N. Jacobsen, B.M. Pedersen, O. Poulsen, A. Dambourg and B. Schultz (1992). Removal of micropollutants in laboratory activated sludge reactors. Biodegradability. Wat. Res. 26, 339-353. (26) Jacobsen, B.N., N. Nyholm, B.M. Pedersen, O. Poulsen and P. Ostfeldt (1993). Removal of organic micropollutants in laboratory activated sludge reactors under various operating conditions: Sorption. Wat. Res. 27, 1505-1510. (27) ISO 14592 (ISO/TC 1477 SC57 WG4, N264) (1998). Water Quality - Evaluation of the aerobic biodegradability of organic compounds at low concentrations in water. International Organization for Standardization, Geneva. (28) Nyholm, N., F. Ingerslev, U.T. Berg, J.P. Pedersen and H. Frimer-Larsen (1996). Estimation of kinetic rate constants for biodegradation of chemicals in activated sludge wastewater treatment plants using short-term batch experiments and |ig/l range spiked concentrations. Chemosphere 33, 851-864. (29) Berg, U.T. and N. Nyholm (1996). Biodegradability simulation studies in semi- continuous activated sludge reactors with low (|ig/l range) and standard (ppm range) chemical concentrations. Chemosphere 33, 711-735. (30) Nyholm, N., U.T. Berg and F. Ingerslev (1996). Activated sludge biodegradability simulation test, Environmental Project No. 337. Danish Environmental Protection Agency, Ministry of Environment and Energy, Copenhagen. (31) Hales, S.G, T.C.J. Feijtel, H. King, K. Fox and W. Verstraete, eds. (1997). 36 ------- Biodegradation kinetics: generation and use of data for regulatory decision making. Proceedings of the SETAC Europe Workshop held at Port Sunlight, UK, 4-6 September 1996. SETAC Europe, Brussels. (32) Birch, R. R. (1991). Prediction of the fate of detergent chemicals during sewage treatment. J. Chem. Tech. Biotechnol. 50, 411-422. (33) Grady, C.P.L., B.F. Smets and D.S. Barbeau (1996). Variability in kinetic parameter estimates: a review of possible causes and a proposed terminology. Wat. Res. 30, 742-748. 37 ------- |