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Aquacultural Engineering 34 (2006) 198–213

www.elsevier.com/locate/aqua-online

Comparative performance of fixed-film biological filters:


Application of reactor theory
Barnaby J. Watten *, Philip L. Sibrell
United States Geological Survey, Leetown Science Center, 11649 Leetown Road,
Kearneysville, WV 25430, USA

Received 20 December 2004; accepted 25 March 2005

Abstract

Nitrification is classified as a two-step consecutive reaction where R1 represents the rate of formation of the intermediate
product NO2-N and R2 represents the rate of formation of the final product NO3-N. The relative rates of R1 and R2 are
influenced by reactor type characterized hydraulically as plug-flow, plug-flow with dispersion and mixed-flow. We develop
substrate conversion models for fixed-film biofilters operating in the first-order kinetic regime based on application of
chemical reactor theory. Reactor type, inlet conditions and the biofilm kinetic constants Ki (h1) are used to predict changes
in NH4-N, NO2-N, NO3-N and BOD5. The inhibiting effects of the latter on R1 and R2 were established based on the g
relation, e.g.:
 N
Ki ½BOD5 
g¼ ¼ 1
Ki;max ½BOD5;max 

where BOD5,max is the concentration that causes nitrification to cease and N is a variable relating Ki to increasing BOD5.
Conversion models were incorporated in spreadsheet programs that provided steady-state concentrations of nitrogen and
BOD5 at several points in a recirculating aquaculture system operating with input values for fish feed rate, reactor volume,
microscreen performance, make-up and recirculating flow rates. When rate constants are standardized, spreadsheet use
demonstrates plug-flow reactors provide higher rates of R1 and R2 than mixed-flow reactors thereby reducing volume
requirements for target concentrations of NH4-N and NO2-N. The benefit provided by the plug-flow reactor varies with
hydraulic residence time t as well as the effective vessel dispersion number, D/mL. Both reactor types are capable of
providing net increases in NO2-N during treatment but the rate of decrease in the mixed-flow case falls well behind that
predicted for plug-flow operation. We show the potential for a positive net change in NO2-N increases with decreases in the
dimensionless ratios K2;ðR2 Þ =K1;ðR1 Þ and [NO2-N]/[NH4-N] and when the product K1;ðR1 Þ t provides low to moderate NH4-N
conversions. Maintaining high levels of the latter reduces the effective reactor utilization rate (%) defined here as (RNavg/
RNmax)100 where RNavg is the mean reactive nitrogen concentration ([NH4-N] + [NO2-N]) within the reactor, and RNmax
represents the feed concentration of the same. Low utilization rates provide a hedge against unexpected increases in
substrate loading and reduce water pumping requirements but force use of elevated reactor volumes. Further g effects on R1

* Corresponding author. Tel.: +1 304 724 4425; fax: +1 304 724 4428.
E-mail addresses: barnaby_watten@usgs.gov (B.J. Watten), philip_sibrell@usgs.gov (P.L. Sibrell).

0144-8609/$ – see front matter. Published by Elsevier B.V.


doi:10.1016/j.aquaeng.2005.03.006
B.J. Watten, P.L. Sibrell / Aquacultural Engineering 34 (2006) 198–213 199

and R2 can be reduced through use of a tanks-in-series versus a single mixed-flow reactor configuration and by improving the
solids removal efficiency of microscreen treatment.
Published by Elsevier B.V.

Keywords: Modeling; Nitrification; Aquaculture; Reactor theory; Performance

1. Introduction and Williams, 1974; Manthe et al., 1984). Reactor


staging can be used to improve nitrification rates when
Fixed-film biological filters are often used to treating waters with high concentrations of organic
oxidize fish excretory products in recirculating matter (Srna, 1975; Antonie, 1976; Miller and Libey,
aquaculture systems (RAS) so as to reduce both 1984; Watten et al., 1993). This configuration
make-up water requirements and pollutant loads on promotes the development of biofilms adapted
receiving streams (Liao and Mayo, 1974; Wheaton specifically to wastewaters present within each
et al., 1994; Shnel et al., 2002). Fixed-film treatment successive stage, e.g., heterotrophs in initial stages
also shows potential for improving discharge quality and nitrifers in later stages. Additionally, staging can
in single pass fish culture applications (Losordo and be used to establish fluid residence time distributions
Westers, 1994; Bergheim and Brinker, 2003). In both (RTD) that approximate plug-flow behavior known to
cases, biofilm development is encouraged within provide superior substrate conversion when reaction
reactors designed to provide the substrate, surface area rates are substrate limited—reaction orders > 0
and hydrodynamic conditions necessary to maintain (Levenspiel, 1972). Examples of fixed-film reactors
activity at high biomass concentrations. Active designed to operate in the plug-flow mode include
surfaces within the reactor consist of a matrix of multi-stage RBC’s (Grady and Lim, 1980; Miller and
microorganisms and extra-cellular polymers that Libey, 1984), up-flow and down-flow submerged beds
allow for attachment to solid surfaces (Hagopian (Haug and McCarty, 1972; Paller, 1992; Ridha and
and Riley, 1998). The composition, density and Cruz, 2001), trickle filters (Rogers and Klemetson,
thickness of the biofilm that develops, following an 1985; Kruner and Rosenthal, 1983; Kamstra et al.,
initial conditioning period, is influenced by site 1998) and fluidized beds (Summerfelt and Cleasby,
specific conditions including wastewater composition, 1993; Nam et al., 2000; Sandu et al., 2002). The latter
substrate flux, biofilm growth, decay and shear losses type is unique in that the solid phase (media with
(Rittmann and McCarty, 1980, 1981; Meunier and attached biofilm) is mixed providing a homogenous
Williamson, 1981). Biofilms in typical aquaculture distribution of reactive surfaces and the potential for
applications include autotrophic bacteria of the genus providing effluent substrate concentrations that lie
Nitrosomonas and Nitrobacter responsible for the below that required, on average, to maintain an active
conversion of NH4-N to NO3-N as well as hetero- biofilm (Rittmann, 1982). The solid phase used in the
trophic bacteria capable of oxidizing organic matter, alternative plug-flow filter types is fixed in position.
e.g., the genus Acenitobacter (Bullock et al., 1993). This requirement establishes a heterogeneous biofilm
Heterotrophic bacteria exhibit a relatively high net cell along the longitudinal axis of the reactor (Haug and
yield per unit mass substrate oxidized (Rittmann and McCarty, 1972; Nijhof, 1995). Mixed-flow reactors
Snoeyink, 1984) which can, under high organic are designed to operate with complete mixing in both
loading conditions, lead to inhibition or displacement liquid and solid phases. Examples here include the
of nitrifers from the biofilm matrix (Liao and Mayo, moving bed biofilter (Rusten et al., 1998; Zhu and
1974; Ohashi et al., 1995; Satoh et al., 2000; Zhu and Chen, 1999), the rotating biodrum (Rogers and
Chen, 2001). Inhibition or displacement can result in Klemetson, 1985; Wheaton et al., 1994) and single
incomplete nitrification with an associated rise in stage RBC’s. Mixed-flow reactors are preferred when
NH4-N and NO2-N above design limits established to reaction rates are not substrate limited—reaction
circumvent ammonia toxicity (Colt and Armstrong, order = 0 (Levenspiel, 1972). Biofilm reactor type
1981) and nitrite induced methemoglobinemia (Smith must be chosen carefully given its effect on
200 B.J. Watten, P.L. Sibrell / Aquacultural Engineering 34 (2006) 198–213

performance as measured by required volume, T = 24 8C). When S is much greater than Ks, Equation
pumping requirements and changes in water chemistry (3) reduces to an expression that is zero-order with
(Rittmann, 1982; Levenspiel, 1972; Weber, 1972). We respect to S. When S is limiting and smaller than Ks, as
quantify these effects following development of in typical salmonid aquaculture applications Equation
performance algorithms that allow standardization (3) reduces to an expression that is first-order with
of certain steady-state biofilm kinetic parameters. respect to S. Here, the rate expressions for each
Model use focuses on both organic effects and nitrogen component of the reaction can be expressed
incomplete nitrification given the sensitivity of fish as (Levenspiel, 1972; Srna and Baggaley, 1975;
to NO2-N at relatively low concentrations. Weatherley, 1984):
1 dMNH4 -N
rNH4 -N ¼ ¼ K1 ½NH4 -N (4)
2. Model development V dt
1 dMNO2 -N
2.1. Nitrification rNO2 -N ¼ ¼ K1 ½NH4 -NK2 ½NO2 -N
V dt
(5)
Nitrification within the biofilm is classified as a
1 dMNO3 -N
two-step consecutive reaction where R1 represents the rNO3 -N ¼ ¼ K2 ½NO2 -N (6)
rate of formation of the intermediate product NO2-N V dt
and R2 represents the rate of formation of the final where M is the mass substrate reacted, V reactor
product NO3-N. The stoichiometry of the reaction has volume and K1 and K2 are the empirically derived
been described as (Haug and McCarty, 1972): first-order reaction rate constants (time1) that repre-
sent the product of a substrate utilization rate constant
R1 : 55NH4 þ þ 5CO2 þ 76O2 and the active microbial mass per unit volume of the
! C6 H7 O2 N þ 54NO2  þ 52H2 O þ 109Hþ reactor. Chemical reaction kinetics, as described in the
(1) equations above, have been used with success to
follow the progress of nitrification within fixed-film
R2 : 400NO2  þ 5CO2 þNH4 þ þ 195O2 þ2H2 O reactors (O’Shaughnessy et al., 1984; Srna and Bag-
! C6 H7 O2 N þ 400NO3  þ Hþ (2) galey, 1975; Weatherley, 1982, 1984; Weatherley
et al., 1993; Watten et al., 1993, 1998). Values of
where C6H7O2N represents the yield (mass) of bac- K1 and the ratio K2/K1 will vary with reactor type and
terial cells. The reactions above are further classified application. Srna and Baggaley (1975) established rate
as being heterogeneous, i.e., fluid and solid phases are constants for a marine subgravel filter system operat-
present and necessary for the reactions to proceed. In ing with an inlet NH4-N of 0.1–0.7 mg/L. Tempera-
both cases, reaction kinetics follow the mixed-order ture, pH and sulfide ion (0.03 mg/L) affected K1 and
Monod relationship (Benefield and Randall, 1980): K2 but small changes in salinity did not (5–8 ppt). K1
dS km xS (h1) rose with increasing pH whereas K2 (h1) fell as
¼ (3) described in the relations: K1 = 0.230 (pH) 1.6
dt Ks þ S
(7.4 < pH < 7.8); K2 = 0.053 (pH) +0.531
where (dS/dt) is the overall substrate utilization rate, (6.6 < pH < 8.6). O’Shaughnessy et al. (1984) pre-
mass volume1 time1, km the maximum rate of sub- sent rate constants for a horizontal plug-flow reactor
strate utilization per unit of attached biomass, time1, 25 m in length. K1 over the NH4-N range of 1.0–
S the substrate concentration, mass volume1, Ks the 1.5 mg/L averaged just 0.039 h1 reflecting the low
saturation constant which has a value equal to the specific surface area provided by the reactor design
substrate concentration when (dS/dt)/x = 0.5km, and x (156 m2/m3). K2/K1 averaged 1.91. Weatherley (1984)
is the active biomass concentration, mass volume1. correlated K1 and K2 with pH based on Srna and
Typical values for Ks;NH4 -N and Ks;NO2 -N are, respec- Baggaley (1975), temperature as described by an
tively, 0.5–2.0 mg/L (Benefield and Randall, 1980) Arrhenius type relationship and dissolved oxygen
and 2.7 mg/L (Rittmann and Snoeyink, 1984; (DO) following the observations of Knowles et al.
B.J. Watten, P.L. Sibrell / Aquacultural Engineering 34 (2006) 198–213 201

(1965). A rate modifying factor for the latter was used where t is expressed in hours. Nitrification is, for all
to describe a linear reduction in K1 with decreases in practical purposes, a unimolecular type reaction
DO within the threshold range 0.7–2.0 mg/L and for (Equation (1) and (2)). Therefore, the following nitro-
K2 within the threshold range 0.7–4.0 mg/L. Predicted gen balance holds:
Ki values agreed well with values established for a
subgravel filter during model verification runs. Here, ½NH4 Nin ¼ ½NH4 -Nout þ ½NO2 -Nout þ ½NO3 -Nout
K1 and K2 averaged 0.430 and 0.100 h1, respectively, (9)
providing a K2/K1 ratio of 0.233. Ebeling (2000)
correlated K1 with hydraulic loading (HL) during an which leads to a solution for [NO3-N]out (Weber,
evaluation of a commercial bubble-wash bead filter 1972):
(T = 21–23 8C). K1 increased with HL from a low of  
12.0 h1 at HL = 13.2 L/min to a high of 35.5 h1 at K1 eK2 t K2 eK1 t
½NO3 -Nout ¼ ½NH4 -Nin 1 þ 
HL = 80.6 L/min. Brazil (2005) reported rate con- K2  K1 K2  K1
stants for a commercial scale RBC operating at a (10)
temperature of 28 8C. In this case, K1 averaged
2.4 h1 with a K2/K1 average of 4.5. Watten et al. Equations (8)–(10) assume NO2-N and NO3-N are
(1993) reported a mean K1 and K2/K1 ratio of 13.9 h1, not present in the influent, an unusual case in salmonid
and 1.6 for a fluidized bed of plastic beads (960 m2/ aquaculture operations. Correcting Equations (8)–(10)
m3) operating with an inlet NH4-N of 0.2–1.5 mg/L for inlet concentrations above zero results in:
(14.3 8C). Concurrently, K1 and the ratio K2/K1 varied
with location in a second reactor treatment of equal ½NO2 -Nout
volume that consisted of three fluidized bed compo- K1 ½NH4 -Nin K1 t K2 t
nents operated in series—K1 and the ratio K2/K1 were ¼ ðe e Þ þ ½NO2 -Nin eK2 t
K2  K1
15.8 h1 and 2.8 for stage 1, 20.3 h1 and 1.5 for stage (11)
2, and 12.8 h1 and 3.1 for stage 3. Staging effects on
Ki values have also been reported for RBC applica-  
tions (Brazil, 2005) reflecting changes in component K1 eK2 t K2 eK1 t
½NO3 -Nout ¼ ½NH4 -Nin 1 þ 
feed composition and substrate loading. Clearly, Ki K2  K1 K2  K1
values vary widely and must therefore be established þ ½NO2 -Nin ð1  eK2 t Þ þ ½NO3 -Nin
for a specific set of operating conditions either empiri- (12)
cally or through application of theoretical models like
those of Rittmann (1982) and Rittmann and McCarty The rate constant K1 is calculated based on
(1980, 1981). Equation (7) given NH4-N conversion, t and the
relation:
2.2. Plug-flow conversion  
½NH4 -Nout
Integration of Equations (4) and (5) gives effluent K1 t ¼ ln (13)
½NH4 -Nin
NH4-N, NO2-N and NO3-N concentrations versus
reactor retention time t when the influent NH4-N The rate constant K2 is solved for by trial and error
concentration is known. In the plug-flow reactor case, given [NH4-N]in, [NO2-N]in, [NO2-N]out, t, Equation
we have (Levenspiel, 1972; Srna and Baggaley, 1975; (11), and a corresponding K1 from Equation (13).
Weatherley, 1982, 1984):
2.3. Mixed-flow conversion
½NH4 -Nout ¼ ½NH4 -Nin eK1 t (7)
Integration of the rate expressions rNH3 -N (Equation
(4)) and rNO2 -N (Equation (5)) for the mixed-flow
K1 ½NH4 -Nin K1 t reactor case gives alternate conversion models for each
½NO2 -Nout ¼ ðe  eK2 t Þ (8)
K2  K1 of the nitrogen components of interest (Levenspiel,
202 B.J. Watten, P.L. Sibrell / Aquacultural Engineering 34 (2006) 198–213

1972; Weber, 1972): the expression (Levenspiel, 1979):


   2  
1 s2 D D mL=D
½NH4 -Nout ¼ ½NH4 -Nin (14) ¼2 2 1e (20)
1 þ K1 t t2 mL mL
  where D/mL is dimensionless. D/mL varies from 1 for
K1 t
½NO2 -Nout ¼ ½NH4 -Nin ideal mixed-flow to 0 for ideal plug-flow. When non-
ð1 þ K1 tÞð1 þ K2 tÞ
ideal behavior occurs, the effects of D/mL on substrate
(15) conversion can be modeled as a variable number n of
  mixed-flow reactors operating in series where n, under
K1 K2 t 2 certain conditions, is correlated with D/mL following
½NO3 -Nout ¼ ½NH4 -Nin
ð1 þ K1 tÞð1 þ K2 tÞ the relation 1/n = 2 (D/mL) (Levenspiel, 1979). When
(16) first-order kinetics apply the model below gives
conversion of NH4-N as a function of n, t and K1
Correcting for the effects of inlet NO2-N and (Levenspiel, 1972):
NO3-N results in the expressions:  
  1
K1 t ½NH4 -Nout ¼ ½NH4 -Nin (21)
½NO2 -Nout ¼ ½NH4 -Nin ð1 þ K1 ti Þn
ð1 þ K1 tÞð1 þ K2 tÞ
  Here, we assume individual reactor components of the
1
þ ½NO2 -Nin (17) series have a common volume and residence time, ti.
1 þ K2 t
When compared to an ideal plug-flow case, the rela-
  tive volume requirements of the tank-in-series reactor
K1 K2 t 2 reduces to the following at a fixed rate of conversion
½NO3 -Nout ¼ ½NH4 -Nin
ð1 þ K1 tÞð1 þ K2 tÞ (Levenspiel, 1972):
 
1
þ ½NO2 -Nin 1 þ ½NO3 -Nin Vseries K1 t
1 þ K2 t ¼1þ (22)
Vplug-flow 2n
(18)
where V is total volume and t is total retention time.
Here, K1 is calculated given changes in [NH4-N], t, Note that plug-flow behavior is approached at a
and the relation below derived from Equation (14): decreasing rate with increasing values of n.
 
1
K1 t ¼ 1 (19) 2.5. Oxidation of organic matter
½NH4 -Nout =½NH4 -Nin

K2 is solved for by trial and error given [NH4-N]in, The rate constants K1 and K2 used to establish
[NO2-N]in, [NO2-N]out, t, Equation (17) and a corre- reactor performance will vary with operating condi-
sponding K1 from Equation (19). tions including the feed concentration of degradable
organic matter that stimulates heterotrophic bacterial
2.4. Tanks-in-series conversion growth (Bovendeur et al., 1990; Ohashi et al., 1995;
Zhu and Chen, 2001). The stoichiometry of the
The conversion models presented thus far assume oxidation reaction associated with organic matter has
ideal plug-flow or mixed-flow reactor behavior. Ideal been expressed as (Benefield and Randall, 1980):
reactor behavior is difficult to achieve, particularly in C5 H12 þ 8O2 ! 5CO2 þ 6H2 O (23)
the plug-flow case, given the sensitivity of RTD to
system geometry. The vessel dispersion coefficient, D/ Although reaction kinetics adhere to the mixed-
mL, is used to identify reactor type given the measured order Monod relationship (Equation (3)), S in
mean residence time, t, and variance, s2, of a salmonid RAS applications (e.g., BOD5) is typically
conservative tracer. These variables are related with much smaller than Ks resulting in kinetics that are
B.J. Watten, P.L. Sibrell / Aquacultural Engineering 34 (2006) 198–213 203

again first-order with respect to S, i.e.


1 dMBOD5
rBOD5 ¼ ¼ K3 ½BOD5  (24)
V dt
where K3 is the BOD5 reaction rate constant (time1)
or treatability factor that represents the product of a
substrate utilization rate constant and the active micro-
bial mass per unit volume of the reactor (Benefield and
Randall, 1980). K3 is related to operating conditions
that include for example, in the trickle filter case,
temperature, packing type, packing depth, surface
hydraulic loading and waste source (Eckenfelder,
1961). Additional variables of importance are dis-
solved oxygen and pH (Benefield and Randall,
1980). The first-order conversion models developed
Fig. 1. Effect of the BOD poisoning coefficient N on the response of
for plug-flow (Equation (7)), mixed-flow (Equation the ratio K1/K1,max to increases in the ratio BOD5/BODmax.
(14)) and tanks-in-series (Equation (21)) reactors
apply here when [NH4-N] and K1 are replaced with
[BOD5] and K3. For example, in the mixed-flow case case, however, a two-step calculation procedure can be
we have: used—[BOD5]out is established based on Equation
  (25), then is used in a second step to adjust both K1 and
1 K2 for inhibition (Equation (26)). Adjusted Ki values
½BOD5 out ¼ ½BOD5 in (25)
1 þ K3 t are then used to predict effluent concentrations of
NH4-N, NO2-N and NO3-N as described earlier
We correct K1 and K2 for the inhibiting effects of
(Equations (14)–(18)). The mixed-flow calculation
BOD5 using a model form (Levenspiel, 1979)
procedure just described, when combined with the
developed to describe product poisoning in microbial
tanks-in-series approach, allows conversion rates to be
fermentation systems. In our case, K1 or K2 established
identified for the plug-flow (with dispersion) reactor
without inhibition (Ki,max) is adjusted given the BOD5
operating with g < 1. Examples include the trickle
concentration that causes nitrification to cease
filter and submerged bed filter. Here, concentrations of
(BOD5,max), the steady-state concentration of BOD5
BOD5, NH4-N, NO2-N and NO3-N calculated in
within the reactor, and a value for N, a coefficient that
effluent of the first reactor stage of a selected number
characterizes the response of Ki values to increasing
of stages (n) are used as the influent condition for the
BOD5 concentrations, i.e.:
second reactor stage in the series. This stage-by-stage
 N calculation procedure is repeated until the effluent
Ki ½BOD5 
g¼ ¼ 1 (26) condition has been identified for the last tank in the
Ki;max ½BOD5;max 
series. This procedure also allows Ki,max to be
If g < 1, the apparent values of Ki established based adjusted, when necessary, for changes in biofilm
on Equation (19) represent the product gKi,max. Fig. 1 characteristics that may occur independently of the
gives a plot of K1/K1,max versus BOD5/BOD5,max for effects of degradable organics (g).
selected values of N. Note that initial reductions in K1
with increasing BOD5 are accelerated as the coeffi- 2.6. Spreadsheet program simulating RAS water
cient N increases. When BOD5 oxidation occurs and chemistry
g < 1, application of Equation (26) precludes use of
the steady-state conversion models developed for the We developed an Excel spreadsheet to carry out the
plug-flow and tanks-in-series reactors given that calculations required to establish steady-state con-
BOD5, and hence Ki/Ki,max, will vary along the centrations of NH4-N, NO2-N and NO3-N within a
longitudinal axis of the reactors. In the mixed-flow salmonid RAS versus selected operating conditions.
204 B.J. Watten, P.L. Sibrell / Aquacultural Engineering 34 (2006) 198–213

Fig. 2. Spreadsheet model components used to simulate the effect of reactor type on water quality dynamics in an RAS. The letters (a–j)
represent model prediction points for the variables BOD5, NH4-N, NO2-N and NO3-N.

Model inputs included reactor type (plug-flow or addressed here but was in a similar spreadsheet
mixed-flow), K1, the ratio K2/K1, system make-up flow designed to simulate the effects of a microscreen
rate (Qmf, m3/h), recirculating flow rate (Qrf, m3/h), BOD5 removal step and reactor staging. Major com-
make-up flow composition ([NH4-N]mf, [NO2-N]mf, ponents of the system modeled are given in Fig. 2. Net
[NO3-N]mf, mg/L), reactor volume (V, m3) and fish BOD5 input was taken as the product of fish feed
feed rate (kg/d). The latter was used to calculate NH4- rate (kg/d), 1  E, and the ratio g biosolids/kg feed,
N loading based on the ratio 29 g/kg feed which where E represents the biosolids removal efficiency
represents a typical value for salmonids (Speece, of the microscreen as a decimal fraction. We used a
1973; Liao and Mayo, 1974). Net changes in nitrogen net biosolids (BOD5) production rate of 400 g/kg
components were established using the reactor feed based on the observations of Speece (1973)
specific conversion models described earlier (either and Liao and Mayo (1974). BOD5 was tracked through
Equations (7)–(12) or (14)–(18)) in combination with each RAS component with conversion accounted for
a material balance. For example, in the case of NH4-N in the primary mixed-flow reactor and tanks-in-series
the following balance holds: reactors (Equation (25)). Reactor specific BOD5
concentrations were used to correct K1 and K2 for
Qmf ½NH4 -Nmf þ MNH4 N ¼ Qof ½NH4 -Nof inhibition effects given a selected value for N
þ ðQmf þ Qrf Þð½NH4 -Nin ½NH4 -Nout Þ (27) (Equation (26)). Additional program inputs included
reactor volumes and reactor configuration—either a
where in this case NH4-N concentrations are single mixed-flow reactor, a tanks-in-series reactor
expressed as g/m3, Qof is a system overflow rate (six stages) or a combination of the both types as
(Qof = Qmf, m3/h) and MNH4 -N is the mass of NH4- illustrated in Fig. 2. In each of the three spreadsheet
N produced by the fish (g/h). The spreadsheet was programs we assume dissolved oxygen, CO2, tem-
designed to allow system operation without recircula- perature, pH and alkalinity are maintained within
tion, if desired, so as to simulate single pass or post desirable ranges by RAS system components not
treatment applications of the biofilm reactors, i.e., included in our modeling exercise and that the unit
Qrf = 0. When recirculation is employed (Qrf > 0), processes/operations used here do not influence the
an iteration procedure and check for convergence reactants of interest. Further, and following the RAS
was required given the rise in reactant concentrations models of Weatherley (1982, 1984) and Weatherley
that occur with time when reactant conversion per pass et al. (1993), we do not address conversion of BOD5,
is less than 100%. Organic inhibition was not NH4-N or NO2-N that may occur outside of the
B.J. Watten, P.L. Sibrell / Aquacultural Engineering 34 (2006) 198–213 205

reactors in the bulk recirculating flow or on piping or


tank surfaces.

3. Model application

We used the spreadsheets to establish reactor


sensitivity to certain operating conditions and to
compare reactor performance. Fig. 3 demonstrates a
typical response of reactor output to changes in
hydraulic residence time t. Here, the NH4-N present in
a plug-flow reactors effluent drops rapidly following a
first-order conversion (R1) to the intermediate product
NO2-N (Equations (1) and (7)). Concurrently, NO2-N Fig. 4. Effect of reactor type on the conversion of [NH4-N] vs.
rises then falls as its own rate of conversion to NO3-N hydraulic retention time when K1 is fixed at 3 or 14.5 h1.
begins to exceed R1. This response is similar to that
observed in experimental biofilm reactors (Ebeling,
2000; O’Shaughnessy et al., 1984; Srna and Baggaley, case is uniformly low throughout the reactor and equal
1975; Zhu and Chen, 1999) and demonstrates a to the reactor’s effluent concentration. The disparity in
declining rate of return on investments in reactor conversion rates will decrease as reactor geometry is
volume or t, particularly with regards to R1. This latter altered so as to lower the working vessel dispersion
point is illustrated in Fig. 4. Here, NH4-N conversion number (D/mL) from the mixed-flow case (1) towards
is plotted versus reactor retention time for both plug- the plug-flow case (0), e.g., by adopting the tanks-in-
flow and mixed-flow reactors operating with a series configuration. This effect is illustrated in Fig. 5
common K1 of 3 or 14.5 h1. The K1 values used where the percent reduction in NH4-N conversion is
are similar to those reported for a commercial scale plotted versus K1t and D/mL. The reduction in
RBC (Brazil, 2005) and a pilot scale fluidized bed conversion in this example drops from a high of
(Watten et al., 1993). Note that in accordance with about 23% with D/mL = 1 to a low of about 3% with D/
theory, the plug-flow reactor provides higher levels of mL = 0.07. The latter corresponds to an RTD provided
conversion given that S (NH4-N) in the mixed-flow by seven mixed-flow reactors operated in series. Note

Fig. 3. Effluent composition of a plug-flow biofilm reactor vs.


hydraulic retention time when inlet [NH4-N] = 1 mg/L. Line A Fig. 5. Effect of the product K1t on the relative rate of NH4-N
represents reactive nitrogen (RN) concentration, i.e., NH4- conversion (%) at selected levels of hydraulic dispersion (D/mL)
N + NO2-N. Line B represents RNmax. within the reactor.
206 B.J. Watten, P.L. Sibrell / Aquacultural Engineering 34 (2006) 198–213

mortality of test salmonids when NO2-N levels rose


above 0.15 mg/L as a result of incomplete nitrification
in both trickle and submerged bed type biofilters.
Smith and Williams (1974) report exposure of
salmonids to 0.15 mg/L NO2-N for just 48 h results
in a 75% conversion of heme iron in hemoglobin from
the ferrous to the ferric state—methemoglobin. This
condition greatly reduces the ability of the blood to
transport oxygen and should therefore be avoided. In
those RAS applications that maintain very low make-
up-flow rates it may be feasible to negate the effect of
the NO2-N on hemoglobin by maintaining high Cl
concentrations in solution as practiced in pond
production of channel catfish (Tucker, 1985). Here,
the objective is to maintain a molar ratio of NO2/Cl of
0.25. This condition provides an acceptable compro-
mise between the cost/logistics of applying NaCl or
CaCl2 and the degree of conversion of hemoglobin to
methemoglobin. Fig. 6 also gives the rearing unit
NO2-N concentrations that correspond with the
changes in reactor volume. As with NH4-N, reactor
volume requirements for the target NO2-N level
Fig. 6. Effect of reactor type and volume on steady-state concen- (0.2 mg/L) are substantially lower for the plug-flow
trations of NH4-N and NO2-N in the rearing unit component of an
versus the mixed-flow reactor application; 17 m3
RAS. Arrows indicate volume requirements for a selected [NH4-N]
of 1 mg/L and a selected [NO2-N] of 0.2 mg/L. versus 26 m3. Fig. 7 shows that NO2-N rises then falls
with increases in t in both reactor types but the rate of
decrease in the mixed-flow case falls well behind that
also that the benefit provided by a plug-flow reactor predicted for plug-flow operation. It is interesting to
rises and then falls as K1t increases. This response is note that K1 and the ratio K2/K1 influence the time at
explained by the converging levels of ammonia removal which NO2-N is maximized (tmax), i.e., through
shown previously in Fig. 4. Fig. 6 gives the net effect of differentiation of the [NO2-N]out functions (Equations
reactor type on volume requirements for a selected set (8) and (15)) and setting d[NO2-N]out/dt = 0, we
of RAS operating conditions including feed rate (60 kg/ obtain for plug-flow (Levenspiel, 1972):
d), total recirculating flow (99 m3/h) and make-up flow
(1 m3/h). NH4-N within the rearing unit declines at a lnðK2 =K1 Þ
tmax;NO2 -N ¼ (28)
decreasing rate with increasing reactor volume in both K2  K1
plug-flow and mixed-flow modes but NH4-N is always
lower in the plug-flow case. The effect of this relation on and for mixed-flow
reactor volume requirements will vary, as shown, with
1
the target NH4-N concentration, e.g., selecting a tmax;NO2 -N ¼ pffiffiffiffiffiffiffiffiffiffiffi (29)
target of 1 mg/L results in volume requirements of 9 K2 K1
and 18.5 m3 for the plug-flow and mixed-flow reactors,
The [NO2-N]out corresponding to tmax;NO2 -N can be
respectively.
derived by combining Equations (8) and (28) in the
Rational design procedures for reactor sizing must
plug-flow case:
also include an analysis of NO2-N given linked effects
on fish stress and mortality (Colt and Armstrong,  K2 =ðK2 K1 Þ
1981; Manthe et al., 1984; Nijhof and Klapwijk, K1
½NO2 -Nmax ¼ ½NH4 -Nin (30)
1995). Liao and Mayo (1974) observed a rapid rise in K2
B.J. Watten, P.L. Sibrell / Aquacultural Engineering 34 (2006) 198–213 207

Fig. 7. Effect of the ratio K1/K2 and hydraulic retention time on a


plug-flow and mixed-flow reactor’s effluent [NO2-N] when K1 is
fixed at 14.5 h1and influent [NO2-N] is 0.2 mg/L. Fig. 8. Effect of influent [NO2-N] on the peak [NO2-N] in effluent of
a plug-flow and mixed-flow reactor.

and by combining Equations (15) and (29) in the


mixed-flow case: K2 = 0.75, as we show the ratio [NO2-N]out/[NO2-
N]in is dependent on the dimensionless ratio [NO2-
1 N]in/[NH4-N]in. This relationship is in agreement
½NO2 -Nout;max ¼ ½NH4 -Nin pffiffiffiffiffiffiffiffiffiffiffiffiffi (31)
½ K2 =K1 þ 12 with the observations of Srna and Baggaley (1975)
and Nijhof and Klapwijk (1995). Fig. 10 shows that
The equations above were developed with the [NO2-N]out drops below an example inlet NO2-N of
caveat [NO2-N]in = 0. Inspection reveals (1) as the 0.2 mg/L only when reactor volume provides for
ratio K2/K1 tends toward 0, both tmax and [NO2- high levels of NH4-N conversion (R1), i.e., with
N]out,max increase as illustrated in Fig. 7, (2) tmax operating K2/K1 ratios of 0.50, 0.75, 0.99 and 1.50
plug-flow is less than tmax mixed-flow and (3) plug- the corresponding NH4-N conversion requirements
flow [NO2-N]out,max is greater than mixed-flow are 97, 94, 88 and 77%, respectively. Surprisingly,
[NO2-N]out,max. Fig. 8 shows that when [NO2-N]in this same figure demonstrates that when K2/K1 is
is greater than 0, [NO2-N]out,max increases while tmax fixed, mixed-flow reactors have a lower NH4-N
is shifted towards lower values. Fig. 8 also shows the conversion requirement for the target [NO2-N]out
ratio [NO2-N]out,max/[NO2-N]in declines as [NO2- than plug-flow reactors—73% versus 88%. However,
N]in rises in response, for example, to a reactor following Equations (7) and (14), the reactor
operating with low conversion rates. Here, net retention time t required to achieve the target
increases in NO2-N across the reactor are masked conversion level (R1) with the mixed-flow reactor
by high ambient NO2-N levels and low NH4-N is still greater then that associated with plug-flow
conversions. Fig. 9 illustrates this effect, with K1/ operation, in this case 30.3 min versus 8.8 min. In
208 B.J. Watten, P.L. Sibrell / Aquacultural Engineering 34 (2006) 198–213

Fig. 9. Effect of K1t and the ratio [NO2-N]in/[NH4-N]in on the ratio [NO2-N]out/[NO2-N]in when operating a plug-flow reactor.

both reactor types, the high NH4-N conversion rates potential (g N/(m3 d)). For example, line A, Fig. 3,
required to establish the condition [NO2-N]out/[NO2- gives the sum of NH4-N and NO2-N versus location
N]in  1.0 lead to a substantial degree of under- along the longitudinal axis of a plug-flow reactor
utilization of the biofilm substrate conversion constructed with a uniform cross-sectional area. We
define the sum of these two nitrogen components as
reactive nitrogen (RN) given their combined or
individual abilities to sustain nitrification reactions.
Here, the microbes within the reactor work at a rate
that is fixed, in the first-order regime, by a mean RN
concentration that lies well below inlet levels
(RNmax). The effective RN concentration (RNavg)
can be calculated by applying the mean value
theorem of integral calculus given functions describ-
ing either the individual or combined (RN) nitrogen
component curves. Considering the combined func-
tion, we know from our material balance (Equation
(3)) that at any time t:

RN ¼ RNmax  ½NO3 -Nout (32)

Then Equation (8), modified so as to reflect the


inverted mirror image relationship between RN and
NO3-N (Fig. 3), gives RN directly as a function of
[NH4-N]in, t, K1 and K2:
  
K1 eK2 t K2 eK1 t
½RNout ¼ ½NH4 -Nin 1 1þ 
K2  K1 K2  K1
(33)
Fig. 10. Effect of the ratio K1/K2 and ammonia conversion (%) on
effluent [NO2-N] when operating a plug-flow reactor with an Applying the mean value theorem of integral
influent [NO2-N] of 0.2 mg/L. calculus to Equation (33) gives RNavg as a function of
B.J. Watten, P.L. Sibrell / Aquacultural Engineering 34 (2006) 198–213 209

the same variables:

RNavg ¼ ½NH4 -Nin


 
K1
K2 ðK2K1 Þ ðe
K2 t
1Þ K1 ðKK22K1 Þ ðeK1 t 1Þ

t
(34)

A somewhat different approach was used to


establish RNavg for the mixed-flow reactor. Here,
we start with [NO3-N]out based on Equations (16).
Recognizing that in this type of reactor RNout = RNavg
and considering Equation (32), we obtain RNavg as a
function of the variables of interest without applica-
tion of the mean value theorem:
 
K1 K2 t2
RNavg ¼ ½NH4 -Nin 1  (35)
ð1 þ K1 tÞð1 þ K2 tÞ
The RNavg calculated for a selected reactor type or
set of operating conditions is compared to RNmax to
establish the effective reactor utilization rate:
 
RNavg
Reactor utilization rate  ð%Þ ¼ 100
RNmax
(36)
Fig. 11. Effect of reactor type, K2/K1 and K1t on reactor utilization
The utilization rate then represents the degree to rate (%) = (RNavg/RNmax)  100.
which the biofilm present within the reactor is
saturated with RN relative to that present in the
reactor’s feed. Fig. 11 shows utilization rates drop Our modeling also suggests that high reactor utilization
with increases in K1t (or NH4-N conversion, rates are indicative of net increases in [NO2-N] across
Equation (7)) and rise as the ratio K2/K1 tends the reactor (Figs. 7–10) that may cause [NO2-N] to rise
toward 0. For example, with a K2/K1 = 0.75, K1t above species-specific standards. Therefore the design
values providing NH4-N conversions of 37 and 95% approach used to size the reactor should consider the
(plug-flow) result in reactor utilization rates of 97.8 interrelationships between conversion rate, pumping
and 60.8%, respectively. Reactor utilization rates are requirements, reactor capital, water chemistry and fish
somewhat lower in the mixed-flow versus the plug-flow health.
reactor when compared at a common K1t value Simulation runs discussed thus far have not
(Fig. 11). With K1t = 2.33 and K2/K1 = 0.75, for addressed the effects of organics (BOD5) on reactor
example, reactor utilization rates for the plug-flow performance. Fig. 12 gives the NH4-N and NO2-N
and mixed-flow reactors are 72.7 and 55.5%, respec- concentrations predicted for the rearing unit compo-
tively. Selecting a K1t with either reactor type that nent of the RAS defined in Fig. 2 when operating with
provides a high reactor utilization rate can minimize either of two reactor configurations—a single mixed-
reactor volumes needed to handle average daily loads flow reactor (3 m3 volume) or a tanks-in-series reactor
but (1) it will not provide the reserve capacity available (3 m3 volume). The latter includes a primary mixed-
with low utilization rates that are useful in hedging flow reactor (0.75 m3 volume) followed by six
against diel or unexpected increases in substrate loading secondary mixed-flow reactors (2.25 m3 total volume)
and (2) it will increase water pumping requirements. simulating plug-flow operation with a homogeneous
210 B.J. Watten, P.L. Sibrell / Aquacultural Engineering 34 (2006) 198–213

Fig. 13. Effect of microscreen efficiency and reactor type on [NO2-


Fig. 12. Effect of feed rate and reactor type on [NO2-N] and [NH4- N] and [NH4-N] in the fish tank component of an RAS.
N] in the fish tank component of an RAS.

solid phase, e.g., a fluidized bed. The K3 value required gives g and BOD5 versus position as well as model
for BOD5 conversion estimates (6.3 h1; Equation predicted NH4-N, NO2-N and NO3-N when operating
(25)) was taken from Watten et al. (1993). The product- at feed rates of 2 and 12 kg/d. Note g increases, at
poisoning coefficient N (Equation (26)) was fixed at a 12 kg/d, from a low of 0.13 in the primary reactor to a
value of 5 to explore a case of high initial sensitivity to high of 0.61 in the last stage of the series reactor. An
BOD5 (Fig. 1). BODmax (Equation (26)) was set at initial rise then fall in NO2-N can be seen as water
20 mg/L, for example purposes only, based on the moves from stage to stage following the response
observations of Antonie (1976) and Weng and Molof predicted in Fig. 7. Further runs (Table 1) show
(1974). The make-up flow requirement of the RAS in all steady-state concentrations of NO2-N and NH4-N
cases (0.1 m3/h) represented 1% of the total flow drop significantly when the poisoning coefficient N is
directed through the rearing unit (10 m3/h). The reduced from 5 to 1, the latter establishing a linear
removal of suspended solids across the microscreen (negative) effect of BOD5 on g (Fig. 1), e.g., in the fish
was initially held at 60% (E = 0.6). This lies within the tank effluent NO2-N and NH4-N drop from 0.55
range of E = 0.21  0.68 reported for RAS applications to 0.14 and 1.99 to 1.55 mg/L, respectively. The g
by Bergheim and Brinker (2003) and Twarowska et al. factor here rises to a range of 0.61–0.91. Reducing
(1997). Fish feed rates were varied from 2 to 12 kg/d the microscreen efficiency to 30% (E = 0.3) acts to
which correspond to a change in dissolved oxygen lower g and elevate BOD5, NO2-N and NH4-N
across the rearing unit of between 2.1 and 12.5 mg/L (Table 1). Fig. 13 shows this effect on fish tank
assuming an oxygen demand ratio of 0.25 kg/kg feed effluent composition over the solids removal effi-
(Losordo and Westers, 1994). Model predicted con- ciency range of 10–80%. In this case the N used to
centrations of BOD5 in the microscreen effluent define g was fixed at 3. Note that NH4-N and NO2-N
(reactor feed) ranged from 2.0 to 12.2 mg/L in the drop at a decreasing rate as solids removal efficiency
mixed-flow case and from 1.6 to 9.9 mg/L in the tanks- approaches 80%. The E-value required for a design
in-series case. The latter provided lower NH4-N and level of NH4-N and NO2-N are lower in the tanks-in-
NO2-N concentrations than the mixed-flow reactor series versus mixed-flow reactor configuration.
(Fig. 12) in agreement with our earlier simulation
results established without BOD5 inhibition (Figs. 4–6).
The inhibition parameter g (Equation (26)), in the 4. Summary
mixed-flow case, dropped from 0.92 to 0.31 as feed rate
increased. In the tanks-in-series application, g varied We develop substrate conversion models for fixed-
with position along the length of the reactor axis film biological filters operating in the first-order
reflecting stage-by-stage reductions in BOD5. Table 1 kinetic regime based on application of chemical
Table 1
Model predicted water chemistry variables vs. sample point in an RAS operating under four test case conditions
Test case Variable RAS component

B.J. Watten, P.L. Sibrell / Aquacultural Engineering 34 (2006) 198–213


Fish tank Fish tank Micro-screen Primary reactor Tanks-in-series reactor
(in) (out) (out) (out) Stage 1 Stage 2 Stage 3 Stage 4 Stage 5 Stage 6
(out) (out) (out) (out) (out) (out)
2 kg/d; N = 5; E = 0.6 BOD5 0.3 3.6 1.6 1.1 0.9 0.7 0.6 0.5 0.4 0.3
g 0.75 0.79 0.83 0.86 0.89 0.91 0.92
NH4-N 0.02 0.26 0.26 0.14 0.10 0.07 0.05 0.03 0.02 0.02
NO2-N 0.02 0.02 0.02 0.06 0.06 0.06 0.05 0.04 0.03 0.02
NO3-N 23.87 23.87 23.87 23.94 23.98 24.02 24.05 24.07 24.09 24.11
12 kg/d; N = 5; E = 0.6 BOD5 1.9 21.9 9.9 6.7 5.4 4.4 3.5 2.9 2.3 1.9
g 0.13 0.21 0.29 0.38 0.46 0.54 0.61
NH4-N 0.54 1.99 1.99 1.75 1.58 1.37 1.14 0.92 0.72 0.54
NO2-N 0.55 0.55 0.55 0.65 0.71 0.75 0.75 0.71 0.64 0.55
NO3-N 141.65 141.65 141.65 141.79 141.90 142.07 142.29 142.55 142.83 143.10
12 kg/d; N = 1; E = 0.6 BOD5 1.9 21.9 9.9 6.7 5.4 4.4 3.5 2.9 2.3 1.9
g 0.67 0.73 0.78 0.82 0.86 0.88 0.91
NH4-N 0.10 1.55 1.55 0.92 0.66 0.47 0.33 0.23 0.15 0.11
NO2-N 0.14 0.14 0.14 0.38 0.40 0.37 0.31 0.25 0.15 0.11
NO3-N 143.27 143.27 143.27 143.67 143.90 144.13 144.33 144.50 144.63 144.73
12 kg/d; N = 1; E = 0.3 BOD5 3.3 23.2 17.3 11.7 9.5 7.7 6.2 5.0 4.1 3.3
g 0.41 0.53 0.62 0.69 0.75 0.80 0.84
NH4-N 0.17 1.62 1.62 1.13 0.89 0.67 0.49 0.35 0.25 0.17
NO2-N 0.21 0.21 0.21 0.43 0.47 0.46 0.42 0.35 0.28 0.21
NO3-N 143.14 143.14 143.14 143.41 143.61 143.83 144.06 144.27 144.44 144.58

211
212 B.J. Watten, P.L. Sibrell / Aquacultural Engineering 34 (2006) 198–213

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