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Water Research 37 (2003) 18901904

Impact of bubble and free surface oxygen transfer on diffused aeration systems
Connie D. DeMoyera, Erica L. Schierholza, John S. Gullivera,*, Steven C. Wilhelmsb
a

St. Anthony Falls Laboratory, Department of Civil Engineering, University of Minnesota, Mississippi River at 3rd Avenue, SE, Minneapolis, MN 55414, USA b US Army Corps of Engineers Research and Development Center, Waterways Experiment Station, 3909 Halls Ferry Road, Vicksburg, MS 39180, USA Received 1 November 2001; received in revised form 1 November 2002

Abstract The primary location of oxygen transfer in a diffused aeration system is examined by separately determining the surface airwater and bubblewater mass transfer coefcients. The mass transfer model developed to determine the mass transfer coefcients advances the McWhirter and Hutter (A.I.Ch.E. J. 35(9) (1989) 1527) model by tracking oxygen and nitrogen transfer into and out of the bubbles as they rise to the water surface. The resulting vertical proles of the liquid-phase equilibrium concentration inside the bubble and the gas-phase oxygen composition give insight into how the bubblewater concentration gradient changes over depth. The surface mass transfer coefcient, kLs as ; is 5985% of the bubble mass transfer coefcient, kL ab ; and the driving concentration difference is smaller for surface transfer. Surface transfer and bubble transfer both contribute signicantly to oxygen transfer; however, bubble transfer is the primary mode of oxygen transfer for this system at the air ow rates used. Further experiments demonstrate that most of the surface transfer occurs above the bubble plume. r 2002 Elsevier Science Ltd. All rights reserved.
Keywords: Submerged diffuser; Aerator; Transfer coefcient; Lake aeration; Surface transfer; Bubble transfer

1. Introduction Submerged aeration systems are used in lakes, reservoirs, and wastewater treatment facilities to increase dissolved oxygen (DO) levels and promote water circulation. Submerged diffusers release air or pure oxygen bubbles at depth, producing a free, turbulent bubble-plume that rises to the water surface through buoyant forces at roughly an 111 angle of spreading [1]. The ascending bubble plume entrains water, causing vertical circulation and lateral surface spreading. Oxygen transfers to the water across the bubble interfaces as the bubbles rise from the diffuser to the water surface.
*Corresponding author. Tel.: +612-625-4080; fax: +612627-4609. E-mail address: gulli003@tc.umn.edu (J.S. Gulliver).

Oxygen transfer also occurs across the airwater interface at the free surface due to turbulence induced by bubble-plume motion and water circulation. Manufacturers provide performance estimates for specic diffusers based on experimental tank test results. Diffuser depth is typically between 3 and 5 m. Buyers can determine the total rate of oxygen transfer that a diffuser achieves under varying gas ow rates at the testing depth, but they cannot determine how the diffuser will perform at greater depths. Performance estimates also do not specify where oxygen is transferred in the system. Determining the location of oxygen transfer is important for the proper design of diffused aeration systems at depths other than those tested. In a lake or reservoir that is not well mixed, the inuence of the airwater transfer rate and the bubble water transfer rates at various depths in the water

0043-1354/03/$ - see front matter r 2002 Elsevier Science Ltd. All rights reserved. PII: S 0 0 4 3 - 1 3 5 4 ( 0 2 ) 0 0 5 6 6 - 3

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Nomenclature at Acs As At C Cb
CN Co

Csat Css D h hd H Jb Js

total specic surface area cross-sectional tank area water surface area total surface area for transfer actual dissolved oxygen concentration gas-phase oxygen concentration inside a given bubble liquid-phase equilibrium nitrogen concentration of a bubble liquid-phase equilibrium oxygen concentration of a bubble saturation oxygen concentration in water at atmospheric pressure steady-state dissolved oxygen concentration diffusion coefcient of gas in water total water depth depth to diffuser Henrys law constant bubblewater oxygen transfer rate free surface oxygen transfer rate

k kG kL kLs kL ab kL at kLs as P Pwv Qa R SK SK V y z dc y

bulk transfer rate coefcient gas lm transfer rate coefcient liquid lm transfer rate coefcient water surface mass transfer rate coefcient volumetric bulk mass transfer coefcient for bubble surface total volumetric mass transfer coefcient volumetric mass transfer coefcient for water surface atmospheric pressure water vapor pressure gas ow rate ratio of normalized sensitivity coefcients normalized sensitivity coefcient volume of water body gas-phase oxygen composition distance from the diffuser instantaneous thickness of the concentration boundary layer empirical coefcient for temperature adjustment

column can be important in designing diffuser placement. The relationship between diffuser depth and oxygen transfer is also an important design criteria for activated sludge systems in wastewater treatment. Since there is a trend to design deeper aeration tanks of 8 12 m instead of the historically standard 35 m tanks, a more detailed investigation of airwater and bubble water transfer can be justied for wastewater treatment applications [2]. By understanding where oxygen transfer occurs, diffuser systems can be designed to either maximize bubble transfer at certain water depths or to maximize surface turbulence and mixing which induces greater free surface transfer. In this paper the relative amount of surface and bubble oxygen transfer in an aerated water body is estimated by separately determining the surface-transfer coefcient and bubble-transfer coefcient. This is accomplished by modifying McWhirter and Hutter [3] oxygen mass transfer model to include both oxygen and nitrogen transfer as the bubbles rise through the water column. The model results are compared to aeration tests in which the water surface was reduced with oating Styrofoam slabs, in order to identify where the surface transfer occurred.

dures for clean water [4]. Sodium sulte with a cobalt chloride catalyst is used to chemically deoxygenate the tank water. A minimum of four DO probes is placed inside the test tank to measure DO and temperature. DO concentrations are recorded continuously over time until the oxygen level in the tank reaches at least 98% of the presumed steady-state DO value, assuming the difference between the steady-state concentration and actual concentration decays exponentially (Fig. 1). The total change in DO concentration in a completely mixed body of clean water, due only to aeration is often expressed as dC kL at Css C ; dt 1

2. Background 2.1. Standard testing methodology The oxygen transfer tests used in the model were conducted in accordance with ASCE Standard proce-

where at (L1) is the total specic surface area At =V ; V the volume of water body (L3), kL the bulk liquid lm transfer rate coefcient (L T1), At the total surface area for transfer (L2), Css the steady-state DO concentration during aeration, and C the actual DO concentration in water body. The ASCE Standard applies the experimental data set of measured DO concentrations over the testing time period to this equation. A non-linear regression determines an initial DO concentration, the steady-state DO concentration, Css ; and the total volumetric oxygen transfer coefcient, kL at (T1), for each tank test. Performance parameters used in designing aeration systems such as the standard oxygen transfer rate (SOTR), standard oxygen transfer efciency (SOTE), and standard aeration efciency (SAE) are then calculated from these curve-t coefcients.

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0.3

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Css
0.25

Dissolved oxygen, mol/m

Csat
0.2

0.15

0.1

0.05

0 0 1 2 3 4 5 6 7 8 9

Time, hrs
Fig. 1. DO versus time curve for free surface test, Qa 51 scmh. Css is the steady-state DO concentration and Csat is the saturation concentration of oxygen in water.

2.2. Challenges beyond standard testing methodology When a submerged diffuser is operated, there are two main interfaces over which oxygen transfer occurs. Oxygen transfer occurs across the bubble interfaces as the bubbles rise through the water column. Oxygen transfer also occurs across the water surface at the air water interface. Eq. (1) can be separated into airwater oxygen transfer and bubblewater oxygen transfer components. At the free surface, oxygen transfer is driven by a concentration gradient between the saturation (equilibrium) concentration of oxygen dissolved in the water at the water temperature and atmospheric pressure, Csat ; and the actual DO concentration, C : The free surface oxygen transfer rate, Js ; is described by Z kLs Csat C dAs ; 2 Js
As

oxygen concentration inside a bubble also depends on gas ow rate and the changing bubblewater transfer coefcient over depth. In order to describe bubble-transfer behavior, the difference in the liquid-phase equilibrium oxygen con centration of the bubble, Co ; and the actual DO concentration in the water, C ; produces bubblewater oxygen transfer, Jb ; according to Z kL ab Co C dV ; 3 Jb
V

where kLs (L T1) is the mass transfer rate coefcient for the water surface. The surface ux is integrated over the water surface area, As : The bubble-transfer rate involves some additional considerations. The liquid-phase equilibrium concentration of a given bubble is not only a function of temperature and atmospheric pressure, but also hydrostatic pressure and gas-phase oxygen composition. As bubbles rise, bubblewater gas transfer of oxygen, nitrogen, argon, carbon dioxide, and trace gases occurs due to a concentration gradient between the equilibrium bubble concentration and the ambient water concentration. Over depth, the bubblewater transfer of all gases affects the gas-phase oxygen composition and the equilibrium oxygen concentration. The equilibrium

where kL ab (T1) is the volumetric bulk mass transfer coefcient for the bubble surfaces. The bubble oxygen ux is integrated over the water volume. Mass conservation of volatile gases in a clean-water aeration test is then described by combining Eqs. (2) and (3): Z dC V kL a b C o C dV dt V Z kLs Csat C dAs : 4
As

The kLs value depends on the region of oxygen transfer at the water surface. Oxygen transfer occurs as bubbles burst in the surfacing bubble plume. Transfer also occurs outside of the bubble plume across the surrounding water surface due to turbulence induced by bubbleplume motion and water circulation. Since the surface mass transfer rate coefcient depends on the level of turbulence produced at the water surface, kLs is generally believed to vary somewhat between the turbulent region of the surfacing bubble plume and the less turbulent region surrounding the bubble plume [5]. This research examines the importance of total water

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surface transfer in comparison to bubble transfer, and also species the region through which the surface transfer occurs. A constant bubble kL value over depth is assumed, which should be reasonable if plume turbulence does not vary greatly with depth. The bubble size and surface area, however, change during bubble rise due to pressure reduction, bubble splitting and coalescence, and oxygen and nitrogen mass transfer into and out of the bubble. Since the changing bubble size is important but difcult to measure, a single bulk bubble-transfer coefcient, kL ab ; to represent the rate of oxygen transfer throughout the entire water depth has been used in previous research [3]. Thus, the investigations that split mass transfer coefcients into kL ab and kL as have assumed that these coefcients are constant in the integration [3,58]. This simplication is also used herein. In addition, the water concentration is assumed to be constant over space in the tank. With these assumptions, Eq. (4) simplies to Z dC kL ab C C dz kLs as Csat C ; 5 dt hd z o where hd is the depth from diffuser to water surface, z is the distance from diffuser, and as As =V : 2.3. Previous research Conicting claims have been made regarding the contribution of surface transfer and bubble transfer to overall aeration in diffused aeration systems. In activated sludge applications, it is commonly believed that bubble transfer is the primary location of oxygen transfer. For diffused aeration systems in lakes and reservoirs, the most inuential location of oxygen transfer, across the free surface or the bubble interface, is still being debated. Values of kL for bubblewater and airwater transfer have been determined by a number of researchers under various test conditions (Table 1). The most relevant papers relating to the determination of separate transfer locations are more thoroughly discussed below. Under typical activated sludge tank operating conditions with a mean bubble diameter of 1.8 mm and a retention time of 10 s, Camp [6] estimates that the interfacial surface area of an air bubble plume, Ab ; is about 42 times greater than the interfacial surface area of the water surface, As : Camp claims that the rate of renewal of the liquid lm at the water surface is most likely less than the rate of renewal of the air bubble surfaces. When assuming, however, that the rate of renewal of the water surface and bubble surface are equal, the rate of oxygen transfer from the water surface will only comprise 2.4% of the total oxygen transfer in the system. From this estimation, Camp concludes that

bubbles, therefore, are the principal means by which gas transfer is accomplished, and the smaller the bubbles the more effective the transfer. To determine the most important design criteria for submerged aerators in reservoirs, Neilson [5] studied whether articial aeration results primarily from transfer across bubble surfaces or from mixing that induces surface transfer. At a gas ow rate of 0.069 standard cubic meters per hour (scmh), Neilson varied the water depth from 0.1 to 1 m and the water volume from 0.01 to 0.1 m3. By reducing the tank surface area from 0.015 to 0.1 m2 with styrene slabs and estimating interfacial areas, Neilson separated the liquid lm coefcients for various oxygen transfer locations. He obtained kL values of 82, 90, and 15 cm h1 for bubble transfer during bubble formation and rise, surface transfer as bubbles burst at the surface, and surface transfer from outside the region of bubbly ow, respectively. Holroyd and Parker [7] obtained similar values by using a sintered glass diffuser in a smaller tank, yielding kL values of 78, 264, and 25 cm h1 for bubble formation and rise, bubble bursting, and surface transfer outside of the bubbly ow region, respectively. Neilson attributes both higher surface liquid lm coefcients to greater turbulence and circulation patterns produced in a smaller volume tank. When Neilson applies his small-scale experimental values to a large-scale water supply reservoir, he concludes that bubble transfer and bubble bursting at the surface account for only 6% of the total aeration. In this example, surface transfer induced by mixing outside of the surfacing bubble plume dominates the transfer process since the interfacial surface area of this reservoir appears to be much larger than the interfacial areas of the other transfer modes. However, interfacial areas must be carefully estimated. The radius of inuence of the diffusers may not be large enough to induce surface transfer throughout the entire interfacial area of the reservoir water surface. Additionally, the interfacial area of the bubble plume can be easily underestimated. Wilhelms and Martin [8] developed an approach to separate surface and bubble transfer by releasing nitrogen gas from a diffuser rather than air. They assume that no oxygen is initially present in the bubbles, thereby eliminating the estimation of a value for concentration inside the bubbles. Steady state is reached between the absorption of oxygen through surface transfer and the stripping of oxygen from the water by nitrogen bubbles. They conducted aeration tests in a 1.1 m deep, 3.72 m3 rectangular tank with a surface area of 3.38 m2. At a gas ow rate of 1.134 scmh, their results indicate that approximately one-third of the total oxygen transfer is surface transfer, while two-thirds of the oxygen transfer is from the bubble plume. They speculate that the

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Table 1 Mass transfer coefcients in literature Bubble mass transfer kL (cm h ) kL ab (1 h ) 140 108252 78 264 25 115162 110200 36216 29 122 181800 4397 112170 50108 36266 Gas velocity=114 cm s1
1 1

Surface mass transfer kLs (cm h1) kLs as (1 h1) Details Bubble diameter 2.4 mm Bubble diameters 0.35 mm kLs for bubbles bursting kLs for natural aeration Bubble diameters 35 mm Bubble diameters 0.62 mm For bubble diameter o2.5 mm For bubble diameter >2.5 mm, gas velocity=114 cm s1

Researchers

Description

Scouller and Watson [9] Higbie [10] Holroyd and Parker [7]

Bubble column Penetration theory Tank with sintered glass diffuser; water depth=624 cm

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Coppock [11] Ippen et al. [12] Pasveer [13] Calderbank [14]

Bubble Bubble Bubble Bubble

column column column column

Yoshida and Akita [15] Hughmark [16] Barnhart [17] Calderbank et al. [18]

Lamont and Scott [19]

Carbon dioxide bubbles, diameter 0.050.4 mm Carbon dioxide bubbles

Akita and Yoshida [20]

15700 36162

Akita and Yoshida [21]

Gas holdup range 0.0250.45, pure oxygen injected Single orice spargers, bubble size=2.32 mm 18648

Deckwer et al. [22]

Bubble column Bubble column Bubble column Bubble column: 122 cm high 10.6 cm diameter Turbulent pipe ow: diameter 1.588 and 0.794 cm, horizontal and vertical Bubble column: 400 cm high 7.7 60 cm diameter Bubble column: 250 cm high, crosssections 7.7 7.7 cm, 15 15 cm, 30 30 cm Bubble column

Mavinic and Bewtra [23] 82 90 kLs for bubbles bursting, kLs for natural aeration, air bubble curtain with bubble diameter of 0.5 cm, Qa 0:069 m3 h1; 2.5 cm dia. Brass pipe with 10 holes of 0.061 cm dia.

22180 165241

Neilson [5]

Bubble column: 0.62.7 m high U tube Tank tests: 15.2 66 122 cm tank, water volume=0.010.1 m3, water depth=0.11.0 m, surface area reduced from 0.0150.1 m2 to measure surface transfer 15 36108 1805400 2240 180 Bubble diameter 0.31.0 mm, pure oxygen Gas velocity=428 cm s1 Gas velocity=113 cm s1 Air velocity=2.515 cm s1, air velocity=0.20.7 cm s1 210, 418 213.5 3048, 213.52286 0.7 4, 0.73 2430 coarse bubble diffusers, Qa 213:02683:4 m3 h1; 126 ne bubble diffusers, Qa 125:42462:6 m3 h1 0.36 Qa =1:134 m3 h1, 23 cm dia. Flexible-head diffuser

Motarjemi and Jameson [24] [25]

Mangartz and Pilhofer [26]

Cockx et al. [27]

McWhirter and Hutter [3]

Wilhelms and Martin [8] 0.72 39.6

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Popel and Wagner [2]

Bubble column: 65 cm high, crosssection 12 12 cm Bubble column: 250 cm high 66 cm wide 2.5 cm deep Bubble column: 270 cm high 10 and 14 cm diameter Bubble column (4 m high 20 cm dia.), Deep U tube (8 m high 5.3 cm dia.) Tank tests: water volume=113.2 283.1 m3, water depth=3.05 7.62 m, surface area=37.2 m2 2 parameter regression calculates kL ab ; kLs as Tank tests: 1.3 2.6 1.1 m, water volume=3.72 m3, water depth=1.1 m, surface area=3.38 m2; found KL ab ; KLs as by releasing nitrogen bubbles Empirical Model to simulate oxygen transfer in deep tanks 0173

Bubble diameters 0.43 mm

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relative transfer across the water surface would decrease as the water depth increases, although no evidence is presented to support this assumption. High gas discharge rates were not feasible, however, because of the cost of nitrogen gas. All of the above experiments assumed that hydrostatic pressure effects on the bubble were small and that the gas concentration inside the bubble did not change signicantly. McWhirter and Hutter [3] developed an oxygen mass transfer model to more accurately describe the actual mass transfer processes in diffused aeration systems by separating kL ab and kL as from one aeration test at high gas discharge rates. They describe the steady-state oxygen concentration in the water during tank aeration tests as a dynamic steady-state bulk liquid DO concentration. At this steady-state value, absorption of oxygen from gas bubbles to the water in the deep regions of the tank is balanced by desorption of DO back into the gas bubbles near the water surface and desorption of oxygen across the tank surface into the atmosphere. Their model tracked the change in oxygen concentration in the bubbles as they rose through the water column. Some error was introduced, however, since transfer of other gases from the bubbles, particularly nitrogen, was not incorporated. McWhirter and Hutter separated the surface mass transfer coefcient, kLs as ; and the bubble mass transfer coefcient, kL ab ; by applying experimental aeration test data from the Los Angeles County Sanitation Districts to their oxygen transfer model. In the aeration tests multiple diffusers were placed at a submerged depth of 3.057.62 m with a tank water surface of 37.2 m2 and water volumes of 113.2283.1 m3. Twenty-four to thirty coarse bubble diffusers were operated at air ow rates of 213.0683.4 scmh and 126 ne bubble diffusers were tested at 125.4462.6 scmh. From the experimental data, McWhirter and Hutter obtained best-t mass transfer coefcient values. They determined that kL ab is 58 times greater than kLs as for the ne bubble diffuser system tested, while kL ab is 23 times greater than kLs as for the coarse bubble diffuser system tested by the Los Angeles County Sanitation Districts. Their analysis provides the framework for the analysis procedure in this research.

nitrogen equilibrium concentrations are P Pwv hd z=10:33 n Co CsatO2 1 Pwv y=1 y ; 6 0:21 P Pwv hd z=10:33 n CN CsatN2 1 Pwv 1=1 y ; 7 0:79 where y is gas-phase oxygen composition, which is the molar ratio of oxygen to other gases (primarily nitrogen) in the gas phase, P (atm) is atmospheric pressure, Pwv (atm) is water vapor pressure, hd (m) is depth to the diffuser, and z (m) is a variable distance from the diffuser. To track the oxygen mole ratio inside the bubbles, the transfer of both oxygen and nitrogen across the bubblewater interface must be considered, presuming that the transfer of other gases occurs at the same rate as nitrogen. The gas-phase oxygen composition as a function of depth is computed from the mole ratio for a humid atmosphere and the relationship: dy 1 dCbO2 CbO2 dCbN2 2 : 8 dz CbN2 dz CbN dz
2

The gas-phase concentration of oxygen and nitrogen inside the bubble as a function of depth can be written dCbO2 1 n kL Ab Co C o ; 9 Qa hd dz   dCbN2 1 DN2 1=2 n kL Ab CN CN : Qa hd DO2 dz 10

The kL ab value for nitrogen gas is 94% of that for oxygen gas, assuming a 1 2 power relationship of diffusion coefcients [28]. Combining (8), (9) and (10),  dy Acs 1 n kL ab Co Co n dz Qa C N !   n DN2 1=2 Co n C N C N ; 11 n 2 DO2 C N where Acs is the cross-sectional surface area of tank, Qa the gas ow rate, Co the measured DO concentration in the water, and CN the measured dissolved nitrogen concentration in the water. The boundary condition for Eqs. (6) and (7) is that y 0:266 when the bubbles are released from the diffuser at z 0: With Eqs, (6), (7) and (11), the gas-phase oxygen composition, y; and the equilibrium oxygen concentra tion, Co ; can be calculated at all depths and times. The resulting values of Co can then be used in Eq. (5) along with the experimental DO concentrations over the time duration of each experiment. By minimizing the standard error between the predicted and measured

3. Current approach Using experimental aeration data, a non-linear regression is performed on the unsteady oxygen mass transfer equation (Eq. (5)) to obtain the best-t values for the unknown parameters, kL ab and kLs as : In order to solve Eq. (5), the liquid-phase equilibrium concentration of the bubbles, Co ; must be computed. The oxygen and

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DO concentrations, the best-t values of kL ab and kL as can be determined.

Styrofoam Cover

4. Materials and methods Standardized aeration tests were conducted at the US Army Corps of Engineers Research and Development Center in Vicksburg, MS in a 7.6 m diameter 9.6 m deep cylindrical tank at a water depth of 9.25 m. The test tank is shown in Fig. 2. Under similar conditions in the same tank, four additional tests were conducted with Styrofoam slabs covering the water surface around the surfacing bubble plume (Fig. 3). In these tests, the tank water surface was covered with 30 cm thick Styrofoam blocks pinned together by 7.6 cm wide metal straps. Along the edges of the tank, the exposed water surface was covered with Styrofoam peanuts to reduce oxygen transfer across the airwater interface. In order to release the gas that is not transferred to the water, a 1.8 m diameter hole was cut in the center of the Styrofoam cover, as shown in Fig. 4. The cover reduced the water surface area from 45.6 to 2.6 m2. A stainless steel coarse bubble diffuser, produced by Aercor, Worcester, Massachusetts, was mounted 0.9 m off of the tank bottom. The diffuser has a horizontal inverted trough that distributes gas along the length of the diffuser. Bubbles are released through holes of

Fig. 3. Experimental setup with Styrofoam cover.

Fig. 4. Bubble plume surfacing in center of Styrofoam cover.

Fig. 2. Aeration test tank at U.S. Army Corps of Engineers Research and Development Center, Vicksburg, MS.

varying size drilled in the sides of the trough, or, at high air ow rates, are forced from underneath the edge of the inverted trough. Since large bubbles are unstable and have a high rise velocity, they are sheared down in size, resulting in bubble diameters of approximately 36 mm with occasional bubble diameters of up to 40 mm. The experimental procedure for all tests followed the ASCE Standard for Measurement of Oxygen Transfer in Clean Water [4]. An air compressor supplied air to the diffuser. A lter system removed oil residue in the compressed air. The delivery pressure was measured with a certied Bourdon gauge and a thermistor was

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0 hr

Distance from diffuser, m

7 6 5

1 hr 2 hr 4 hr 8 hr

4 3 2 1 0 0 0.05 0.1 0.15 0.2 0.25 0.3 0.35 0.4 0.45

Co

*,mol/m3

Fig. 5. Bubble oxygen concentrations for free surface test, Qa 51 scmh. The dashed vertical line is the atmospheric oxygen saturation concentration; the solid diagonal line is the pressure-adjusted oxygen saturation value.

placed in the delivery line to monitor the compressed air temperature. A set of Brooks rotameters provided gas ow measurements. The air ow rate at standard temperature (201C) and pressure (1 atm) was set to approximately 51 or 78 scmh. DO concentrations and temperatures were measured with four air-calibrated Hydrolab MiniSonde 4a multiprobes at various locations in the tank. Air calibration was an important aspect of these tests because all measurements were referenced to a local saturation value, and the DO readings relative to this saturation value were needed [29]. After the data logging systems were initiated, a sodium sulte solution with a cobalt chloride catalyst was used to chemically deoxygenate the water to around 1.0 mg L1 at the start of each test. To distribute the sodium sulte throughout the water column, the chemical was dissolved in a batch tank and pumped into the experimental tank through a perforated manifold. Air ow rate, delivery pressure, and compressed air temperature were recorded periodically during the experiments.

5. Results and discussion 5.1. Bulk mass transfer coefcients In this mass transport model, the gas-phase oxygen composition in the bubbles considers both oxygen and nitrogen transfer. Since y is dened as the ratio of the oxygen concentration inside the bubble to the concentration of nitrogen and other gases inside the bubble, it

is important to maintain a local mass balance by tracking all transfer into and out of the bubble. Air released from the diffuser contains an initial gas-phase oxygen composition (mole ratio) of 0.266. The liquidphase equilibrium concentration inside the bubble at the diffuser is the pressure-adjusted oxygen saturation value before transfer occurs (Fig. 5). At the beginning of a test when the water has been deoxygenated, the high oxygen concentration gradient between the bubble and the ambient water DO causes substantial oxygen transfer out of the bubble, as can be seen in Fig. 5 at time=0 h. At the same time, although the solubility of nitrogen is almost twice that of oxygen, the concentration gradient of nitrogen is signicantly lower. The gas-phase oxygen composition, therefore, initially decreases over depth (Fig. 6). As time continues and the ambient water DO increases, the oxygen concentration gradient lessens. The gas-phase oxygen composition then changes little with depth and time and the liquid-phase equilibrium oxygen concentration at various depths approaches the pressure-adjusted saturation values (Figs. 5 and 6). Co and y also vary with gas ow rate, as shown in Fig. 6. A higher gas ow rate produces more bubbles and therefore more interfacial area for transfer. Since this produces a higher rate of oxygen transfer from the bubbles, the ambient water DO increases more rapidly at a higher gas ow rate. With a smaller concentration gradient between the bubble and the surrounding water, the Co and y values do not decrease as quickly as they do at lower gas ow rates. The mass transport model results are listed in Table 2. The standard error of the DO concentration for the bestt kL ab and kLs as coefcients shows the accuracy of the

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Distance from diffuser, m

7 6 5 4 3 2 1 0 0 0.05 0.1 0.15 0.2 0.25

0 hr, 51 scmh 2 hr, 51 scmh 8 hr, 51 scmh 0 hr, 78 scmh 2 hr, 78 scmh 8 hr, 78 scmh

0.3

Gas-phase oxygen composition,y


Fig. 6. Gas-phase oxygen composition for free surface tests, Qa 51 and 78 scmh.

curve-t. Fig. 7 displays a comparison between measured DO concentrations and values tted by the nonlinear regression for a typical test. The free surface mass transfer coefcients are corrected to a standard reference temperature of 201C by using the model veried for free surfaces by Daniil and Gulliver [30]: kL201C kL Sc1=2 Sc201C
1=2

12

where Sc n=D is the dimensionless Schmidt number, n is the kinematic viscosity of water, and D is the diffusion coefcient of oxygen in water. Eq. (12) provides results that are similar to the Arrhenius relationship with empirical coefcient y 1:0241; but has better theoretical justication [31]. The bubble mass transfer coefcient is corrected by using an indexing relationship for gas transfer in bubbly ows. This indexing equation, developed by Gulliver et al. [32], includes the inuence of temperature on bubble diameter, kinematic viscosity, and molecular diffusivity. The average kL ab value under standard conditions is 0.406 h1 at 51 scmh and 0.756 h1 at 78 scmh. At a higher ow rate, when more bubbles are produced, the bubble mass transfer coefcient is greater. McWhirter and Hutter found a similar rate of increase in kL ab with gas ow rate. The kLs values vary from 266.2 to 437.2 cm h1 with a mean value of 347.7 cm h1. Experiments conducted by different researchers can only be compared loosely due to variations in diffuser type, tank size, and gas ow rate. Neilson reports a kLs value of 15 cm h1 for a perforated line diffuser operating at an air ow rate of 0.069 scmh in a small tank. Wilhelms and Martin

determined a kLs value of 39.6 cm h1 in a mid-sized tank at 1.134 scmh with a exible-head diffuser. The experiments conducted for this research were conducted in a large tank with a coarse bubble diffuser at substantially higher air ow rates of 5178 scmh. The surface experiences greater turbulence and mixing at a higher ow rate, which should produce higher kLs values. McWhirter and Hutter found kLs values from 213.5 to 3048 cm h1 using the Los Angeles County Sanitation Districts data where multiple coarse bubble diffusers were operated at gas ow rates of 213.0 683.4 scmh. Since the experimental setup in the 2001 tests included only one diffuser operating at 5178 scmh, direct comparisons are difcult. The ratio of kLs as =kL ab shows the relative importance of the surface-transfer coefcient with respect to the bubble-transfer coefcient and eliminates the need for temperature adjustment between tests. The primary result of these 9.25 m deep experiments is that the surface-transfer coefcient ranges from 59% to 85% of the bubble-transfer coefcient, with a mean value of 70%. The larger bubble-transfer coefcient reects the dominance of bubble transfer with this type of diffuser. Application of submerged diffusers at deeper depths, say 90 m, would likely have an even smaller ratio since the bubblewater oxygen concentration gradient is signicantly greater than the airwater concentration gradient. The oxygen transfer coefcients, kLs as and kL ab ; however, do not fully describe oxygen transfer because the driving concentration gradient, (Co C ), is also greater for the bubbles. The oxygen mass transfer rate across the bubbles, integrated over depth, and the oxygen mass transfer rate across the free surface is given in Fig. 8 for one test. The positive gas transfer from the

1900 kL as =kL ab

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Std. Error (g m3)

air to the water in the early portions of the experiment becomes a negative transfer as the water concentration passes through the local saturation value. The bubble transfer is larger and is always positive because the bubbles, under pressure, have a high equilibrium concentration in the water phase. 5.2. Sensitivity of transfer coefcients

0.826 0.691 0.853 0.694

0.070 0.055 0.066 0.070

0.672 0.059 0.086 0.065

0.587 0.632 0.637

kL as (1 h1)

A sensitivity analysis shows the numerical importance of the kL ab and kLs as values in obtaining a best-t curve. The sensitivity of the curve-t to specic kL ab and kLs as values can be determined by varying each coefcient from the best-t value and examining the change in standard error. The normalized sensitivity coefcients for bubble and surface transfer are dened as SKs and SKb DSE DkLs as =kLs as DSE : DkL ab =kL ab 13

kLs (cm h1)

0.379 0.373 0.390 0.388

Test conditions

kL ab (1 h1)

0.610 0.592 0.590 0.557

564 0.077 547 545 515

350 345 361 359

14

0.459 0.540 0.457 0.559

0.908 1.008 0.934 0.874

Standard conditions

kL as (1 h )

The ratio of the surface-transfer sensitivity coefcient to the bubble-transfer sensitivity coefcient is dened as RSK SKs =SKb : From Fig. 9, the RSK value is relatively constant within the range of 0.81.2 for 51 and 78 scmh when the kL ab and kLs as values are changed by less than 20%. This means that the standard error is sensitive to both kL ab and kLs as : 5.3. Analysis of surface-transfer coefcient A lake or reservoir will have a surface area that is much greater than the experiments herein. Application of these results to lakes and reservoirs requires a further analysis of the surface-transfer coefcient to differentiate between surface transfer caused by the bubble plume and the transfer across a free surface without a bubble plume. The kLs values determined from these measurements were between 266 and 564 cm h1 (Table 2). These are larger than those measured in lakes and reservoirs without aerators. Donelan and Wanninkhof [33] provide a recent summary of the impacts of wind on gas transfer in a water body. The recorded measurements for wind impact vary from 4 to 64 cm h1, and a measurement of 60 cm h1 requires a wind velocity of roughly 16 m s1. There is, therefore, a one to two order of magnitude difference between the measurements provided herein with an aerator and the literature measurements without an aerator. The tests conducted with Styrofoam slabs covering the water surface except for a 1.8 m diameter hole in the center can be used to further rene the kLs measurements. A comparison of steady-state oxygen

kLs (cm h )

270 266 278 276 0.293 0.288 0.300 0.299 0.370 0.436 0.368 0.450 117.5 119.7 116.4 119.3 7.38 7.32

kL ab (1 h )

Css (%)

Csat (g m )

7.37 30.74 78.15 78 1 FS

Tw (1C)

30.92

31.03

Table 2 Free surface tank test results

Qa (scmh)

51.19

51.14

Test no.

51 1 FS

51 2 FS

78 2 FS

77.14

30.34

7.40

117.6 120.0 119.0 117.7

0.735 0.816 0.762 0.713

0.473 0.459 0.462 0.436

437 424 427 403

C.D. DeMoyer et al. / Water Research 37 (2003) 18901904


0.3

1901

0.25

Dissolved oxygen, mol/m

0.2

Fitted Measured

0.15

0.1

0.05

0 0 1 2 3 4 5 6 7 8 9

Time, hrs
Fig. 7. Fitted versus measured DO concentrations, Qa 51 scmh.

3.50 3.00

Free-surface Bubbles Total

Oxygen transfer rate, g/m3/hr

2.50 2.00 1.50 1.00 0.50 0.00 -0.50 -1.00 0 1 2 3 4 5 Time, hr 6 7 8

10

11

Fig. 8. Oxygen transfer rate from the bubbles and free surface for test, Qa =51 scmh.

concentration values between the covered surface and free surface experiments shows the inuence of oxygen transfer across the water surface outside of the bubble plume. Since the water temperatures during the two sets of experiments varied substantially, the most accurate way to compare the tests is by examining the oxygen concentration as a percent of the local saturation value, set to 100% in the DO probes during air calibration. The steady-state oxygen concentration for the covered surface tests was consistently higher than the free surface

tests by 1.52% of the saturation value (Table 3). When the water surface is covered around the surfacing plume, all oxygen transfer will occur either across the bubble surfaces, or at the highly turbulent plume surface. Since the driving force for bubble transfer is greater than the driving force for surface transfer, Csat ; the steady-state water DO will be higher with a covered surface. Although the bubble mass transfer coefcient is greater at higher ow rates, the surface-transfer coefcient is also greater. Therefore, any dependence of the

1902
1.2

C.D. DeMoyer et al. / Water Research 37 (2003) 18901904

1.1

1 Test 51_1 FS Test 78_1 FS 0.9 Test 51_2 FS Test 78_2 FS 0.8

R SK

0.7

0.6 0.01 0.1 1

kLa/kLa
Fig. 9. Ratio of normalized sensitivity coefcients as a function of fractional change in tted kLa coefcients from best-t coefcients.

Table 3 Comparison of steady-state percent saturation oxygen concentrations Free surface tests Covered surface tests Estimate of kLs distribution under standard conditions Experimentally determined Css (%) 120.7 120.3 120.2 119.9 Above plume (cm h1) 3866 3961 6773 6487 Outside of plume (cm h1) 51 54 47 48

Test no.

Qa (scmh) 51 51 78 77

Experimentally determined Css (%) 118.6 117.9 118.8 118.4

Computed Test no. without surface transfer Css (%) 130.3 130.9 132.4 132.2 51 51 78 78 1 2 1 2 CS CS CS CS

Qa (scmh)

51 51 78 78

1 2 1 2

FS FS FS FS

52 52 77 77

steady-state oxygen concentration on the gas ow rate is weak. The model, with the tted kL ab and kLs as values, can now be used to estimate the liquid lm coefcient of the plume surface, inside of the 1.8 m diameter hole. The free surface tests will be analyzed as if the entire water surface had been covered. At steady state where C -Css ; Eq. (5) can be written Z kL ab C n Css dz kLs as Csat Css 0 15 hd z o and solved for the steady-state oxygen concentration R n kL ab =hd z Co dz kLs as Csat Css : 16 kL ab kL as If surface transfer is considered to be negligible, Z kL ab C n Css dz 0 hd z o

and Css 1 hd Z
z
n Co dz:

18

When the steady-state DO concentration is computed with and without surface transfer, an increase in the steady-state value of approximately 13% occurs when surface transfer is restricted (Table 3). The kLs values for the surface directly over the plume and outside of the plume can now be estimated as follows: kLs plume Css jCS Css jOP As kLs ; Css jCS Css jFS AOP Css jOP Css jFS Css jCS Css jFS As kLs ; As AOP 19

kLs surrounding plume 17

20

C.D. DeMoyer et al. / Water Research 37 (2003) 18901904

1903

where Css jCS is the covered surface calculations with the model and the tted kL ab and kLs as values, Css jOP is the steady-state value from measurements with the 2.6 m2 opening, Css jFS is the steady-state value from measurements with the open free surface, As is the area of the free surface, and AOP is the area of the open plume surface with the Styrofoam cover. The kLs values used were the mean of those given in Table 2 for each test. The results, given in Table 3, indicate that the estimate of surface-transfer coefcients outside of the plume is fairly constant at a mean value of 50 cm h1. Directly above the plume, however, the kLs value increases with air discharge from a mean of 3914 cm h1 at 51 scmh to 6630 cm h1 at 77.5 scmh. These results indicate that the surface transfer estimates above the plume are (1) dependent upon air discharge and (2) substantially higher than those outside of the bubble plume.

systems for lakes, reservoirs, and wastewater treatment facilities at a variety of water depths.

Acknowledgements The experiments described and data presented, unless otherwise noted, were part of research conducted under authority given by the US Army Corps of Engineers DistrictChicago. Permission was granted by the Chief of Engineers to publish this information. The authors thank Jian Peng and Miki Hondzo for their conceptual input into this research and their helpfulness in conducting aeration tests. We also thank Calvin Buie and Jason Giovannettone for assisting with aeration experiments during hot July days in Mississippi.

6. Conclusions The standard testing methodology for oxygen transfer in aerated systems oversimplies the oxygen transfer process and makes adjustment of measured values to other depths intangible. This paper more accurately describes the oxygen mass transfer process and advances McWhirter and Hutters mass transfer model by considering both oxygen transfer and the transfer of other gases, primarily nitrogen, into and out of the bubbles as they rise to the water surface. Model results indicate that the surface-transfer coefcient in a 9.25 m tank with an air ow rate of 5176 scmh is 5985% of the bubble-transfer coefcient. The analysis of the gasphase oxygen composition and liquid-phase equilibrium concentration shows that the bubblewater concentration gradient is also of greater magnitude than the air water concentration gradient. Experiments and analysis designed to determine the relative location of high surface-transfer coefcients indicate that the large transfer coefcient directly above the bubble plume is related to air discharge, while the lower transfer coefcient outside of this region is not related to air discharge. Surface transfer and bubblewater transfer both contribute signicantly to the total oxygen transfer in this type of diffused aeration system. Bubblewater transfer, however, is the dominant means of oxygen transfer. These results were obtained numerically and veried experimentally. The results can be applied to aerated systems at similar depths or to deeper water systems where the higher bubblewater concentration gradient near the submerged diffuser should cause an even greater dominance of bubble transfer in the aeration process. Insight into the relative importance of transfer across the water surface and bubble surface can be used to design more effective diffused aeration

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