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Article history:
Received 10 June 2015
Received in revised form 20 October 2015
Accepted 22 October 2015
Available online 30 October 2015
The application of microwave (MW) radiation followed by aeration (A) for the purpose of ammonia
removal from both synthetic solutions and landll leachate was investigated in this study. 100 mL of
synthetic solution or landll leachate was subjected to MW radiation for 30, 45, 60, 90 and 120 s under
50 and 100% power output level and a pH of 10, 10.5 and 11. The samples were then aerated for 10 min. The
initial, after MW application and nal total ammonia nitrogen (TAN) were measured. Results conrmed
that the sequential microwave/aeration process was an effective approach for removal of ammonia from
aqueous systems. Maximum ammonia removal of 81.7% for 100 mL synthetic solution and 70% for 100 mL
landll leachate was achieved by applying 78 KJ microwave energy output and 10 min aeration. Factorial
design and response surface methodology were applied to evaluate and optimize the effects of pH, MW
energy level and microwave power output. When applying the same energy output to the batch tests, the
effect of varying MW power output is negligible. For 100 mL synthetic ammonia solution, the optimum
pH and MW energy output level for ammonia removal were 11 and 78 KJ and the maximum ammonia
removal efciency predicted for the synthetic solution is 76.3%. R2 of 0.941 indicates that the observed
results tted well with the model prediction.
2015 Elsevier Ltd. All rights reserved.
Keywords:
Ammonia
Microwave
Aeration
Leachate
Factorial design
Response surface methodology
1. Introduction
As one of the major inorganic pollutants in surface water,
ammonia exists in aqueous solution in two forms: un-ionized
ammonia (NH3) and ionized ammonia (NH4+) [1]. It is common in
aquatic chemistry to refer to and express the sum of NH3 and NH4+
as simply ammonia or total ammonia nitrogen (TAN) [2]. Previous
research has shown that toxicity is mainly due to NH3 form [3,4].
The concentration distribution of the ionized and un-ionized
ammonia depends on pH, temperature, and total ammonia
concentration. Under low pH conditions, the majority of TAN is
in the form of NH4+, while under high pH conditions, NH3 becomes
the dominant species [1]. Agricultural drainage and wastewaters
from steel, fertilizer, petroleum, and meat-processing industries
and landll leachate are the main sources of ammonia in natural
water bodies [5]. According to the EPAs fresh water criteria,
ammonia is toxic to aquatic organisms even at low levels (1.9 mg/L
as TAN at 20 C and pH of 7) [6]. Also, discharge of wastewater with
* Corresponding author.
E-mail addresses: msartaj@uottawa.ca, msartaj@yahoo.com (M. Sartaj).
http://dx.doi.org/10.1016/j.jece.2015.10.029
2213-3437/ 2015 Elsevier Ltd. All rights reserved.
101
Table 1
Experimental design of MW processes for the synthetic solution.
MW time (s)
30
45
60
90
120
50
100
50
100
50
100
50
100
50
100
pH
U
U
U
U
U
U
U
U
U
U
U
U
U
U
U
U
U
U
U
U
U
10
10.5
11
102
and hence they were not carried out. For MW + A, the aeration time
was kept at 10 min for all samples. The aeration time was selected
based on another preliminary set of tests.
MW with and without aeration process for landll leachate was
conducted using 50% power output with 120 s radiation time under
three pH levels of 10, 10.5, 11 and 10 min of aeration if applicable.
Fig. 1 presents the order of tests carried out. For the each test,
100 mL of either synthetic solution or leachate was used. pH was
adjusted to desired level using 10 mol/L NaOH solution. The sample
was then exposed to MW radiation for the desired radiation time
according to the conditions presented in Table 1. The sample
temperature was measured immediately after the MW treatment.
Distilled water was used to compensate any water loss. Then, TAN,
pH and temperature of the sample were measured. The sample was
aerated 10 min and TAN, pH and temperature was measured again
after another adjustment for water loss.
C C0
100%
C0
Table 2
Experimental design and the levels of independent process variables.
Independent variable
Symbol
Coded levels
1
0.33
0.33
X1
X2
19.5
10
39
10.5
58.5
78
11
Pt
1000
103
percent removal (Y) were obtained. All the data was evaluated by
DesignExpert1 to detect any outlier and unreliable result. External
studentized residuals were calculated to eliminate the outliers. All
collected data was in the acceptable range to be used to develop the
model. Regression analysis was applied to develop the best-t
model using the collected data. The response ammonia removal
percentage (Y) was predicted by a second-order polynomial
equation shown as Eq. (4) below.
Y 54:49 21:11X 1 3:20X 2 1:65X 1 X 2 1:12X 21 2:07X 22
Fig. 2. Ammonia removal using the same energy output with 50% and 100% of the
total power output under pH of 10 (a), 10.5 (b), 11(c).
104
Table 3
Analysis of variance (ANOVA) for RSM (a) full and (b) reduced quadratic model parameters.
(a)
Source
Sum of squares
df
Mean square
F value
Model
X1
X2
X1X2
13614.64
12442.30
412.49
53.64
14.45
5
1
1
1
1
2722.93
12442.30
412.49
53.64
14.45
197.22
901.18
29.88
3.88
1.05
<0.0001
<0.0001
<0.0001
0.054
0.311
59.90
59.90
4.34
0.042
786.98
165.56
621.42
14401.62
57
6
51
62
13.81
27.60
12.18
2.26
0.052
X 21
X 22
Residual
Lack-of-t
Pure error
Total
R2 = 0.945
R2adj 0:941
Signicant
Not signicant
R2pred 0:933
(b)
Source
Sum of squares
df
Mean square
F value
Model
X1
X2
13546.55
12990.65
496.009
59.90
3
1
1
1
4515.512
12990.65
496.01
59.90
311.57
896.36
34.23
4.13
<0.0001
<0.0001
<0.0001
0.047
Signicant
855.06
233.64
621.42
14401.62
59
8
51
62
14.49
29.21
12.18
2.40
0.028
Signicant
X 22
Residual
Lack-of-t
Pure error
Total
R2 = 0.941
R2adj 0:937
R2pred 0:932
80
Predicted
70
60
50
40
30
20
20
30
40
50
60
70
Actual
Fig. 3. Predicted versus actual values for ammonia percent removal.
80
90
105
Fig. 4. Diagnostics plots for ammonia removal (a) externally studentized residual versus predicted values, (b) externally studentized residual versus run values.
106
107
Fig. 8. Ammonia removal from landll leachate under three different pH levels of
10, 10.5 and 11 using 50% of total MW output for 120 s MW irradiation time.
108
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