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Biosystems and Agricultural Engineering, College of Engineering, Michigan State University, East Lansing, MI 48824, United States
DQY Agricultural Technology Co. LTD, Beijing 100081, China
h i g h l i g h t s
g r a p h i c a l
a b s t r a c t
a r t i c l e
i n f o
Article history:
Received 21 May 2014
Received in revised form
28 September 2014
Accepted 1 October 2014
Available online 15 October 2014
Keywords:
Electrocoagulation
Anaerobic digestion
Biogas purication
Nutrient removal
Water reclamation
a b s t r a c t
A new multiple-stage treatment process was developed via integrating electrocoagulation with biogas
pumping to simultaneously reclaim anaerobic digestion efuent and clean up biogas. The 1st stage of electrocoagulation treatment under the preferred reaction condition led to removal efciencies of 30%, 81%,
37% and >99.9% for total solids, chemical oxygen demand, total nitrogen and total phosphorus, respectively. Raw biogas was then used as a reactant and pumped into the efuent to simultaneously neutralize
pH of the efuent and remove H2 S in the biogas. The 2nd stage of electrocoagulation treatment on the
neutralized efuent showed that under the selected reaction condition, additional 60% and 10% of turbidity and chemical oxygen demand were further removed. The study concluded a dual-purpose approach
for the rst time to synergistically combine biogas purication and water reclamation for anaerobic
digestion system, which well addresses the downstream challenges of anaerobic digestion technology.
2014 Elsevier B.V. All rights reserved.
1. Introduction
Anaerobic digestion (AD) has been proved as a practical and
efcient technology to treat organic wastes (i.e., animal manure,
municipal sludge, and food wastes), and produce renewable energy
Corresponding author at: Department of Biosystems and Agricultural Engineering, Michigan State University, 203 Farrall Hall, East Lansing, MI 48824, United
States. Tel.: +1 517 432 7387; fax: +1 517 432 2892.
E-mail address: liuyan6@msu.edu (Y. Liu).
http://dx.doi.org/10.1016/j.jhazmat.2014.10.009
0304-3894/ 2014 Elsevier B.V. All rights reserved.
484
MSU Dairy Teaching and Research Center, and the food wastes were
from MSU cafeterias. The AD efuent was rst ltered with a 200mesh sieve to remove large-sized chunks. The ltrate was collected
and then diluted with water to an initial total solid (TS) of approximately 1% (w/w). The diluted ltrate as the liquid AD efuent for
this study was collected and stored at 4 C. The characteristics of
the liquid AD efuent were listed in Table 1.
2.2. Experimental setup
A combined EC and biogas pumping unit was established to
carry out the study. The liquid AD efuent was rst treated by an
EC, the liquid portion from the 1st EC treatment was separated and
bubbled by raw biogas, and then a 2nd EC was applied on the biogas treated liquid to reclaim the water (Fig. 1). Another combined
EC process without biogas pumping was also conducted as the
control.
2.2.1. EC setup and operation
DC power supply (XPOWERTM 30 V 3 A) was selected to provide
electricity. Two pairs of steel CRS 1018 were used as electrodes for
both anodes and cathodes (Fig. 1b). Three different effective electrode surface areas of 62 cm2 , 134 cm2 and 210 cm2 were tested.
Rectangular glass containers (effective volume of 500 mL) were
adopted as reactors. PVC holders were placed on the top of the
beakers to hold electrodes in the reactors with 1 cm distance
between electrodes. The electrodes were connected with power
supply and with each other in parallel pattern.
Five hundred milliliter of the liquid AD efuent was used for
individual EC runs. Voltage and power consumption were monitored throughout EC operation via a Kill A WattTM power monitor.
The pH was also measured with FisherTM Scientic pH meter. The
EC treated liquid was separated into three phases of top foaming
layer, middle supernatant, and bottom solid layer. Post-EC treatments described as follow were conducted differently for 1st EC
and 2nd EC.
Post 1st EC treatment: three layers were clearly separated after
the 1st EC treatment. The middle part was siphoned out and stored
at 4 C.
Post 2nd EC treatment: since the middle supernatant was overlapped with the thicker top foaming layer and bottom solid layer,
a mixing and settling process was applied after the 2nd EC. After
30 min settlement, the clear supernatant was collected for nutrient
analysis and removal efciency evaluation.
2.2.2. Biogas pumping setup and operation
500 mL of collected supernatant (middle part) from the 1st EC
was used as the solution. Raw biogas was bubbled into the solution via a pump (GastTM ), and the ow rate was controlled at
Table 1
Characteristics of AD liquid efuent.
Parameters
Value
pH
TS (w/w, %)
TSS (mg L1 )
TDS (mg L1 )
TOC (mg L1 )
Color absorbance (527.5 nm)
Conductivity (s cm1 )
COD (mg L1 )
TP (mg L1 )
TN (mg L1 )
7.58.0
0.90 0.03a
4125b
2035b
2332b
0.718b
4740.7b
9140 140a
340 17.3a
1233 101a
a
b
485
1 vvm (volume gas/volume treated liquid/minutes, the corresponding ow is 0.5 L/min) by an air ow meter from VWRTM . The gas
ow correction factor of the air ow meter to measure biogas ow
is 1.0067, which is calculated based on the specic biogas gravity (1.011) at the operational conditions of 35 C and 5 in. water
pressure. A gas outlet on the top of the bottle and a luer-lock
12 gauge 20 needle submerged in the solution were installed for
releasing biogas and taking biogas and liquid samples, respectively
(Fig. 1(c)). Bubble size was around 1 mm of diameter (based on the
observation from pumping the biogas into the tap water). Liquid
samples were taken every 10 min for pH measurement. Airbags
were used to take gas samples. H2 S concentrations in the original biogas and treated biogas were monitored during the pumping
process.
486
Fig. 2. TS and COD removal ratios of 1st stage EC. * Columns with sparse dots stand
for TS removal, and columns with dense dots stand for COD removal. Blue (left),
red (middle) and black (right) stand for the retention times of 20, 40 and 60 min
respectively. (a) TS and COD removal efciency with electrode surface area of 62 cm2 .
(b) TS and COD removal efciency with electrode surface area of 134 cm2 . (c) TS and
COD removal efciency with electrode surface area of 210 cm2 . * Data represent
the average of three replicates with standard deviation. (For interpretation of the
references to color in this gure legend, the reader is referred to the web version of
this article.)
10000
350
9000
8000
300
7000
250
6000
200
5000
150
4000
3000
100
2000
50
0
1000
0
10
20
30
Time (min)
40
50
60
300
250
200
150
100
50
0
10
11.50
0.14
9.5
0.12
10.50
9.50
0.08
9.00
0.06
pH
10.00
0.10
8.50
0.04
8.00
7.50
0.02
7.00
0.00
20
30
Time (min)
10
20
40
50
60
testing period (Table S1). These results indicated that the conditions
of 60 min and 1 vvm are good for the biogas containing 300 ppm or
less H2 S, but may not be suitable for the biogas with high H2 S content. In-depth studies are needed to further understand the effects
of EC solution and biogas pumping on H2 S removal. Gas analysis
also demonstrated that CH4 content stayed stable during the biogas pumping. CO2 was declined slightly at the beginning of the
biogas pumping, and backed up to the content similar with the
raw biogas (Table S1). There was no signicant amount of NH3
detected in the raw biogas, as well as in the treated biogas (Fig.
S3). Meanwhile, the pH level of the liquid efuent had a substantial
reduction, and a pH of 7.25 was obtained at the end of the biogas
pumping (Fig. 4(b)). The results elucidated that the combined operation not only efciently removed H2 S from biogas as a key step for
biogas purication, but also acidied the solution to facilitate the
following EC process. The H2 S removal of biogas pumping could be
theoretically explained based on the following reactions:
H2 S = HS + H+
2Fe
+ HS = 2Fe
2+
+S +H
40
50
60
40
50
60
8.5
8
7.5
7
10
20
30
Time (min)
(b)
(b)
3+
30
Time (min)
9
pH
11.00
0.16
10
(a)
(a)
12.00
487
350
400
Fig. 4. H2 S and pH change of 1st EC efuent during biogas pumping. Blue square
stands for batch 1, green circle stands for batch 2, red triangle stands for batch 3. (a)
Dynamic change of H2 S concentration. (b) Dynamic change of pH. (For interpretation
of the references to color in this gure legend, the reader is referred to the web
version of this article.)
NBP efuent
BP efuent
0.5 0.1
1000 140a
801b
277.0 54.1a
2986.5c
0.6 0.1a
1873 23a
777b
308.0 14.2a
4893.2c
488
60.0
0.14
Energy Consumption (kwh/L)
70.0
Turbidity removal %
50.0
40.0
30.0
20.0
10.0
0.0
0.5A 20min 0.5A 40min
0.12
0.10
0.08
0.06
0.04
0.02
1A 20min
1A 40min
Treatments
2A 20min
0.00
0.5A, 20min 0.5A, 40min
2A 40min
1A, 20min
1A, 40min
Treatments
2A, 20min
2A, 40min
(a)
(a)
70.0
11
60.0
10
9
40.0
pH
COD removal %
50.0
30.0
20.0
10.0
0.0
0.5A, 20min 0.5A, 40min 1A, 20min 1A, 40min
Treatments
2A , 20min
2A, 40min
5
0.5A, 20min 0.5A, 40min
1A, 20min
(b)
Fig. 5. Comparison of COD and turbidity removal between no-biogas-pumped (NBP)
and biogas pumped (BP) after 2nd EC. * Light blue square (left) stands for NBP,
red square (right) stands for BP. (a) Turbidity (b) COD removal. *Data represent
the average of three replicates with standard deviation. (For interpretation of the
references to color in this gure legend, the reader is referred to the web version of
this article.)
1A, 40min
Treatments
2A, 20min
2A, 40min
(b)
Fig. 6. Comparison of power consumption and pH between no-biogas-pumped
(NBP) and biogas pumped (BP) after 2nd EC. * Light blue square (left) stands for
NBP, red square (right) stands for BP. (a) Power consumption, (b) pH. *Data represent the average of three replicates with standard deviation. (For interpretation of
the references to color in this gure legend, the reader is referred to the web version
of this article.)
Table 3
Characteristics of the treated solutions from two-stage EC with NBP and BP.a , b , c
Parameter
Two-stage EC
with NBP
Two-stage EC
with BP
TSS (mg L1 )
TDS (mg L1 )
TOC (mg L1 )
Color absorbance (at 527.5 nm)
COD (mg L1 )
TN (mg L1 )
Turbidity (NTU)
Conductivity (s cm1 )
ND
2574
60
0.085
513.3 46.0
443.3 56.9
144.2 20.4
4778.8
168
2106
101
0.082
808.7 116.1
655.2 5.9c
113.6 6.8
3939.9
a
NBP treatment was carried on at I of 2 A and RT of 40 min, and BP treatment was
carried on at I of 1 A and RT of 40 min.
b
Data represent the average of three replicates with standard deviation.
c
The number was from the run at I of 2 A and RT of 40 min.
489
Fig. 7. Turbidity and color change of the solution during electrocoagulation processes. (a) Left to right: AD efuent, solution after 1st EC, supernatant after 2nd EC. (b) Left to
right: AD efuent, solution after 1st EC and biogas pumping, supernatant after 2nd EC. (For interpretation of the references to color in this gure legend, the reader is referred
to the web version of this article.)
Table 4
Comparison of the selected multiple-stage EC processes with BP and NBP.
Parameter
Two-stage EC
with NBPc
Two-stage EC
with BPd
94.3 0.5
>99.9
64.7 6.3
>99.9
97.4
88.2
54.9 1.5
0.25
91.0 1.3
>99.9
46.9 0.5c
95.9
95.7
88.6
34.0 6.5
0.16
a
Removal was calculated based on unit volume of solution. Data represent the
average of three replicates with standard deviation.
b
Recovery was calculated based on the volume of the initial solution. Data represent the average of three replicates with standard deviation.
c
This set of data was derived from 2nd EC with I of 2 A and RT of 40 min.
d
This set of data was derived from 2nd EC with I of 1 A and RT of 40 min.
e
Data represent the average of two replicates.
Table 5
Mass balance analysis.
Volume (mL)
TNa (mg)
TPa (mg)
Feb (mg)
AD efuent
Electrodes loss
1st EC sludge & other loss
1st EC solution
500
196.7 5.8
303.3 5.8
616.7 50.3
344.2 62.4
272.5 48.3
170 8.7
170 8.7
0
19.4
2100
2017.8
101.6
1.0
100
79.1
37.9
1st EC solution
Electrodes loss
2nd EC sludge & other loss
2nd EC solution
500
47.8 1.9
452.2 1.9
400.5 2.1
182.4 14.8
218.1 48.3
142.8
1333.3
1473.0
3.2
6.7
57.7
59.1
0.5
1st EC solution
Electrodes loss
2nd EC sludge & other loss
2nd EC solution
500
68.3 7.1
431.7 7.1
388.5 61.5
105.7 35.4
282.8 7.1
135
633.3
741.6
26.7
11.3
115.5
110.3
8.1
Mass balance
1st EC stage
Input
Output
2nd EC
stage with
NBPc
2nd EC
stage with
BPc
a
b
c
Input
Output
Input
Output
Data represent the average of three replicates with standard error; TP data are average of two replicates.
Data are from EC treatments on a different batch of AD efuent, and represented the average of three replicates with standard error.
2nd EC condition for NBP group was 2 A of I and 40 min of RT; 2nd EC condition for BP group was 1 A of I and 40 min of RT.
S (mg)b
3.8 0.1
490
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