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Performance Comparison of Phenol Removal in Pharmaceutical Wastewater by Activated Sludge and Extended Aeration Augmented With Activated Carbon
Performance Comparison of Phenol Removal in Pharmaceutical Wastewater by Activated Sludge and Extended Aeration Augmented With Activated Carbon
H O S T E D BY
Alexandria University
a
Civil Engineering Department, AL-Qalam University Collage, Kirkuk, Iraq
b
Sanitary Engineering Department, Faculty of Engineering, Alexandria University, Lotfy El-Sied st. off Gamal Abd El-Naser –
Al Azaritah WA Ash Shatebi – Qesm Bab Sharqi, Alexandria 03 5910052, Egypt
KEYWORDS Abstract This study investigated the removal of phenol, Chemical Oxygen Demand (COD), and
Pharmaceutical; ammonia from pharmaceutical wastewater using activated sludge (AS) and extended aeration
Phenol; (EA) systems. Also, the impact of adding activated carbon media on the performance of the two
Chemical oxygen demand; systems has been studied. Synthetic sewage was used with a composition of COD equaling
Activated sludge; 1500 mg/L. The experimental work was divided into five scenarios for the two reactors based on
Extended aeration; the Phenol concentration, 0.0 mg/L in the first scenario, 50.0 mg/L in the second and third scenar-
Activated carbon ios, but activated carbon has been added to the third one. The concentration of Phenol was
100.0 mg/L and 150.0 mg/L for the fourth and fifth scenarios, respectively. The experimental results
indicated that EA system gives higher removal efficiency than that by AS system for COD, phenol,
and ammonia. In addition adding activated carbon of just 1.0 gm/L of the working reactor volume
in both systems (AS, EA) has improved the removal efficiency. GPS-X simulator was employed to
predict the performances of the biological systems under high effluent concentration of COD reach-
ing up to 19000 mg/L. The simulation results indicated that EA effluent could comply with Egyp-
tian Cod (Law no 44/2000).
Ó 2020 The Authors. Published by Elsevier B.V. on behalf of Faculty of Engineering, Alexandria
University. This is an open access article under the CC BY-NC-ND license (http://creativecommons.org/
licenses/by-nc-nd/4.0/).
1. Introduction
of organic solvents, catalysts, raw materials, and reaction COD, color, ammonia nitrogen, and total dissolved salts com-
intermediates which make their treatment procedure compli- pared with the control biological technology [23]. Jaafarzadeh
cated [1–3]. The presence of toxic or recalcitrant substances et al. (2010) also employed the conventional AS process with
in such wastewater results in lower Chemical oxygen demand and without the addition of PAC to treat pharmaceutical
(COD) removal efficiencies [4]. Physio-chemical processes such wastewater. Results showed that the addition of PAC could
as enhanced coagulation and electrochemical processes have remove antibiotic compounds and subsequently enhance the
been demonstrated to treat such wastewater effluents (Journal removal efficiencies compared with the situation without
of Environmental Chemical Engineering, 2013, Journal of PAC addition [24].
Water Process Engineering, 2020) [5,6]. Biological treatment El-Gohary et al. (1995) revealed that with an extended aer-
methods have traditionally been used for the management of ation period of 20 h COD and BOD removal efficiency of 89–
pharmaceutical wastewater [7]. They may be subdivided into 95% and 88–98%, respectively, can be achieved. The COD
aerobic and anaerobic processes. Aerobic applications include and BOD values of the treated effluent were found to be
activated sludge, membrane batch reactors and sequence batch 74.0 mg/L and 43.0 mg/L, respectively [12]. Besides Mowla
reactors [7–11]. Conventional activated sludge with a long et al. (2014) investigated the performance and effectiveness
hydraulic retention time (HRT) has historically been used of sonophotolytic process, aerobic activated sludge (AS) pro-
for the treatment of pharmaceutical industry wastewater cess, and their combination in the reduction of total organic
[12,13]. It has a lower capital cost than more advanced treat- carbon (TOC), COD, and BOD from a synthetic pharmaceu-
ment methods and a limited operational requirement; it is gen- tical wastewater (SPWW). 90% of TOC reduction was
erally more environmentally friendly than chlorination. obtained in the sonophotolytic process after 180 min retention
During chlorination, the chlorinated organic compounds and time, whereas only 67% in an aerobic AS process for retention
pharmaceutical compounds present in effluents are formed. time of 48 h. Combining sonophotolytic and aerobic AS pro-
These compounds are serious concerns. But in the biological cesses improved the biodegradability of the SPWW with a
technology, the organic and inorganic contaminants change 98% and a 99%removal of TOC and COD, respectively with
into gases and digested sludge that can be the safely disposed. a retention time reduction in sonophotoreactor and aerobic
However, high energy consumption, the production of large AS bioreactor to 120 min and 24 h, respectively [25].
amounts of sludge [3], and operational problems including Khan et al. (2011) designed A lab scale batch plant (inte-
color, foaming and bulking in secondary clarifiers are associ- grated aerobic biological treatment) aimed to minimize and
ated with activated sludge plants [13]. Factors which affect removing suspended solids, dissolved solids, nutrients, and
the efficiency of activated sludge facilities for the treatment toxic compounds from pharmaceutical wastewater. The maxi-
of pharmaceutical wastewater include HRT, temperature, mum hydraulic retention time was 15 days. About 75%
pH, dissolved oxygen (DO), organic load, microbial commu- removal of COD was achieved employing hydraulic retention
nity, presence of toxic or recalcitrant substances, and the batch times of 15 days. The analysis of the treated wastewater reveals
operation of pharmaceutical production facilities [7,11,14]. that the parameters pH, BOD, COD, TSS, TDS, and color
These variables require modification for adaptation of phar- were found within the prescribed permissible limits indicating
maceutical industry wastewater treatment. the efficiency of the treatment. The results of this study demon-
Phenolic compounds are one of the main components of strate the potential for air injection to accelerate the biological
anti-pruritic, anti-inflammatory, analgesic and blemish treatment process, with the greatest influence on COD removal
removal pharmaceuticals. A large amount of utilized phenolic from the wastewater [26]. Wang et al. (2020) investigated the
compound caused phenol contamination in environment treatment of pharmaceutical wastewater by moving bed bio-
including municipal and industrial wastewater treatment sys- film reactor (MBBR) and total reflux sludge reactor process
tems [15,16]. The contamination from pharmaceutical uses (STR) system. By cultivating specific bacterial groups, optimiz-
and pharmaceutical production could be up to milligram per ing reactor process parameters, and comparatively analyzing
liter level [15]. Although the wastewater treatment systems the pollutant removal efficiency under stable operating condi-
could be able to remove phenolic compounds, these toxic com- tions of the system, the treatment efficiency of the two systems
pounds at high concentrations significantly inhibited the under the combined impact load of organic pollutants on the
wastewater treatment performance [16,17]. However, several target pollutants indole and naphthalene was studied. The
processes are affordable for the high toxicity of the effluent. results of this research found that the MBBR process has a
Granular activated carbon adsorption and its derivative by a stronger treatment effect on pharmaceutical wastewater than
conventional process representing an environmentally friendly the STR system during the stable period and the impact load
alternative phenolic [18]. stage [27].
Activated carbon adsorption is an effective chemical– phys- To the best of our knowledge, no published work has been
ical treatment technology widely used in the treatment of emphasized on comparison of phenol removal efficiency in
industrial wastewater and potable water [19–21]. Most organic pharmaceutical wastewater treatment between activated sludge
components inside water can be strongly adsorbed into acti- and extended aeration augmented with activated carbon.
vated carbon because of a well-suited surface and micro pores Therefore, this work aims to investigate the performance and
[22]. Some researchers have applied powdered activated car- treatment capability of activated sludge and extended aeration
bon (PAC) into the activated sludge (AS) process to improve systems under normal operation and after adding phenol
the performance of biological treatment. Aziz et al. (2011) beside studying the effect of added Granular Activated Carbon
investigated the performance of a PAC–AS system in a to improve removal efficiency. Also, using GPS-X simulator to
sequencing batch reactor to treat landfill leachate. The system predict the performance of the two reactors at different feed
displayed superior performance in the removal efficiencies of compositions.
Performance Comparison of Phenol Removal in Pharmaceutical Wastewater by Activated Sludge and Extended Aeration Augmented with Activated Carbon 5189
2. Material and methods into five scenarios for each reactor to evaluate the perfor-
mance of the treatment under different concentrations of phe-
2.1. Experimental set-up nol and the feasibility of adding granular activated carbon in
the two reactors. Fig. 2 illustrates a schematic diagram of the
experimental scenarios. The Phenol concentration in the first
The experimental set-up used in this study was a BIOTEST
scenario was 0.0 mg/L, while it was 50.0 mg/L in the second
unit located at the laboratory of Sanitary Engineering Depart-
and third scenarios with addition of activated carbon in the
ment, Faculty of Engineering, Alexandria University. The unit
third scenario. The Phenol concentration in the fourth and
has been run for the two reactor systems; the first was Conven-
fifth scenarios was 100.0 and 150.0 mg/L, respectively. Sam-
tional Activated Sludge and the second was Extended Aeration
ples were collected daily from the feed and effluent streams
Activated sludge. Fig. 1 illustrates a schematic diagram of the
and analyzed to evaluate the performance of the two
experimental set-up that consists of two basins; the first was
reactors.
the aeration tank (diameter = 19.0 cm and depth of
During the startup period, both Activated Sludge and
water = 37.0 cm) with a total volume of the 9.0 L and the sec-
Extended Aeration systems were seeded with a wastewater
ond was operated as a final settling tank (diameter = 19.0 cm,
from the aeration tank of El-dekheela wastewater treatment
depth of water = 18.0 cm, and height of cone = 17.0 cm). The
plant up to reaching steady state conditions. The effluent
set-up also connected with a control unit that contains the ON-
COD concentration stability was used as a primary indicator
OFF switch, air pump, flow meter to regulate the flow rate,
of steady state conditions. After that the two reactors were
feeding pump, and returning pump for recycling the sludge
fed with the prepared synthetic sewage and the systems were
from settling tank. The aeration tank was fed by the synthetic
run based on the experiment scenario. The length of each sce-
sewage by a feed pump at a continuous and constant flow rate.
nario was set at 8 days and the two reactors were cleaned and
Then the treated wastewater entered the settling basin for
operated as a startup period after each scenario.
sludge removal. Part of the removed sludge had been pumped
back to the aeration basin to improve the system biodegrad-
2.5. Measurements and analysis methods
ability. Table 1 shows the operation condition of the two
systems.
All experimental measurements in steady state operation and
2.2. Pharmaceutical industry wastewater characteristics batch tests for system were determined by using standard
methods for the examination of water and wastewater [30].
The measured parameters were Phenol, COD, soluble ammo-
In this study, a synthetic sewage was used as influent wastew-
nia nitrogen (NH3-N), Nitrate nitrogen (NO3-N).
ater for AS and EA reactors and was prepared according to
The chosen techniques and calculations for the determina-
Battistoni et al. (1993). A stock solution was prepared by add-
tion of parameters are described below:
ing 120 g of glucose (C6H12O6, 99% – Manufactory leading
worldwide chemicals companies), 34.95 g of hydrous sodium
Phenol measurements
phosphate (Na3PO412H2O, 99% – manufactory ALPHA
CHEMIKA), and 24.6 g of ammonium sulfate ((NH4)2SO4,
In this test the sample is mixed with 0.5 N of NH4OH solu-
98.5% – manufactory El Nasr Pharmaceutical Chemicals
tion and immediately adjusted to pH of 7.9 ± 0.1 with phos-
Company) in 1.0 L of tab water. . . Then the stock solution
phate buffer, and 4-aminoantipyrine solution, and K3Fe(CN)6.
was diluted with tap water (1:100) and was daily prepared
After 15 min, the sample has been transferred to the cell and
fresh to keep the COD for the influent approximately constant
read absorbance of sample and standards against the blank
at 1500 mg/L, NH4-N = 75 mg/L, and the ratio between
at 500 nm. Estimate sample phenol content from photometric
COD:N:P of 100:5:1. The characteristics of typical pharmaceu-
reading by using a constructed calibration curve.
tical industry wastewater are shown in Table 2.
A
Mg phenol=L ¼ 1000
2.3. Granular activated carbon specification B
where
Table 3 presents the specification and the properties of granu-
lar activated carbon used in this study which is a highly eco- A = mg phenol in sample, from calibration curve
nomical, medium activity produced by vapor activation of B = mL original sample
chooses degree of bituminous coal. The ideal balance between Chemical Oxygen Demand (COD)
adsorption and transport pore supplies optimal performance
in a wide range of water treatment applications. The amount The chemical Oxygen Demand (COD) is used as a measure
of active carbon, which has been placed in the aeration tank, of the oxygen equivalent of the organic matter content of a
is1.0 gm/L. sample that is susceptible to oxidation by strong chemical oxi-
dant. It measures those organic materials that can be oxidized
2.4. Experimental scenarios by a strong chemical oxidizing agent as potassium dichromate.
The units of measurement of COD are in terms of mg/L of
To achieve the objectives of this research, two pilot units oxygen involved in the oxidation reaction.
were operated in parallel; the first reactor was Conventional In this test, the sample is mixed with sulfuric acid (H2SO4),
Activated Sludge and the second reactor was Extended Aer- silver sulfate (Ag2SO4) reagent and potassium dichromate oxi-
ation Activated Sludge. The experimental work was divided dizing agent (K2Cr2O7). The mixture is then refluxed (boiled
5190 B.M. Mareai et al.
Table 1 The operation conditions of the two systems. Table 3 Properties of media GAC.
Operation Condition Conventional Extended Parameter Value
Activated Sludge Aeration
Iodine number Min. 850 mg/g
Influent flow rate (L/d) 16 4.5 Humidity Max. 5%
Return sludge flow rate (L/d) 8 4.5 The total ash content Max. 15%
Detention time in the aeration 9 24 Wettability Min. 95%
tank (hr) Hardness Min. 95%
Volume of the tank (L) 9 9 Surface area 900 m2/g
The range of dissolved oxygen in 1–3 2–6 Methylene blue number 200 mg/g
the aeration tank (mg/L) Total pore volume 0.88 cm3/g
Water soluble ash 0.2%
Ostensible density 510 kg/m3
pH 8–11
inhibit the action of microorganisms especially when the Activated sludge Extended aeration
wastewater is not rich in all nutrients required for the growth 100 97.87
mg/L
50
40
30
20
10
0
1 2 3 4 5 6 7 8
Time (day)
Fig. 6 Concentration of phenol effluent at different phenol scenarios for AS.
90
80
70
60
mg/L
50
40
30
20
10
0
1 2 3 4 5 6 7 8
Time (day)
100
NH3 effluent (mg/L)
20 5
0 0
50 50 + A.C 100 150 0 50 50 + A.C 100
Phenol influent concentration (mg/l) Phenol influent concentration (mg/L)
Fig. 8 Comparison between AS and EA according to the phenol Fig. 9 Comparison between AS and EA according to concen-
removal efficiency for different phenol scenarios. tration of NH3-N effluent for different phenol scenarios.
additional removal of nitrogen compounds by having advan- plant in Fig. 11 consist two stages, first is aeration tank and the
tages of both biodegradation and adsorption [35]. second is finally clarifier tank. Table 4 shows model calibration
used for both AS and EA plants. The systems plant was mod-
4. Modelling and simulations elled by using the GPS-X version 5.0 programs.
4.1. Plant configuration and operation conditions 4.2. Activated Sludge Model No. 1 (ASM1)
Simulations were performed on the two reactors (AS and ES) A model is a simplified representation of what occurs in reality
using modular program GPS-X with the aim to know the per- and they are also useful for process optimization and control.
formance of AS and EA under different conditions. The model The Model is defined by a series of mathematical equations
5194 B.M. Mareai et al.
6
model for both AS and EA plants.
5 4.23 4.12
4 3.38
3.69 Parameter Concentrations (mg/L)
2.89 2.64
3 BOD5 1050
1.8
2 Total SS 20
1 TKN 56
0
0 50 50 + A.C 100
Phenol influent concentration (mg/L)
AS experimental AS simulation EA experimental EA simulation 5. Based on the data obtained from GPS-X model, increasing
120 the flow rate in activated sludge system increase the effluent
COD effluent (mg/L)
2000
1647
financial interests or personal relationships that could have
1500 1183 1126 appeared to influence the work reported in this paper.
1000
577
433.5
500 219.8 215.5 References
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