applied

sciences
Article
Influence of Ammonia Stripping Parameters on the Efficiency
and Mass Transfer Rate of Ammonia Removal
Eun Ju Kim , Ho Kim and Eunsil Lee *

Center for Plant Engineering, Institute for Advanced Engineering, Yongin-si 17180, Korea; [email protected] (E.J.K.);
[email protected] (H.K.)
* Correspondence: [email protected]

Abstract: This study analyzed the influence of different ammonia stripping parameters on ammonia
removal efficiency and mass transfer rate. Ammonia stripping was performed on two devices,
a column and a packed tower, with artificial ammonium hydroxide wastewater. First, ammonia
concentration and pH were varied in a column without liquid circulation. At the same pH, the
removal efficiency and mass transfer rate were constant, irrespective of initial ammonia concentration.
When pH was increased, the ammonia fraction also increased, resulting in higher removal efficiency
and mass transfer rate. Second, the effects of stripping were assessed using a packed tower with
fluid circulation. The ammonium hydroxide concentration did not affect the removal efficiency or
mass transfer rate. Furthermore, at apparatus liquid-gas ratios of 26.8–107.2 L/m3 , a lower liquid-gas
ratio led to increased ammonia removal efficiency and mass transfer rate. Conversely, the lower the
liquid-gas ratio, the greater the air consumption. In conclusion, considering the removal rate and
volume of air supply, the range of optimal liquid-gas ratio was determined as 26.8–53.6 L/m3 . In
particular, the 26.8 L/m3 condition achieved the best ammonia removal rate of 63.0% through only 6
h of stripping at 70 ◦ C and pH 8.5.



Keywords: wastewater treatment; nitrogen removal; ammonia stripping; air stripping; stripping tower



Citation: Kim, E.J.; Kim, H.; Lee, E.

Influence of Ammonia Stripping
Parameters on the Efficiency and
1. Introduction
Mass Transfer Rate of Ammonia
Removal. Appl. Sci. 2021, 11, 441.
With industrial development and population growth, there has been a rapid increase
https://doi.org/
in the amount of wastewater containing ammonia from various sources, including sewage
10.3390/app11010441 sludge, cattle excrement, food waste, and biomass [1]. Ammonia containing wastewater is
also generated in the energizing process of waste resources [2,3]. Ammonia in wastewater
Received: 10 November 2020 should be removed because it causes eutrophication and ecotoxicity when it leaks into
Accepted: 31 December 2020 ecosystems [4,5].
Published: 5 January 2021 There are various methods for removing ammoniacal nitrogen from solution, including
physical, electronic, and biological methods. Ammonia stripping is a particularly efficient
Publisher’s Note: MDPI stays neu- method for ammonia recovery from high concentration wastewater [6,7], In ammonia
tral with regard to jurisdictional clai- stripping system, ammoniacal nitrogen is removed as a gas by supplying gas such as air
ms in published maps and institutio- or steam [6–9]. The reactor is usually a fixed-bed column or packed bed tower [6–9]. In
nal affiliations. tower-type reactors, ammonia mass transfer is achieved by gas-liquid contact within the
packing material [10]. Therefore, the liquid-gas ratio should be carefully considered to
optimize the operating conditions of packed towers.
Copyright: © 2021 by the authors. Li-
In this regard, substantial research and development have focused on the operating
censee MDPI, Basel, Switzerland.
conditions and other factors affecting stripping towers for different types of wastew-
This article is an open access article
ater [11–16]. For example, Ferraz et al. [12] performed ammonia stripping from land-
distributed under the terms and con- fill leachate using a packed tower at room temperature and pH 11 and achieved a re-
ditions of the Creative Commons At- moval efficiency of 98% after 24 h of stripping at a liquid-gas ratio (L/G) of 6.7–20 L/m3 .
tribution (CC BY) license (https:// Guštin et al. [13] used a continuous flow packed tower to strip ammoniacal nitrogen from
creativecommons.org/licenses/by/ anaerobic digestate at a liquid-gas ratio of 2.5 L/m3 , achieving a removal efficiency of 55%
4.0/). at 50 ◦ C and pH 10. Liu et al. [14] evaluated the ammonia removal efficiency and rate

Appl. Sci. 2021, 11, 441. https://doi.org/10.3390/app11010441 https://www.mdpi.com/journal/applsci

Appl. Sci. 2021, 11, 441 2 of 13

for the urine with temperature, pH, concentration, and liquid-gas ratio. Zhu et al. [15]
and Li et al. [16] also analyzed ammonia removal rate by temperature, pH and air supply
condition.
Conventional ammonia stripping processes are typically performed at a temperature
between room temperature and 50 ◦ C and in a pH range of 10–12 [11–16]. These process
require a large amount of reagents to adjust the pH [13,17]. In the ammonia stripping
process, a basic reagent is used to increase the pH. After ammonia removal, the pH must
be adjusted to neutral for wastewater treatment and discharge. One method for reducing
the use of these reagents is high-temperature stripping; at a high temperature, the same
removal efficiency can be achieved with a smaller quantity of reagent [17]. Although
there is a problem that a heat is required for high-temperature stripping, the heat energy
consumption can be minimized by using waste heat. For example, the hydrothermal
thermal carbonization (HTC) reaction is carried out at 180–260 ◦ C [18,19], and it is possible
to raise the temperature of the HTC wastewater up to 70–80 ◦ C by using HTC heat. In
addition, the high-temperature process can be operated more economically by reducing
the air supply [8].
The purpose of this study is to design a high-temperature stripping tower and derive
the optimal operating factors that will reduce the use of reagents and air supply while
maintaining the ammonia fraction at an operating temperature of 70 ◦ C. To this end,
the ammonia removal efficiency and mass transfer coefficient are assessed at different
temperatures, pH, ammonium hydroxide concentration, and airflow volume. Specifically,
by deriving the optimal liquid-gas ratio and air supply volume for efficient liquid-to-gas
contact in the packing layer, this study provides useful data on the key factors in the design
of high-temperature ammonia stripping devices.

2. Theoretical Considerations
2.1. Ammonia–Water System
In aqueous solution, total ammonia exists as both free ammonia (NH3 ) and ammonium
ions (NH4+ ), as shown in Equation (1), and the water is dissociated into ions, as shown in
Equation (2) [10].
NH3 + H2 O ↔ NH4+ + OH − , (1)
H2 O ↔ H + + OH − , (2)
The total ammonia concentration in the solution is expressed by Equation (3).

[ NH3,L ] T = [ NH3,L ] + NH4+ ,

 
(3)

where [ NH3,L ] T , [ NH3,L ], and NH4+ mean the molar concentration (mol/L) of total
 

ammonia, free ammonia, and ammonium ion, respectively.

The ionization constants for water (K H2 O ) and ammonia (K NH3 ) are known in Equations (4)
and (5), respectively.
K H2 O = H + OH − ,
  
(4)
NH4+ [OH − ]
 
K NH3 = , (5)
[ NH3,L ]
where [ H + ] and [OH − ] are the molar concentration (mol/L) of hydronium ion and hydrox-
ide ion, respectively.
In addition, the ionization constants are expressed as a function of absolute tempera-
ture (K), as shown in Equations (6) and (7) [6,10,11,20].

ln K H2 O = 140.932 − 13445.9/T − 22.4773 ln T, (6)

ln K NH3 = 97.976 − 5930.7/T − 15.063 ln T − 0.01127T, (7)

Appl. Sci. 2021, 11, 441 3 of 13

2.2. Ammonia Stripping

In aqueous solution, the free ammonia can be stripped through transfer from liquid to
gas. Thus, the concentration ratio of the free ammonia to total ammonia is a major factor in
stripping and is defined as the ammonia fraction ( f NH3 ) in Equation (8) [13].

[ NH3,L ]
f NH3 = , (8)
[ NH3,L ] + NH4+


The ammonia fraction is also expressed by Equation (9) from Equations (4) and (5).

K H2 O 1
f NH3 = = , (9)
+ 1 + K NH3 /K H2 O ·10− pH


K H2 O + K NH3 [ H ]

Since the ionization constants is described as a function of absolute temperature in

Equation (6), the ammonia fraction is dependent on both temperature and pH.
The percentage of ammonia removal (η) is calculated as the amount of ammonia
removed compared to the initial ammonia and is expressed as Equation (10):

[ NH3,L ]0T − [ NH3,L ]tT

η= , (10)
[ NH3,L ]0T

2.3. Mass Transfer of Ammonia

In the process of ammonia stripping, the mass transfer rate of ammonia (FNH3 ) from
liquid to gas phase is given by Equation (11) [14,21,22].

[ NH3,L ] T
FNH3 = VL , (11)
dt
where t is time and VL is the total volume of liquid.
In a batch reactor, the mass transfer rate for liquid ammonia to gas is defined by
Matter-Mueller, as shown in Equation (12) [14,22]:
 
K L, NH3 aVL

FNH3 = QG HNH3 [ NH3,L ] 1 − exp − , (12)
QG HNH3

where QG is the gas flow rate and HNH3 is the dimensionless Henry’s law constant. K L, NH3
is the mass transfer coefficient of liquid ammonia. The interfacial area per unit volume
between liquid and gas is indicated by a.
Combining Equations (8), (10) and (12) and integrating the total ammonia concentra-
tion over time gives Equation (13):

[ NH3,L ]tT QG HNH3 f NH3 K L, NH3 aVL

  
− ln = 1 − exp − t, (13)
[ NH3,L ]0T VL QG HNH3

The slope for the logarithm of ammonia concentration ratio over time is then given by
Equation (14):
QG HNH3 f NH3
 
K L, NH3 aVL

slope = 1 − exp − , (14)
VL QG HNH3
From Equations (13) and (14), the overall mass transfer coefficient for liquid ammonia
to gas is calculated as follows:

[ NH3,L ]tT
( !)
QG HNH3 VL
K L, NH3 a = − ln 1 + ln , (15)
VL QG HNH3 f NH3 t [ NH3,L ] T 0
Appl. Sci. 2021, 11, 441 4 of 13

QG HNH3
 
VL
K L, NH3 a = − ln 1 − × (slope) , (16)
Appl. Sci. 2021, 11, x FOR PEER REVIEW VL QG HNH3 f NH3 4 of 13
The main variables in ammonia stripping are the ammonia fraction, the rate of change
in the ammonia concentration, the volume of gas supplied, and the overall mass transfer
coefficient accordingaccording
transfer coefficient to the typeto of
thereactor
type ofasreactor
shownasinshown
Equations (12) and (12)
in Equations (14).and
Hence,
(14).
inHence,
this study,
in thiswe analyzed
study, the effectthe
we analyzed ofeffect
the major
of thestripping factors—ammonia
major stripping concentra-
factors—ammonia con-
tion, fractionfraction
centration, and gasand
flowgas
rate—on the ammonia
flow rate—on removal efficiency
the ammonia and massand
removal efficiency transfer
mass
coefficient.
transfer coefficient.
3. Materials and Methods
3. Materials and Methods
3.1. Preparation
3.1. Preparation
In this study, air stripping experiments were conducted and stripping factors were
In this
evaluated forstudy,
high air stripping
ammonia experimentswastewater
concentration were conducted
such and stripping
as HTC factors were
or anaerobic liq-
evaluated for high ammonia concentration wastewater such as HTC
uids [1–4,18,19,23]. These wastewaters contain ammonia up to 4000 mg/L [1,3,4]. or anaerobic liquids
To
[1–4,18,19,23].
simulate These
artificial wastewaters
wastewater, contain
1000–3700 ammonia
mg/L ammoniaup to 4000 mg/L
solution was [1,3,4].
preparedToby
simulate
dilut-
artificial
ing wastewater,
a 28–30% ammonia1000–3700 mg/L ammonia
solution (SAMCHUN) solution
with was prepared
tap water. by diluting
To evaluate a 28–
the physical
30% ammonia
degassing solution
properties of (SAMCHUN)
ammonia, thewith tapon
effects water.
traceTo evaluateofthe
amounts physical
nitrate, degassing
nitrite were
properties
excluded. of ammonia, the effects on trace amounts of nitrate, nitrite were excluded.

3.2.Stripping
3.2. StrippingColumn
Column
AAcolumn-type
column-typeammonia
ammoniastripping
strippingdevice
devicewas
wasconfigured
configuredasasshown
shownininFigure
Figure1.1.The
The
capacityofofthe
capacity thecolumn
columnwas was22L,L,and
andaadisk-type
disk-typeair
airdiffuser
diffuserwas
wasinstalled
installedatatthe
thebottom,
bottom,
through
throughwhich which external
externalairair
could be supplied.
could The The
be supplied. air required for stripping
air required was controlled
for stripping was con-
attrolled
a pressure ≤
at a pressure of ≤30 Pa using a blower and regulator, and a flow meter wascontrol
of 30 Pa using a blower and regulator, and a flow meter was used to used to
the volume.
control To control
the volume. Tothe pH ofthe
control thepH
solution, NaOH solution
of the solution, NaOH was supplied
solution using an auto
was supplied using
titration
an autosystem (905
titration Titrando,
system (905 Metrohm
Titrando, AG, Switzerland).
Metrohm Stripping was
AG, Switzerland). performed
Stripping on
was per-
1formed
L of artificial
on 1 Lwastewater, and the air flow
of artificial wastewater, andrate wasflow
the air set to 900was
rate L/h.
setThe stripping
to 900 factors
L/h. The strip-
were
pingassessed whileassessed
factors were varyingwhile
the ammonia concentration
varying the and the pH ofand
ammonia concentration thethe
wastewater,
pH of the
under the conditions shown in Table 1.
wastewater, under the conditions shown in Table 1.

Figure 1. Schematic view of the ammonia stripping column.

Figure 1. Schematic view of the ammonia stripping column.

Table 1. Experimental conditions of NH3 stripping using a stripping column.

Temperature pH Initial NH3 Concentration

(°C) (-) (mg/L)
8.9 2900
9.4 1500–2900
20
10.2 2900
10.8 2900
Appl. Sci. 2021, 11, 441 5 of 13

Table 1. Experimental conditions of NH3 stripping using a stripping column.

Temperature pH Initial NH3 Concentration

(◦ C) (-) (mg/L)
8.9 2900
Appl. Sci. 2021, 11, x FOR PEER REVIEW 9.4 1500–2900 5 of 13
20
10.2 2900
10.8 2900

3.3. Packed
3.3. Packed Tower
Tower
Figure 22 shows
Figure shows the the packed
packed tower
tower system
system constructed
constructed to to determine
determine the the effect
effect ofofthe
the
liquid-gas contact ratio on the stripping factors. The tower
liquid-gas contact ratio on the stripping factors. The tower was designed with a diameterwas designed with a diameter
of 0.2
of 0.2 mm and
and aaheight
heightofof1.5 1.5mm toto
enable
enable observation
observation of the physical
of the characteristics
physical characteristics of NH of3
air stripping at the bench scale. The precise specifications are
NH3 air stripping at the bench scale. The precise specifications are shown in Table 2. The shown in Table 2. The inter-
nal packing
internal packingmaterial consisted
material consistedof 18ofmm18 mmPP pall rings,
PP pall and and
rings, the height of the
the height of packing
the packing was
0.48 0.48
was m. Them. maximum
The maximum capacity of theoftank
capacity was 147
the tank wasL;147 theL;effective capacity
the effective for the
capacity forstrip-
the
ping experiment was set to 100 L. The stripping temperature
stripping experiment was set to 100 L. The stripping temperature was set to 70 C, and a was set to 70 °C, and◦ a heater
in the in
heater tank
theandtanka and
heatagun heatwere used used
gun were to control the stripping
to control the strippingtemperature.
temperature. Air was sup-
Air was
plied using the heat gun into the bottom of the tower and
supplied using the heat gun into the bottom of the tower and was emitted from the top was emitted from the top of the
tower.
of The flow
the tower. Therate
flowofrateair ofwas
aircontrolled
was controlled usingusinga valve and measured
a valve and measured through a flow
through a
meter.
flow The liquid
meter. was supplied
The liquid was supplied into the
intotoptheof theoftower
top the towerfromfrom
the tank usingusing
the tank a pump; after
a pump;
spraying
after through
spraying a nozzle,
through the liquid
a nozzle, passes
the liquid through
passes throughthe packing layer,layer,
the packing then then
cycled back
cycled
into the
back intotank. The cycling
the tank. rate of
The cycling theofliquid
rate and the
the liquid andflowthe rate
flowofrate
theofgas
thearegasspecified along
are specified
with the
along with other operating
the other conditions
operating in Table
conditions 3. A 3.
in Table temperature-adjusted
A temperature-adjusted pH sensor
pH sensor was
installed
was inside
installed the tank
inside to monitor
the tank the pH
to monitor the and
pH and temperature,
temperature, and and
the NaOH
the NaOH solution was
solution
was supplied
supplied intointo
the the
tank tank using
using a pump
a pump totocontrol
controlthe thepH.pH. Ammonia
Ammonia stripping using using thethe
packed
packed tower
tower was was performed
performed at 70◦°C
at 70 C andandpH pH8.5 8.5(NH(NH33 fraction
fraction 76.1%).
76.1%). To Toascertain
ascertainthe the
optimal
optimaloperating
operatingconditions
conditionsfor forthe
thetower,
tower,the theliquid
liquidflow flowrateratewas
wasfixed
fixedatat117.0
117.0L/h,
L/h,and
and
the stripping efficiency was assessed according to the liquid-gas
the stripping efficiency was assessed according to the liquid-gas ratio by varying the gas ratio by varying the gas
flow
flow rate.
rate.

Figure 2. Schematic
Figure 2. Schematic view
view of
of the
the ammonia
ammonia stripping
strippingpacked
packedtower
towersystem.
system.

Table 2. Design parameters of the stripping tower.

Design Parameter Value Unit

Tower diameter 0.2 m
Tower height 1.5 m
Packed layer height 0.48 m
Appl. Sci. 2021, 11, 441 6 of 13

Table 2. Design parameters of the stripping tower.

Design Parameter Value Unit

Tower diameter 0.2 m
Tower height 1.5 m
Packed layer height 0.48 m
Packed materials PP pall ring -
Liquid tank volume 147 L

Table 3. Experimental conditions of NH3 stripping using a packed tower.

Initial NH3 Conc. Liquid Flow Rate Gas Flow Rate Liquid-Gas Ratio, L/G
(mg/L) (L/h) (L/h) (L-Liquid/m3 -Gas)
1100–3700 117.0 26,200 4.5
1100 117.0 4367 26.8
1100 117.0 2183 53.6
1100 117.0 1092 107.2

3.4. Analysis
The ammonia concentration in the aqueous solution was analyzed to assess the
stripping efficiency. Solution samples of 10 mL were taken from stripping column and
packed tower tank at regular time intervals. All samples were treated with sulfonic
acid to pH 2.5, and the concentrations of ammonium ions were quantified using ion
chromatography (930 Compact IC Flex, Metrohm AG, Herisau, Switzerland) equipped with
a cation separation column (Metrosep C 4 150/4.0, Metrohm AG, Herisau, Switzerland).

4. Results
4.1. Air Stripping without Liquid Circulation
Ammonia stripping was performed using the stripping column in Figure 1. In the
column reactor, the contact surface between liquid and gas is the interface of the air
bubble [14]. The mass transfer interfacial area is related to the size and number of air
bubbles. Therefore, it is possible to compare the mass transfer coefficient in the constant
conditions: total liquid volume; air flow rate; temperature [14]. As an experimental
condition, the airflow rate was constant of 900 L/h on 1 L of artificial wastewater. The
stripping efficiency and mass transfer rate of ammonia were analyzed according to initial
concentration and pH. Ammonia removal efficiency and mass transfer coefficient were
calculated by Equations (10), (15), and (16).
Figure 3 shows the results of stripping at different ammonium hydroxide concentra-
tions at 20 ◦ C and pH 9.4. Figure 3a shows the ammonia removal rate according to the
concentration. The removal rate increased with increasing time. After 3 h, similar results of
38.4%, 38.5%, and 38.3% were observed for concentrations of 1500, 2200, and 2900 mg/L,
respectively.
Figure 3b shows the natural logarithm of the relative change in total ammonia con-
centration over time. A linear regression analysis was conducted against time; the mean
slope was 0.16 ± 20.011. The R2 values were 0.980, 0.973, and 0.996 for each respective
concentration, indicating that the results were reliable. The overall volumetric mass transfer
coefficients on the liquid phase (K L, NH3 a) were calculated from the slope of Figure 3a and
Equation (16). The mean K L, NH3 a was 0.319 h−1 , which remained constant regardless of
the initial ammonia concentration in the solution. Therefore, the ammonium hydroxide
concentration had little effect on the removal efficiency or rate.
The change of pH in the ammonia solution causes a change of ammonia fraction,
which means that the higher pH, the more ammonia can be removed. pH is an important
parameter affecting the stripping efficiency and mass transfer coefficient.
 Appl. Sci. 2021, 11, x FOR PEER REVIEW 7 of 13

Appl. Sci. 2021, 11, 441 7 of 13

100 1.6
2900 mg/L 20 oC, pH 9.4 20 oC, pH 9.4
1.4
2200 mg/L Air flow rate = 900 L/h
80 Air flow rate = 900 L/h
1500 mg/L 1.2

-ln( [NH3,L]Tt / [NH3,L]T0 )

NH3 removal (%)

Initial NH3 slope KLNH3 a

60 1.0
(mg/L) (/h) (/h)
0.8 2900 0.173 0.309
40 2200 0.156 0.307
0.6 1500 0.158 0.340
0.4
20
0.2

0 0.0
0.0 0.5 1.0 1.5 2.0 2.5 3.0 0.0 0.5 1.0 1.5 2.0 2.5 3.0
Time (h) Time (h)

(a) (b)
Figure
Figure 3. Ammonia
3. Ammonia stripping
stripping performance
performance according
according to to initial
initial concentration
concentration at 20 ◦ C°C
at 20 and
and pHpH
9.4:9.4:
(a)(a) Ammonia
Ammonia removal
removal
rate;
rate; (b)(b) logarithm
logarithm of the
of the ammonia
ammonia concentration
concentration ratio.
ratio.

The change
Figure 4 representsof pHthe in results
the ammonia
of ammoniasolution causesaccording
stripping a changeto ofpH ammonia
at 2900 fraction,
mg/L
ammonia concentration and 20pH, ◦ C. The ammonia removal rate was shown as a linear
which means that the higher the more ammonia can be removed. pH is an important
increase
parameter overaffecting
time; after the2.5 h of stripping,
stripping the and
efficiency removal
massrate increased
transfer from 13.9% to 72.6%
coefficient.
when pH was4increased
Figure representsfrom 8.9 to 10.8.
the results To analyze
of ammonia the influence
stripping according of topHpH onatammonia
2900 mg/L
removal, the ratio of removal rate to ammonia
ammonia concentration and 20 °C. The ammonia removalNH fraction (η/ f rate ) was compared.
3 was shown as a linear
η/ f NH3in-
was approximately
crease over time; after constant
2.5 hfor
of pH 9.4–10.8;
stripping, theThe ratios rate
removal wereincreased
72.0%, 71.2%,from and 75.2%
13.9% at
to 72.6%
pH 9.4, 10.2
when pH andwas10.8, respectively.
increased from 8.9 From theseTo
to 10.8. results,
analyzeit wastheconfirmed
influence that of pH theon
ammonia
ammonia
removal
removal, ratethewas linearly
ratio affected
of removal by to
rate theammonia
ammoniafraction
fraction(𝜂/𝑓 according) wasto the 𝜂/𝑓
pH change.
compared.
Figure 4b shows the natural logarithm of the relative change
was approximately constant for pH 9.4–10.8; The ratios were 72.0%, 71.2%, and 75.2% in total ammonia con-at
centration against time; the slopes for each pH value were obtained
pH 9.4, 10.2 and 10.8, respectively. From these results, it was confirmed that the ammonia by linear regression
2 = 0.997, 0.980, 0.993, 0.989). As a result, the slope and mass transfer coefficient increased
(Rremoval rate was linearly affected by the ammonia fraction according to the pH change.
proportionally
Figure 4b with
showsincreasing pH. logarithm of the relative change in total ammonia con-
the natural
centration against time; the slopeswas
Appl. Sci. 2021, 11, x FOR PEER REVIEW
The amount of NaOH which for used
each topHadjust
value thewere pH was determined.
obtained NaOH
by linear regression
8 of 13
consumption was 0.74,
(R2 = 0.997, 0.980, 1.44,
0.993, 1.84,Asand
0.989). 1.92 gthe
a result, of 100%
slope NaOH/L
and mass liquid for
transfer pH 8.9, 9.4,
coefficient 10.2,
increased
and 10.8, respectively,
proportionally with to maintainpH.
increasing pH at 20 ◦ C. When pH increased, the ammonia removal
rate and Themass
amounttransfer rate were
of NaOH whichincreased,
was used but the amount
to adjust the pH was of chemical
determined. required
NaOH also
con-
increased.
sumption was 0.74, 1.44, 1.84, and 1.92 g of 100% NaOH/L liquid for pH 8.9, 9.4, 10.2, and
10.8, respectively, to maintain pH at 20 °C. When pH increased, the ammonia removal
100 1.6
pH8.9 rate and mass20transfero
C rate were increased, butpHthe amount slope KLNH3 ofachemical required also in-
pH9.4 1.4 (/h) (/h)
creased.
Air flow rate = 900 L/h
80
-ln( [NH ] / [NH ] )

pH10.2 8.9 0.056 0.219

T

1.2
3,L 0
NH3 removal (%)

pH10.8 9.4 0.173 0.340

1.0 10.2 0.384 0.462
60
10.8 0.521 0.574
0.8
T
3,L t

40 0.6

0.4
20 20 oC
0.2 Air flow rate = 900 L/h

0 0.0
0.0 0.5 1.0 1.5 2.0 2.5 3.0 0.0 0.5 1.0 1.5 2.0 2.5 3.0
Time (h) Time (h)

(a) (b)
Figure
Figure 4.4.Ammonia
Ammonia stripping
stripping performance
performance according
according toto
pHpH
atat ◦ C:
2020 °C:(a)(a)Ammonia
Ammoniaremoval
removal rate;
rate; (b)logarithm
(b) logarithm
ofof ammonia
ammonia
concentration ratio.
concentration ratio.

4.2. Packed Tower Air Stripping with Liquid Circulation

To analyze the effect of liquid-to-gas contact efficiency on the stripping tower oper-
ating factors, the stripping performance was assessed using the packed tower in Figure 2.
In the packed tower, the mass transfer interfacial area is a water film on the surface of
Appl. Sci. 2021, 11, 441 8 of 13

4.2. Packed Tower Air Stripping with Liquid Circulation

To analyze the effect of liquid-to-gas contact efficiency on the stripping tower operating
factors, the stripping performance was assessed using the packed tower in Figure 2. In the
packed tower, the mass transfer interfacial area is a water film on the surface of packed
materials. In this study, tower design, packed layer height, and liquid flow rate were
constant as shown in Tables 2 and 3. In consequence, a relative comparison of mass transfer
coefficients is possible using overall volumetric mass transfer coefficients.
Stripping was performed on 100 L of artificial wastewater at ammonia concentrations
of 1100 and 3700 mg/L with the packed tower. The liquid flow rate was 117.0 L/h and
the gas flow rate was 26,200 L/h. The stripping results for ammonia concentration in the
packed tower were shown in Figure 5.
Figure 5a shows the ammonia removal rate over time. After 1 h, the removal rate
reached 30.1% and 18.4%, in 1100 and 3700 mg/L solutions, respectively. The reason for
the difference in ammonia removal rate is that pH of the 1100 mg/L solution decrease to 8.
Thereafter, NaOH was used to maintain the pH at approximately 8.5, and the ammonia
removal rate showed similar trends over total stripping time.
Figure 5b shows the natural logarithm of the change in the ammonia concentration
ratio. As a result of linear regression analysis against time, the R2 values were relatively
low (0.923–0.957), but reliable results were obtained. The slopes were similar between the
two solution concentrations and the mass transfer coefficients of liquid ammonia were also
similar. At 70 ◦ C, pH 8.5, and 4.5 L/m3 L/G ratio, the mean mass transfer coefficient was
Appl. Sci. 2021, 11, x FOR PEER REVIEW 9 of 13
0.192 ± 0.003 h−1 . Stripping using the packed tower exhibited similar patterns regardless
of the solution concentration as shown in Figure 3. Finally, the ammonia concentration
of solution had little effect on the removal rate or mass transfer rate in both the stripping
column and packed tower.

100 1.2
1100 mg/L Initial NH3 slope KLNH3 a
3700 mg/L 1.0 (mg/L) (/h) (/h)
80
1100 0.147 0.189
-ln( [NH3,L]Tt / [NH3,L]T0 )

0.8 3700 0.143 0.194

NH3 removal (%)

60
0.6
40
0.4
70 oC, pH 8.5 70 oC, pH 8.5
20 Air flow rate = 26,200 L/h 0.2 Air flow rate = 26,200 L/h
Liquid flow rate = 117.0 L/h Liquid flow rate = 117.0 L/h
0 0.0
0 1 2 3 4 5 6 0 1 2 3 4 5 6
Time (h) Time (h)

(a) (b)
Figure
Figure 5. Ammonia
5. Ammonia stripping
stripping performance
performance according
according to to ammonia
ammonia concentration
concentration forfor
thethe packed
packed tower
tower at 70 ◦ C°C
at 70 and
and pHpH 8.5:
8.5:
(a) Ammonia removal rate; (b) logarithm of ammonia concentration
(a) Ammonia removal rate; (b) logarithm of ammonia concentration ratio. ratio.

ToTo identify
identify thethe optimal
optimal liquid-to-gas
liquid-to-gas contact
contact rangerange for tower,
for the the tower, the stripping
the stripping per-
perfor-
formance
mance was compared
was compared at different
at different gas rates
gas flow flow in
rates
thein the range
range L/m3 .L/m
of 4.5–107.2
of 4.5–107.2 3. Figure
Figure 6a
shows the removal
6a shows rate for
the removal 1100
rate for mg/L ammonium
1100 mg/L ammonium hydroxide solution
hydroxide at different
solution L/G ra-
at different L/G
tios. The The
ratios. ammonia removal
ammonia rate tended
removal to increase
rate tended as the L/G
to increase as theratio
L/Gdecreased. A decrease
ratio decreased. A de-
in crease
the L/Gin ratio corresponds
the L/G to an increase
ratio corresponds to aninincrease
the volume
in theofvolume
air supplied
of airper unit effective
supplied per unit
liquid capacity, which improves the ammonia removal efficiency [14,15].
effective liquid capacity, which improves the ammonia removal efficiency [14,15]. However, when
How-
the L/G ratio was excessively reduced (4.5 L/m 3 level here), 3airflow rate was too much,
ever, when the L/G ratio was excessively reduced (4.5 L/m level here), airflow rate was
resulting
too much,in aresulting
reduction inina ammonia
reduction removal
in ammonia efficiency.
removal In efficiency.
Figure 6a, In
theFigure
removal6a, rates
the re-
moval rates after 6 h were 57.1%, 63.0%, and 57.1% for L/G of 4.5, 26.8, 53.6 L/m3, respec-
tively. The most effective removal performance was shown at L/G 26.8 L/m3.
Figure 6b shows the natural logarithms of the relative concentration according to L/G
ratios. Figure 6b indicates that the slope and mass transfer coefficients increased with de-
creasing L/G ratio, except for 4.5 L/m3. The reason the mass transfer coefficient increases
Appl. Sci. 2021, 11, 441 9 of 13

after 6 h were 57.1%, 63.0%, and 57.1% for L/G of 4.5, 26.8, 53.6 L/m3 , respectively. The
most effective removal performance was shown at L/G 26.8 L/m3 .
Figure 6b shows the natural logarithms of the relative concentration according to L/G
ratios. Figure 6b indicates that the slope and mass transfer coefficients increased with
decreasing L/G ratio, except for 4.5 L/m3 . The reason the mass transfer coefficient increases
with reducing L/G is that contact efficiency improves at the liquid-to-gas interface due to
increased airflow rate. Base on the L/G ratio of 107.2 L/m3 , when it decreases by 1/2 or 1/4,
the gas flow rate increases by two or four times, and the mass transfer coefficient increased
1.4 or 1.6 times, respectively. However, when L/G reduced to 4.5 L/m3 , the gas flow
rate increases significantly by 24 times, whereas the mass transfer coefficient increases by
1.5 times. As a result, it was derived that the mass transfer coefficient increased according
to L/G decrease but decreases below a certain level. The gas flow rate and the mass transfer
coefficient are not necessarily proportional, and the optimal point should be derived.
Appl. Sci. 2021, 11, x FOR PEER REVIEW 10 of 13
The amount of NaOH consumed was 1.09 g of 100% NaOH/L liquid to maintain
pH 8.5 at L/G 107.2 L/m3 for 24 h. When compared to the results by pH at 20 ◦ C, the
ammonia removal efficiency is excellent despite less air supply and NaOH consumption
for the unit liquid.

100 2.0
70 oC, pH 8.5 70 oC, pH 8.5
Liquid flow rate = 117.0 L/h Liquid flow rate = 117.0 L/h
80
-ln( [NH3,L]Tt / [NH3,L]T0 )

1.5
NH3 removal (%)

60
1.0
40 L/G slope KLNH3 a
4.5 L/m3 (L/m3) (/h) (/h)
26.8 L/m3 0.5 4.5 0.143 0.194
20 53.6 L/m3 26.8 0.159 0.222
53.6 0.122 0.174
107.2 L/m3
107.2 0.068 0.099
0 0.0
0 2 4 6 8 10 12 14 16 18 20 22 24 0 2 4 6 8 10 12 14 16 18 20 22 24
Time (h) Time (h)

(a) (b)
Figure6. 6.Ammonia
Figure Ammonia stripping
stripping performance
performance according
according to the
to the liquid-gas
liquid-gas ratioratio ◦ C70
at 70at °C pH
and and8.5:
pH(a)
8.5: (a) Ammonia
Ammonia removal
removal rate;
rate;
(b) (b) logarithm
logarithm of ammonia
of ammonia concentration
concentration ratio. ratio.

Figure7 7shows
Figure showsthe thetotal
totalair airsupplied
suppliedagainst
againstthe theammonia
ammoniaremoval
removalrate rateatatdifferent
different
L/G
L/Gratios.
ratios.Here,
Here,the thetotal
totalair
airsupplied
suppliedrefersreferstotothe thetotal
totalcumulative
cumulativeair airforfor1 1LLofofartificial
artificial
wastewater.
wastewater.ToTocompare compare the total
the totalairair
supplied
supplied according
according totoL/G
L/Gratio,
ratio,ititwas
wasrevealed
revealedthat that
the
thelower
lowerL/G L/Gratio,
ratio,thethegreater
greaterthe thetotal
totalairairconsumed
consumedatatthe thesame
sameremoval
removalrate. rate.The
Thetotal
total
volume
volumeofofair airrequired
requiredwas was240 240L/LL/Lliquid
liquidatat53.6 53.6L/m L/m33 and
and 212
212 L/L water at
L/L water at 107.2
107.2 L/mL/m3 3to
toachieve
achieve76.1%,76.1%,wherewherethe the ammonia
ammonia removal removal rate was was equal
equal totothe
theammonia
ammoniafraction fraction
(η/ f NH3 ==1).
(𝜂/𝑓 1). AtAt L/G ratiosof
L/G ratios of4.5–26.8
4.5–26.8L/m L/m 3, 3
it, is
it predicted
is predicted that
that a greater
a greater volume
volume of air
of air will
will be required
be required more morethanthan
1600 1600andand 300300L/LL/L liquid,
liquid, respectively.
respectively.
From
FromFigures
Figures6 6and and7,7,it itwas
wasfoundfoundthatthatasasL/G L/Gratio
ratioincreased,
increased,thethemass
masstransfer
transferrate rate
improved,
improved, and the more air supply was required to ensure the same ammoniaremoval
and the more air supply was required to ensure the same ammonia removal
rate.
rate.ToTo increase
increase thethe
air air
supply,
supply,the size
the and
size power
and power costs of the of
costs blower need toneed
the blower be increased.
to be in-
Therefore, it is necessary to determine the optimal L/G
creased. Therefore, it is necessary to determine the optimal L/G ratio consideringratio considering removal efficiency,
removal
air supply, and time. In andthis time.
study,Inthe most efficient L/Gefficient
condition was 26.8 L/m 3 , and
efficiency, air supply, this study, the most L/G condition was 26.8
53.6 L/m 3 also seemed to be appropriate when trying to lower the total air supply. In
L/m , and 53.6 L/m also seemed to be appropriate
3 3 when trying to lower the total air sup-
3 was selected as an optimal condition for
consequence, a liquid-gas
ply. In consequence, a liquid-gas ratio of 26.8–53.6 L/m
ratio of 26.8–53.6 L/m was selected as an optimal condi-
3
packed
tion fortower
packed operating at 70 ◦ C, pH
tower operating at 708.5.
°C, pH 8.5.

1600
(L-air/L-liquid)

4.5 L/m3
1400 26.8 L/m3
1200 53.6 L/m3
107.2 L/m3
1000
 rate. To increase the air supply, the size and power costs of the blower need to be in-
creased. Therefore, it is necessary to determine the optimal L/G ratio considering removal
efficiency, air supply, and time. In this study, the most efficient L/G condition was 26.8
L/m3, and 53.6 L/m3 also seemed to be appropriate when trying to lower the total air sup-
ply. In consequence, a liquid-gas ratio of 26.8–53.6 L/m3 was selected as an optimal condi-
Appl. Sci. 2021, 11, 441 10 of 13
tion for packed tower operating at 70 °C, pH 8.5.

1600

Total air supplied (L-air/L-liquid)

4.5 L/m3
1400 26.8 L/m3
1200 53.6 L/m3
107.2 L/m3
1000

800

600 70 oC, pH 8.5

Liquid flow rate = 117.0 L/h
400

200

0
0 20 40 60 80 100
NH3 removal (%)

7. Ammonia removal ◦ C, pH 8.5, and

Figure
Figure 7. Ammonia removal rate rate according
according to thetovolume
the volume
of airof air supplied
supplied at 70
at 70 °C, pH 8.5, and
different
different L/GL/G ratios.
ratios.

4.3. The Comparison of Results with Literature

Table 4 shows the comparison of results for ammonia stripping system with the
literature. First, the stripping column results according to pH were compared. In this
study, the ammonia removal efficiency increased in proportion to ammonia fraction as the
pH increased. Zhu et al. [15] reported that an increase in pH increase leads to improve
ammonia stripping rate and mass transfer rate. When ammonia fraction and air supply are
similar, the removal rate and mass transfer coefficients are also similar to those derived
from literature [15].
Secondly, packed tower results were compared. It is difficult to compare the mass
transfer coefficient arithmetically because the interfacial area for the packed tower varies
depending on the design of the tower and the packed material. However, it is possible
to compare the approximate mass transfer rates by considering the ammonia fraction, air
supply, and liquid ratio.
Liu et al. [14] derived the mass transfer coefficient according to air flow rate. Although
there is no mention of the L/G ratio, it can be interpreted that the lower L/G, the higher
K L, NH3 a, since the L/G decreases as the air flow rate increases. When compared with this
study, it was confirmed that K L, NH3 a was almost same under similar air supply conditions.
It is considered that the calculated K L, NH3 a values are within a reasonable range when
compared with the reports by Liu et al. [14] and Ferraz et al. [12]. Li et al. [16] reported
the highest value of K L, NH3 a values under very low L/G ratio when compared to other
literatures.
In addition, ammonia removal rate was also compared for the jet loop reactor and the
water-sparged aerocyclone. In these two reactors, as in the column and packed tower, the
mass transfer coefficient increased as the liquid to gas ratio decreased.
Appl. Sci. 2021, 11, 441 11 of 13

Table 4. The comparison of removal rate and overall volumetric mass transfer coefficient based on the liquid phase of ammonia.

T Time Air Supplied L/G a η KL, NH3 a

Equipment pH fNH3 Ref.
(◦ C) (h) (L-Air/L-Liquid) (L-Liquid/m3 -Air) (%) (/h)
8.9 0.260 13.9 0.219
9.4 0.527 38.0 0.340
20 2.5 2250 - This work
Stripping 10.2 0.875 62.4 0.462
column without 10.8 0.965 72.6 0.574
circulation 10 0.864 1125 24.8 0.084
25 12 0.998 3 1125 - 55.4 0.24 [15]
12 0.998 2250 76.1 0.44
6 1572 4.5 57.1 0.194
6 262 26.8 63.0 0.222
70 8.5 0.761 This work
12 262 53.6 77.3 0.174
24 262 107.2 81.5 0.099
Packed tower 720 63.6 0.086
with circulation 50 10 0.970 12 1440 - 83.4 0.166 [14]
2880 98.7 0.368
25 11 0.985 24 4500 6.67 99 0.18 [12]
15 10.8 b 0.937 b 3.5 3000 0.332 75 0.42 [16]
7.8 930 2500 45.6 0.081
Jet loop reactor 20 11 0.978 7.8 1400 1667 87.2 0.299 [24]
6.8 2030 1000 96.3 0.629
Water-sparged 1540 0.0032 98.9 0.78
aerocyclone
25 11.5 b 0.995 3.5
2660 0.0018 93.7 1.32
[22]
a Liquid to gas ratio, L/G. b Average value.
Appl. Sci. 2021, 11, 441 12 of 13

5. Conclusions
Stripping experiments were performed using an air stripping column and a packed
tower on an ammonium hydroxide solution to calculate the major operating factors for each
device. For ammonia stripping with a column, an increase in pH resulted in higher recovery
efficiency and a larger mass transfer coefficient, and a proportional relationship was
observed between ammonia removal efficiency and ammonia fraction. However, ammonia
concentration did not affect ammonia removal rate or the mass transfer coefficient. For the
packed tower, the operating factors were analyzed at 70 ◦ C, pH 8.5. As the liquid-gas ratio
decreased in the range of 26.8–107.2 L/m3 , the mass transfer rate and air consumption
increased. The 26.8 L/m3 condition achieved the largest mass transfer coefficient and
63.0% of ammonia removal rate by only 6 h operation with 262 L-air/L-liquid. And at
L/G of 53.6 L/m3 , ammonia removal was 77.3% for 12 h with same air consumption.
Therefore, the optimal liquid-gas ratio was chosen as 26.8–53.6 L/m3 , by considering the
optimal mass transfer coefficient and air supply. In addition, through high-temperature
stripping, excellent ammonia removal rate was achieved with low NaOH consumption.
Finally, overall operating conditions such as temperature, pH, and air consumption were
optimized to ensure both performance and economics for ammonia stripping devices
design.

Author Contributions: Conceptualization, E.J.K.; writing—original draft preparation, E.J.K.; funding

acquisition, H.K.; project administration, H.K.; writing—review and editing, E.L. All authors have
read and agreed to the published version of the manuscript.
Funding: This research was funded by the Korea Agency for Infrastructure Technology Advancement
(KAIA) grant funded by the Ministry of Land, Infrastructure and Transport (Grant 21UGCP-B157945-02).
Institutional Review Board Statement: Not applicable.
Informed Consent Statement: Not applicable.
Data Availability Statement: Data available in a publicly accessible repository.
Acknowledgments: This subject was supported by the Korea Agency for Infrastructure Technology
Advancement (KAIA) grant funded by the Ministry of Land, Infrastructure and Transport (Grant
21UGCP-B157945-02).
Conflicts of Interest: There are no conflict of interest to declare.

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