applied

sciences
Article
Effects of Mixing Conditions on Floc Properties
in Magnesium Hydroxide Continuous
Coagulation Process
Yanmei Ding, Jianhai Zhao * , Lei Wei, Wenpu Li and Yongzhi Chi
Tianjin Key Laboratory of Aquatic Science and Technology, School of Environmental and Municipal Engineering,
Tianjin Chengjian University, Tianjin 300384, China; huaerqi@126.com (Y.D.); weilei900210@163.com (L.W.);
hitlwp@126.com (W.L.); 23733403@126.com (Y.C.)
* Correspondence: jhzhao@tcu.edu.cn




Received: 29 December 2018; Accepted: 27 February 2019; Published: 7 March 2019


Abstract: Magnesium hydroxide continuous coagulation process was used for treating simulated
reactive orange wastewater in this study. Effects of mixing conditions and retention time on the
coagulation performance and floc properties of magnesium hydroxide were based on the floc size
distribution (FSD), zeta potential, and floc morphology analysis. Floc formation and growth in
different reactors were also discussed. The results showed that increasing rapid mixing speed led
to a decrease in the final floc size. The floc formation process was mainly carried out in a rapid
mixer; a rapid mixing speed of 300 rpm was chosen according to zeta potential and removal efficiency.
Reducing retention time caused a relatively small floc size in all reactors. When influent flow was
30 L/h (retention time of 2 min in rapid mixer), the average floc size reached 8.06 µm in a rapid mixer;
through breakage and re-growth, the floc size remained stable in the flocculation basin. After growth,
the final floc size reached 11.21 µm in a sedimentation tank. The removal efficiency of reactive orange
is 89% in the magnesium hydroxide coagulation process.

Keywords: magnesium hydroxide; reactive orange; mixing; coagulation; floc size

1. Introduction
Magnesium hydroxide was used as a potential coagulant for reactive dyes wastewater
treatment for many years [1–3]. Typical characteristics of this kind of coagulant include nontoxicity,
an environmentally-friendly nature, recoverability, and rapid reaction [4]. Magnesium hydroxide
precipitate has a positive superficial charge and it can adsorb negative dyes through charge
neutralization or precipitate enmeshment [5,6]. Floc size settling properties are the main parameters
influencing reactive dyes removal efficiency in real industrial scale unit operations [7–9]. A photometric
dispersion technique and laser technique are useful in monitoring floc physical characteristics [10,11].
As previously found [12–14], magnesium hydroxide nucleation and precipitation processes are very
fast; floc size can reach to 15 µm. Although floc size is not very large compared with other coagulants,
the sedimentation process can meet the requirement of pollutant removal.
During the magnesium hydroxide coagulation process, mixing conditions influenced the removal
efficiency and floc properties. Rapid mixing brings the reactants together and homogenizes the solution.
In the rapid stirring process, it will cause nucleation and precipitation of magnesium hydroxide.
The magnesium hydroxide coagulation process had two stages including fast floc formation and
growth of flocs. As for slow mixing, flocs remained stable and the re-growth process was not happened
apparently in our previously found [13]. Several authors have found that operational conditions
influenced the coagulation process and flocs properties especially for mixing conditions [11,15]. Effects
of shearing on floc formation and growth are also related to coagulation mechanisms [16,17].

Appl. Sci. 2019, 9, 973; doi:10.3390/app9050973 www.mdpi.com/journal/applsci

 Appl. Sci. 2019, 9, x 2 of 8

Appl. Sci. 2019, 9, 973 2 of 8

conditions [11,15]. Effects of shearing on floc formation and growth are also related to coagulation
mechanisms [16-17].
Although Although there
there was was aamount
a large large amount
of dataofondata
the on the characteristics
characteristics of floc of
in floc in the coagulation
the batch batch coagulation
process,process, therebeen
there have havelimited
been limited
studiesstudies
on the on the relationship
relationship between between floc characteristics
floc characteristics and mixing
and mixing
conditions using magnesium hydroxide as a coagulant in the continuous process.
conditions using magnesium hydroxide as a coagulant in the continuous process. The main objectives The main objectives
of this of this laboratory
laboratory studyto
study were were to evaluate
evaluate the rolethe
ofrole of mixing
rapid rapid mixing
speed speed on coagulation
on coagulation performance
performance
and flocand floc properties.
properties. Furthermore,
Furthermore, the effects
the effects of retention
of retention time ontime
flocon floc characteristics
characteristics areassessed.
are also also assessed.

2. Materials and Methods

2. Materials and methods

2.1. Synthetic Test Water

2.1. Synthetic and Coagulant
test water and coagulant
Reactive orange orange
Reactive (K-GN) (K-GN)
was purchased from Jinan
was purchased Xinxing
from JinanTextile Dyeing
Xinxing Mill,Dyeing
Textile Shandong,
Mill,China.
Shandong,
Reactive dye solutions with pH 12 were prepared with K-GN and deionized
China. Reactive dye solutions with pH 12 were prepared with K-GN and deionized water water to provide a
to provide
concentration of 0.25 g/L.
a concentration of NaOH solution
0.25 g/L. NaOH was used towas
solution control
usedthetosolution
controlpHthevalue (PHS-25
solution pH Shanghai
value (PHS-25
Jinke Industrial Co., Shanghai, China). MgCl
Shanghai Jinke Industrial Co., Shanghai, 2 · 6H 2China). MgCl2·6H2O (CP. Tianjin Chemical China)
O (CP. Tianjin Chemical Reagent Co. Tianjin, Reagent Co.
was used to prepare the coagulant. Magnesium ion
Tianjin, China) was used to prepare the coagulant. was analyzed with anion
Magnesium ICS-1500 (Dionex, with
was analyzed Sunnyvale,
an ICS-1500
California, USA) ion chromatography system. The concentration of reactive orange in
(Dionex, Sunnyvale, California, USA) ion chromatography system. The concentration of reactive the solution
was analyzed
orange byin athe
UV-VISIBLE spectrophotometer
solution was analyzed by a(UV2550 Shimadzu,
UV-VISIBLE Suzhou, China).
spectrophotometer The reactive
(UV2550 Shimadzu,
orangeSuzhou,
characteristics
China).areTheshown in Table
reactive orange1. characteristics are shown in Table 1.

Reactive
Table 1.Table orange orange
1. Reactive characteristics.
characteristics.
Name
Name Molecular Structure
Molecular Structure λmax (nm)
λmax (nm)

Reactive orange
Reactive orange (K-GN) 476 476
(K-GN)

2.2. Apparatus
2.2. Apparatus and procedures
and Procedures
Continuous
Continuous experiments
experiments were carried
were carried out atout at temperature
temperature of 20 ± ◦ C, and
of 120±1℃, and
in in order
order to to obtain
obtain a a real
Appl.
real continuous
Sci.continuous
2019, 9, x steady
steady experiment,
experiment, K-GN K-GN removal
removal efficiency
efficiency remained
remained stablestable
at 2 h.atFor
2 h.this
Forprocess
this
3 of process
8 to to
occur, occur,
the 1 Lthe 1 L mixer
rapid rapid had
mixertohad
havetoahave
stirringa stirring
speed at speed at 250
250 to 350 to
rpm.350Therpm. The flocculation
flocculation basin was
basin was
every
divided 10divided
minutes.
into threeintoFloc
threesize
parts parts
(each distribution
of(each of 4 aL)(FSD)
4 L) and and awas measured
sedimentation
sedimentation bywas
tank (30tank
L) Mastersizer
(30designed 2000
L) was designed
for the(Malvern
for the removal
removal of
Panalytical,
flocs (Figure Malvern,
of flocs1).(FigureUK)
The slow and
1). The each sample
slowspeed
stirring stirring was
wasspeed measured three
was maintained
maintained times
at 80 rpm at to
in 80 obtain
therpm the average results.
in the flocculation
flocculation basin. 0.25 basin.
g/L 0.25
During
Reactive the slow
g/Lorange
Reactivemixing
and period
orange
250 and 250
mg/L inmagnesium
the
mg/Lthird flocculation
magnesium
ion were basin,
ionpumped zeta
intopotential
were pumped theinto thewas
rapid rapidmeasured
mixer, mixer, by
respectively.
respectively.
zetasizer
The total Nano ZS
Theinfluent (Malvern
total influent
flow was flowPanalytical,
was chosen
chosen Malvern,
at 30 L/h at 30
andL/h UK).
60and The images
L/h,60inL/h, of
in which
which flocs
retention from
retention
time was the
time rapid
was and
2 min mixer,
2 min and 1 min
1 min
third flocculation
in the in the mixer,
rapid rapidbasin,
mixer,and sedimentation
respectively.
respectively. The tank
The operational were
operational captured
conditions
conditions bycontinuous
of the ofIX71 digital
the continuous photomicrography
coagulation
coagulation process process
are are
(Olympus, Tokyo,
shown
shown in Table 2. in Japan).
Table 2.

Table 2. Operational conditions of coagulation process.

Flux Rapid Mixer Flocculation Basin Sedimentation Tank

speed time speed time time
250rpm
30L/h
300rpm 2min 80rpm 24min 60min
350rpm
60 L/h 300rpm 1min 80rpm 12min 30min

2.3. Floc size distribution and properties analysis

During the
Figure
Figure continuous
1. Experimentalcoagulation
1. Experimental
apparatus forprocess,
apparatus for samples
coagulation
coagulation of flocs were
of magnesium
of magnesium taken from a rapid mixer, with
hydroxide.
hydroxide.
the third flocculation basin and sedimentation tank using a tube with an inner diameter of 5 mm
3. Results and Discussion

3.1. Coagulation Behaviors Under Different Rapid Mixing Speed

3.1.1. Floc Size Distribution in Three Processes

Appl. Sci. 2019, 9, 973 3 of 8

Table 2. Operational conditions of coagulation process.

Flux Rapid Mixer Flocculation Basin Sedimentation Tank

speed time speed time time
250 rpm
30 L/h
300 rpm 2 min 80 rpm 24 min 60 min
350 rpm
60 L/h 300 rpm 1 min 80 rpm 12 min 30 min

2.3. Floc Size Distribution and Properties Analysis

During the continuous coagulation process, samples of flocs were taken from a rapid mixer, with
the third flocculation basin and sedimentation tank using a tube with an inner diameter of 5 mm
every 10 minutes. Floc size distribution (FSD) was measured by Mastersizer 2000 (Malvern Panalytical,
Malvern, UK) and each sample was measured three times to obtain the average results. During the
slow mixing period in the third flocculation basin, zeta potential was measured by zetasizer Nano ZS
(Malvern Panalytical, Malvern, UK). The images of flocs from the rapid mixer, third flocculation basin,
and sedimentation tank were captured by IX71 digital photomicrography (Olympus, Tokyo, Japan).

3. Results and Discussion

3.1. Coagulation Behaviors under Different Rapid Mixing Speed

3.1.1. Floc Size Distribution in Three Processes

Continuous experiments were performed under 250 mg/L magnesium ion with 30 L/h to
investigate the effects of rapid mixing conditions on coagulation performance and floc size distribution.
According to FSD, average floc size decreased when rapid mixing speed increased in the rapid mixer
and sedimentation tank. In the flocculation basin, floc size tended to be stable or slightly broken with
the increase of rapid mixing speed to 300rpm. This is consistent with the findings that repulsive forces
tend to stabilize the suspension and prevent particle agglomeration [13,18]. As shown in Table 3,
the average floc sizes 8.39, 8.06 and 8.04 µm were obtained with rapid mixing speeds of 250, 300 and
350 rpm in a rapid mixer, respectively. Small floc had the same trend to aggregate relatively large flocs.
Average floc size was 8.06 and 7.89 µm in the rapid mixer and flocculation basin when the mixing
speed was 300 rpm. In general, the flocs will grow in the flocculation basin, but it seems that floc
size decreased in the flocculation process. In fact, during the flocculation process, particles larger
than 11.25 µm accounted for 4.54% and 4.9% in the rapid mixer and flocculation basin, respectively.
Particles smaller than 1 µm also decreased in the slow mixing period. As can be seen also in Figure 2
(sedimentation tank), particles smaller than 1 µm account for 6.2%, 10.0% and 12.6% with mixing
speeds of 250, 300 and 350 rpm respectively. It was observed that the percentage of smaller particles
increased with the increase of mixing speed. This indicates that the high mixing speed will break the
flocs, and only part of the flocs will aggregate again after the flocs are broken. The general shape of the
curves was broadly similar in different units. The average floc size decreased to a steady state; there
was a dynamic balance between floc growth and breakage. When the stirring speed was increased
from 250 rpm to 350 rpm, small average floc size could be observed in these three units. Following the
breakage and aggregation period, there was only a partial flocs re-growth, showing that the broken
flocs can only re-grow to a very limited extent.
Appl. Sci. 2019, 9, 973 4 of 8

Table 3. Average floc size in different process units.

Average Floc Size (µm)

Rapid Mixing (rpm)
Rapid Mixer Flocculation Basin Sedimentation Tank
250 8.39 7.96 14.41
Appl. Sci. 2019, 9, x 300 8.06 7.89 11.21 4 of 8
350 8.04 7.95 10.58

6
5 250rpm
250rpm
5
300rpm
4 300rpm

Volume(%)
4 350rpm
350rpm
Flocculation basin
Volume(%)

3 Rapid mixer
3
2 2
1 1
0 0
0.01 0.1 1 10 100 1000 0.01 0.1 1 10 100 1000
Size(μm) Size(μm)

(a) (b)

6
250rpm
5 300rpm
350rpm
Volume(%)

4 Sedimentation tank

3
2
1
0
0.01 0.1 1 10 100 1000
Size(μm)

(c)
Figure
Figure 2. 2.Floc
Floc size
size distribution
distribution with
withdifferent
differentrapid mixing
rapid for for
mixing three stages.
three (a) rapid
stages. (a) mixer; (b)
rapid mixer;
flocculationtank.
(b) flocculation basin; (c) sedimentation basin; (c) sedimentation tank.

3.1.2. Removal Efficiency and Zeta

Table Potential
3. Average floc size in different process units.
As shown in Figure 3, the K-GN removal efficiency AverageafterFloc coagulation
Size (µm) remained stable at about 89%
Rapid Mixing
in three different rapid mixing conditions. Although Removal efficiency is not significantly influenced
(rpm) Rapid Mixer Flocculation Basin Sedimentation Tank
by rapid mixing speed, zeta potential increased with increasing rapid mixing speed. Changes in floc
250 8.39 7.96 14.41
characteristics also lead to changes in zeta potential. Rapid stirring speed may change the zeta potential
300 8.06 7.89 11.21
of the colloid, because the rapid mixing could change the floc size and their surface properties. Positive
350 8.04 7.95 10.58
magnesium hydroxide acts as a charge neutralization species. Similar results were also found in the
magnesium hydroxide coagulation process for the removal of reactive dyes [18,19]. Zeta potential is
3.1.2. Removal Efficiency and Zeta Potential
important in terms of the impact on steady state floc size and response to increased levels of shear.
UnderAsdifferent
shown inshear
Figure 3, the K-GN
conditions, theremoval
break-upefficiency
flocs may after
havecoagulation remainedproperties.
different physical stable at about
Floc
89%
properties impacted significantly on the overall process efficiency [20]. Electrical chargesignificantly
in three different rapid mixing conditions. Although Removal efficiency is not or colloidal
influenced
properties ofbytherapid mixing hydroxide-reactive
magnesium speed, zeta potential increased
orange with be
flocs would increasing rapid mixing
greatly affected. Based onspeed.
this
Changes in floc characteristics also lead to changes in zeta potential. Rapid stirring speed
observation, it can be reasoned that charge-neutralization is one of the mechanisms for destabilization may change
the
andzeta potential
removal of the colloid,
of reactive because
orange [21]. the rapid
Normally, slowmixing could
mixing change also
conditions the floc sizethe
affects andflocs
theirbreak-up
surface
properties.
and growth.Positive
However, magnesium hydroxide hydroxide
in the magnesium acts as a charge neutralization
coagulation process, species.
magnesiumSimilar results
hydroxide
were also found in the magnesium hydroxide coagulation process for the removal of
formed and flocs grew fast, then the larger flocs broke into relatively small particles in the slow mixingreactive dyes
[18,19].
period. Zeta potential found
As previously is important in growth
[13], floc terms ofis the
not impact on steady
significantly state floc
influenced by asize
slowand response
mixing to
period.
increased levels of shear. Under different shear conditions, the break-up flocs may have different
physical properties. Floc properties impacted significantly on the overall process efficiency [20].
Electrical charge or colloidal properties of the magnesium hydroxide-reactive orange flocs would be
greatly affected. Based on this observation, it can be reasoned that charge-neutralization is one of the
mechanisms for destabilization and removal of reactive orange [21]. Normally, slow mixing
Appl. Sci. 2019, 9, 973 5 of 8
Appl. Sci. 2019, 9, x 5 of 8

conditions
In on floc
this research, theproperties
effects of were not considered.
slow mixing Ason
conditions hasfloc
been mentioned,
properties werelarge flocs breakage
not considered. As and
has
re-growth
been will happen
mentioned, large simultaneously and,re-growth
flocs breakage and consequently, there is simultaneously
will happen less opportunityand,
for the break flocs
consequently,
to re-grow.
there is less opportunity for the break flocs to re-grow.

90 0

Removal efficiency(%)
-4

Zeta potential(mV)
88
-8

-12
86 Removal efficiency
Zeta potential
-16

84 -20

-24
250 300 350
Rapid mixing (rpm)
Figure 3. Effects
Effects of rapid mixing on removal efficiency and zeta potential.

3.2. Effect of
3.2. Effect of Flow
Flow oon
n Coagulation
Coagulation Performance
Performance
For continuous coagulation
For continuous coagulation reaction,
reaction, thethe flow
flow determines
determines the the retention
retention time
time of
of reactants
reactants inin each
each
reactor. The increase of flow indicates the decrease of retention time. In order to investigate
reactor. The increase of flow indicates the decrease of retention time. In order to investigate the effect the effect
of flow on
of flow on coagulation
coagulation performance,
performance, continuous
continuous experiments
experiments werewere performed
performed under
under magnesium
magnesium ion ion
250 mg/L,rapid
250 mg/L, rapidmixing
mixing speed
speed 300rpm
300rpm with
with 30 L/h
30 L/h and and 60 The
60 L/h. L/h.retention
The retention
time intime in themixing
the rapid rapid
mixing
tank was tank
2min wasand 2min
1minand for1min
flow of for30flow
L/h of
and3060
L/h
L/h,and 60 L/h, respectively.
respectively. As shown inAs shown
Table in average
4, the Table 4,
the average floc size decreased with increasing influent flow for each operation
floc size decreased with increasing influent flow for each operation unit. As for the rapid mixer, unit. As for the rapid
the
mixer,
averagethe average
floc size was floc size
8.06 was
and 7.258.06
μmand for 7.25
30L/hµm for6030L/h
and and 60 L/h, According
L/h, respectively. respectively. According
to earlier to
results
earlier results [14], in the stage of rapid mixing, magnesium hydroxide was
[14], in the stage of rapid mixing, magnesium hydroxide was formed and particles grew in a very formed and particles grew
in a very
short short
time. time. A period
A suitable suitableofperiod
rapid of rapidwas
mixing mixing was necessary
necessary for goodfor good coagulation.
coagulation. ReactiveReactive
orange
orange removal efficiency reached 89% and 83% for 30 L/h and 60 L/h, respectively.
removal efficiency reached 89% and 83% for 30 L/h and 60 L/h, respectively. The retention time in The retention
time
each in each
unit for unit
60L/h forwas
60L/h wasthan
shorter shorter
thatthan
of 30that
L/h,ofespecially
30 L/h, especially in the
in the rapid mixerrapid
of 1mixer of 1 min
min retention
retention
time. Thistime.
is tooThis
shortis to
tooform
shortmagnesium
to form magnesium hydroxide-reactive
hydroxide-reactive orange flocs.
orange flocs.

Table 4.
Table Average size
4. Average size in
in different
different process
process units.
units.

Flow Average
Average Size
Size (µm)
(µm)
Flow (L/h)
(L/h) Rapid
Rapid Mixer
Mixer FlocculationBasin
Flocculation Basin Sedimentation Tank
Sedimentation Tank
30 30 8.068.06 7.89
7.89 11.21
11.21
60 60 7.257.25 7.52
7.52 10.47
10.47

Figure 4 clearly indicates floc formation and growth in the magnesium hydroxide-reactive
Figure 4 clearlycoagulation
orange continuous indicates floc formation
system. andrapid
In the growth in the
mixer andmagnesium
flocculationhydroxide-reactive
basin, average flocorange
size
continuous coagulation system. In the rapid mixer and flocculation basin, average floc
remained stable and flocs aggregated to relatively large flocs in the sedimentation tank. These two size remained
stable
figuresand flocs aggregated
showed to relatively
the same trends large
that the flocs in thehydroxide
magnesium sedimentation tank. These
coagulation two figures
process showed
was similar to
the same trends that the magnesium hydroxide coagulation process was similar
the precipitation process. When magnesium ion is added to the alkaline solution in rapid mixingto the precipitation
process. When
period, the magnesium
reaction ion is added
crystallization to the
process willalkaline
happensolution
rapidly. in rapid mixing
Magnesium period, the
hydroxide reaction
coagulation
crystallization process will happen rapidly. Magnesium hydroxide coagulation
includes magnesium hydroxide nucleation and a combination of reactive orange into flocs. includes magnesium
hydroxide nucleation and a combination of reactive orange into flocs.
Appl. Sci. 2019, 9, x 6 of 8
Appl. Sci. 2019, 9, x 6 of 8
Appl. Sci. 2019, 9, 973 6 of 8

6 7
6 a Flow: 30L/h 7 b Flow: 60L/h
5 a Flow: 30L/h
Rapid mixer 6 b Flow: 60L/h
Rapid mixer
5 Rapid mixer basin
Flocculation 6 Rapid mixer basin
Flocculation
4 Flocculation basin
Sedimentation tank 5 Flocculation basin
Sedimentation tank

Volume(%)
4 5 Sedimentation tank
Volume(%)

Sedimentation tank

Volume(%)
4
Volume(%)

3 4
3 3
2 3
2 2
1 2
1 1
0 1
0 0
0
0.01 0.1 1 10 100 1000 0.01 0.1 1 10 100 1000
0.01 0.1 1 10
Size(μm) 100 1000 0.01 0.1 1 10 100 1000
Size(μm) Size(μm)
Size(μm)
(a) (b)
(a) (b)
Figure 4. Floc size distribution with different flows for three stages. (a) 30 L/h; (b) 60 L/h.
Figure4.4.Floc
Figure Flocsize
sizedistribution
distributionwith
withdifferent
differentflows
flowsfor
forthree
threestages.
stages.(a)
(a)30
30L/h;
L/h; (b) 60 L/h.
L/h.

3.3. Images analysis

Analysis
3.3. Images analysis
The floc size distribution can tell us the percentages
percentages of different floc sizes (shown
(shown inin Figure
Figure 4),
4),
The floc size distribution can tell us the percentages of different floc sizes (shown in Figure 4),
commonly used to
and the removal efficiency is commonly to estimate
estimate the
the coagulation
coagulation performance.
performance. In order to
and the removal efficiency is commonly used to estimate the coagulation performance. In order to
gain further insight into the floc and sediment properties, image analysis was used to predict floc
gain further insight into the floc and sediment properties, image analysis was used to predict floc
characteristics by IX71 digital photomicrography. In In Figure
Figure 5,5, the average
average size of flocs in different
characteristics by IX71 digital photomicrography. In Figure 5, the average size of flocs in different
reactors is clearly indicated. The floc formation and growth processes were carried out in the rapid
reactors is clearly indicated. The floc formation and growth processes were carried out in the rapid
mixer and no more aggregation occurred due to the strong repulsion repulsion between positively charged
mixer and no more aggregation occurred due to the strong repulsion between positively charged
particles ofofmagnesium
particles magnesium hydroxide
hydroxide inflocculation
in the the flocculation basin.
basin. In In the sedimentation
the sedimentation tank, flocs
tank, flocs aggregated
particles of magnesium hydroxide in the flocculation basin. In the sedimentation tank, flocs
aggregated to form relatively large particles. This is consistent with the findings of FSD
to form relatively large particles. This is consistent with the findings of FSD value which are shown value which
in
aggregated to form relatively large particles. This is consistent with the findings of FSD value which
are shown
Figure 4. Asinfor
Figure
Figure4.5a,d,
As for Figure
they 5ashow
clearly and 5d,
thatthey clearlyflow
increasing show that increasing
caused a decrease flow
of thecaused
averagea
are shown in Figure 4. As for Figure 5a and 5d, they clearly show that increasing flow caused a
decrease
size in theofrapid
the average sizeaverage
mixer. The in the rapid mixer.
floc size The average
of magnesium floc size of magnesium
hydroxide-reactive orange hydroxide-
is 8.06 and
decrease of the average size in the rapid mixer. The average floc size of magnesium hydroxide-
reactive
7.25 µm.orange
This is is 8.06
also and 7.25 with
consistent μm. This is also consistent
the findings withstudy
of a previous the findings
[14]. of a previous study [14].
reactive orange is 8.06 and 7.25 μm. This is also consistent with the findings of a previous study [14].

Figure
Figure 5. Floc image
5. Floc image analysis
analysis (a)
(a) rapid
rapid mixer
mixer for
for 3030 L/h; (b) flocculation
L/h; (b) flocculation basin
basin for
for 30
30 L/h;
L/h;
Figure
(c) 5. Floc image
sedimentation analysis
tank for
for 30 L/h; (a)
L/h;(d) rapid
(d)rapid mixerfor
rapidmixer
mixer for6030
L/h.L/h; (b) flocculation basin for 30 L/h;
(c)sedimentation tank 30 for 60 L/h.
(c)sedimentation tank for 30 L/h; (d) rapid mixer for 60 L/h.
4. Conclusions
4. Conclusions
4. Conclusions
In this research, the effects of mixing conditions on magnesium hydroxide continuous coagulation
performance and floc properties were investigated. Rapid mixing speed plays a significant role in floc
Appl. Sci. 2019, 9, 973 7 of 8

formation and growth. The function of the rapid mixer is to provide a place for the rapid nucleation
and precipitation of magnesium hydroxide. In this stage, coagulant and reactive orange formed flocs.
In the flocculation basin, small flocs will form more dense flocs, but average floc size remains stable.
After the sedimentation process, flocs aggregate to form relatively large flocs. Therefore, appropriate
rapid stirring is conducive to the formation of flocculation and the removal of pollutants. Increasing
the flow will cause a short retention time; the average floc size decreases from 11.21 to 10.47µm when
flow increases from 30 to 60 L/h. The coagulation behavior indicates that magnesium hydroxide is an
effective coagulant for reactive orange removal with an efficiency of 89%.

Author Contributions: Investigation, W.L.; data curation, L.W.; writing—original draft preparation, Y.D.;
writing—review and editing, J.Z.; funding acquisition, Y.C.
Funding: This research was funded by the Technology Research and Development Program of Tianjin, China,
grant number 16YFXTSF00390.
Acknowledgments: The authors would like to acknowledge the support from Tianjin Key Laboratory of Aquatic
Science and Technology.
Conflicts of Interest: The authors declare no conflict of interest.

References
1. Huang, X.; Wu, T.; Li, Y.; Sun, D.; Zhang, G.; Wang, Y.; Wang, G.; Zhang, M. Removal of petroleum sulfonate from
aqueous solutions using freshly generated magnesium hydroxide. J. Hazard. Mater. 2012, 82–88, 219–220. [CrossRef]
[PubMed]
2. Gao, B.Y.; Yue, Q.Y.; Wang, Y.; Zhou, W.Z. Color removal from dye-containing wastewater by magnesium
chloride. J. Environ. Manag. 2007, 82, 167–172. [CrossRef] [PubMed]
3. Ayoub, G.M.; BinAhmed, S.W.; Al-Hindi, M.; Azizi, F. Coagulation of highly turbid suspensions using
magnesium hydroxide: Effects of slow mixing conditions. Environ. Sci. Pollut. Res. 2014, 21, 10502–10513.
[CrossRef] [PubMed]
4. Wang, Q.; Luan, Z.; Wei, N.; Li, J.; Liu, C. The color removal of dye wastewater by magnesium chloride/red
mud (MRM) from aqueous solution. J. Hazard. Mater. 2009, 170, 690–698. [CrossRef] [PubMed]
5. Tan, B.H.; Teng, T.T.; Mohd Omar, A.K. Removal of dyes and industrial dye wastes by magnesium chloride.
Water. Res. 2000, 34, 597–601. [CrossRef]
6. Bouyakoub, A.Z.; Lartiges, B.S.; Ouhib, R.; Kacha, S.; El Samrani, A.G.; Ghanbaja, J.; Barres, O. MnCl2
and MgCl2 for the removal of reactive dye Levafix Brilliant Blue EBRA from synthetic textile wastewaters:
An adsorption/aggregation mechanism. J. Hazard. Mater. 2011, 187, 264–273. [CrossRef] [PubMed]
7. Yang, Z.; Li, H.; Yan, H.; Wu, H.; Yang, H.; Wu, Q.; Li, H.; Li, A.; Cheng, R. Evaluation of a novel chitosan-based
flocculant with high flocculation performance, low toxicity and good floc properties. J. Hazard. Mater. 2014,
276, 480–488. [CrossRef] [PubMed]
8. Li, T.; Zhu, Z.; Wang, D.S. Characterization of floc size, strength and structure under various coagulation
mechanisms. Powder. Technol. 2006, 168, 104–110. [CrossRef]
9. Xiao, F.; Yi, P.; Pan, X.R.; Zhang, B.J.; Lee, C. Comparative study of the effects of experimental variables on
growth rates of aluminum and iron hydroxide flocs during coagulation and their structural characteristics.
Desalination 2010, 250, 902–907. [CrossRef]
10. McCurdy, K.; Carlson, K.; Gregory, D. Floc morphology and cyclic shearing recovery: Comparison ofalum
and polyaluminum chloride coagulants. Water Res. 2004, 38, 486–494. [CrossRef] [PubMed]
11. Yu, W.Z.; Gregory, J.; Campos, L.; Li, G. The role of mixing conditions on floc growth, breakage and re-growth.
Chem. Eng. J. 2011, 171, 425–430. [CrossRef]
12. Liu, M.; Lu, J.; Wei, L.; Wang, K.; Zhao, J. Magnesium hydroxide coagulation performance and floc properties
in treating high pH reactive orange wastewater. Water Sci. Technol. 2015, 71, 1310–1316. [CrossRef] [PubMed]
13. Zhao, J.; Shi, H.; Liu, M.; Lu, J.; Li, W. Coagulation-adsorption of reactive orange from aqueous solution by freshly
formed magnesium hydroxide: Mixing time and mechanistic study. Water Sci. Technol. 2017, 71, 1310–1316. [CrossRef]
[PubMed]
14. Zhao, J.; Wang, A.; Wei, L.; Ge, W.; Chi, Y.; Lai, Y. Effect of kaolin on floc properties for reactive orange
removal in continuous coagulation process. Water Sci. Technol. 2018, 78, 571–577. [CrossRef] [PubMed]
Appl. Sci. 2019, 9, 973 8 of 8

15. Xu, W.Y.; Gao, B.Y.; Yue, Q.Y.; Wang, Y. Effect of shear force and solution pH on flocs breakage and re-growth
formed by nano-Al13 polymer. Water Res. 2010, 44, 1893–1899. [CrossRef] [PubMed]
16. Verma, A.K.; Dash, R.R.; Bhunia, P. A review on chemical coagulation/flocculation technologies for removal
of colour from textile wastewaters. J. Environ. Manag. 2012, 93, 154–168. [CrossRef] [PubMed]
17. De Feo, G.; Galasso, M.; Landi, R.; Donnarumma, A.; De Gisi, S. A comparison of the efficacy of organic
and mixed-organic polymers with polyaluminium chloride in chemically assisted primary sedimentation
(CAPS). Environ. Technol. 2013, 34, 1297–1305. [CrossRef] [PubMed]
18. Semerjian, L.; Ayoub, G.M. High-pH—magnesium coagulation—flocculation in wastewatertreatment.
Adv. Environ. Res. 2003, 7, 389–403. [CrossRef]
19. Zhou, Q.; Chen, F.; Wu, W.; Bu, R.; Li, W.; Yang, F. Reactive orange 5 removal from aqueous solution using
hydroxyl ammonium ionic liquids/layered double hydroxides intercalation composites. Chem. Eng. J. 2016,
285, 198–206. [CrossRef]
20. Sharp, E.L.; Jarvis, P.; Parsons, S.A.; Jefferson, B. The impact of zeta potential on the physical properties of
ferric-NOM flocs. Environ. Sci. Technol. 2006, 40, 3934–3940. [CrossRef] [PubMed]
21. Leentvaar, J.; Rebhun, M. Effect of magnesium and calcium precipitation on coagulation—Flocculation with
lime. Water Res. 1982, 16, 655–662. [CrossRef]

© 2019 by the authors. Licensee MDPI, Basel, Switzerland. This article is an open access
article distributed under the terms and conditions of the Creative Commons Attribution
(CC BY) license (http://creativecommons.org/licenses/by/4.0/).