Soil Science and Plant Nutrition

ISSN: 0038-0768 (Print) 1747-0765 (Online) Journal homepage: http://www.tandfonline.com/loi/tssp20

Characterization of Treatment Processes and

Mechanisms of COD, Phosphorus and Nitrogen
Removal in a Multi-Soil-Layering System
Kuniaki Sato , Tsugiyuki Masunaga & Toshiyuki Wakatsuki
To cite this article: Kuniaki Sato , Tsugiyuki Masunaga & Toshiyuki Wakatsuki (2005)
Characterization of Treatment Processes and Mechanisms of COD, Phosphorus and Nitrogen
Removal in a Multi-Soil-Layering System, Soil Science and Plant Nutrition, 51:2, 213-221, DOI:
10.1111/j.1747-0765.2005.tb00025.x
To link to this article: http://dx.doi.org/10.1111/j.1747-0765.2005.tb00025.x

Published online: 17 Dec 2010.

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Soil Sci. Plant Nutr., 5 1 (2), 2 I3 - 22 I , 2005

213

Characterization of Ikeatment Processes and Mechanisms of COD,

Phosphorus and Nitrogen Removal in a
Multi-Soil-LayeringSystem
Kuniaki Sato, Tsugiyuki Masunaga and Toshiyuki Wakatsuki
Laboratory of Soils and Ecological Engineering, Faculty of Life and Environmental Science, Shimane University,
Matsue, 690-8504 Japan; and *Faculty of Agriculture. Kinki University.Nara, 631 -8505 Japun

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Received July 2,2004; accepted in revised form December 15, 2004

Characteristics of the treatment processes inside a MSL system were investigated by using
a laboratory-scale MSL system, which was set up in a D10 x W60 x H73 cm acrylic box
enclosing soil mixture blocks alternating with permeable zeolite layers. For the study of
the treatment processes inside the system, wastewater, with mean concentrations (mg L-)
of COD: 70, T-N: 12, T-P: 0.9, was introduced into the system at a loading rate of 1,000 L m-2
d-I. lkeatment processes in the MSL system were different for the COD, P and N pollutants.
Eighty percent of COD was removed in the 1st soil layer among the 6 layers, and the
removal rate increased as water moved down and finally reached 90% in the last layer of
the system. Phosphorus concentration was lower under the soil mixture layers than under
the permeable layers, presumably because P was adsorbed mainly by soil and mixed iron
particles. The P concentration in water gradually decreased in the lower layers of the system. The concentration of PO,3--P was generally lower in the aerated MSL system than in
the non-aerated one. NH,+-N was adsorbed and nitrified in the upper part of the system.
The NO,--N concentration was lower in water under the soil mixture layers than under the
permeable layers, indicating that denitrification mainly occurred in the soil mixture layers.

Key Words: Multi-Soil-Layering method, nitrogen and phosphorus removal, organic matter
removal, processes of wastewater treatment.
The 21st century is generally considered to be the
century with a growing concern about the preservation
of the environment and water resources. Water pollution
has become a serious problem in advanced as well as
developing countries, and the low quality of the water
supplied is a serious problem worldwide.
Water purification based on soil ecology is carried out
widely all over the world, because of the ubiquitous
presence of soil (Bhamidimarri 1988; Kaplan 1988; Perkins 1989; Ho and Mathew 1993; Reed et al. 1995;
Mara 1996; Lantzke et al. 1999; William 2000). Soil
displays various characteristics related to the environment, including size of pore space, oxidation-reduction
and hydrophilicity-hydrophobicity.As a result, various
species of microorganisms are able to live in soil. Therefore, a kind of purification process occurs simultaneously in soil. Since we were concerned about such environmental cleanup function of soil, we developed and studied a water purification system, the Multi-Soil-Layering
(MSL) system. The MSL system consists of soil units
arranged in a brick-like pattern surrounded by layers of

zeolite or alternating particles of homogeneous sizes

that allow a high hydraulic loading rate. The MSL system is effective for the prevention of clogging and shortcuts which are the main constraints in the conventional
soil-based wastewater treatment systems (Wakatsuki et
al. 1993, 1998, 1999; Masunaga et al. 1998, 2002,2003;
Sat0 et al. 2002,2005).
As described by Attanandana et al. (2000), Boonsook
et al. (2003) and Luanmanee et al. (2001, 2002a, b), the
MSL system can be developed mainly from locally
available resources, such as soil, iron particles, jute or
saw dust, charcoal, and zeolite or alternative materials.
Iron particles mixed in soil to enhance the phosphate
adsorption and denitrification functions act as reducing
agents. Organic materials are added as foods for the
microorganisms and as electron donors for denitrification. Charcoal contributes to the improvement of organic
matter decomposition as an adsorbent and habitat for the
microorganisms. Although appropriate amount and timing of aeration are necessary (Luanmanee et al. 2002a),
the maintenance of the MSL system is simple and it was

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2 14

K. SATO, T. MASUNAGA, and T. WAKATSUKI

found that the MSL system can contribute to the

improvement of the water quality under a wide range of
conditions, even in developing countries (ex. Masunaga
et al. 2002). The MSL system enables to enhance and
control various biological activities by regulating soil
physical and chemical properties.
Although various types of wastewater treatments have
been applied successfully using the MSL system in
Japan, Thailand and Indonesia, the processes of wastewater treatment by the MSL system have not been fully
elucidated. This is because the treatment processes have
been mainly estimated by comparing wastewater and
treated water and the material balance of the system
before and after wastewater treatment so far. Although
experiments in which water was collected inside the
MSL system had been conducted (Wakatsuki et al.
1990), quantitative evaluation of the treatment processes
in the MSL systems has not been achieved because of
the shortage of water sample points. Quantitative characterization of the treatment mechanisms in the MSL
system enables to further improve the efficiency of the
MSL system by appropriate adjustment of the structure
and material composition. Therefore we conducted laboratory-scale experiments in the present study to analyze
quantitatively the processes of wastewater treatment in
the respective layers of the MSL system. In the present
study, the positions inside the MSL system (i.e. soil
mixture layers, permeable layers and depth of the system), changes in the treatment processes with the passage of time and the effect of aeration were systematically and comprehensively investigated.

MATERIALS AND METHODS

Description of MSL system in the present
study. Figure 1 shows the structure of MSL system.
For the MSL system, an acrylic box D10 X W50 X H73
cm in size was used to enclose zeolite and soil mixture
layers forming an alternate brick layer-like pattern.
Twenty five sets of water collection pipes were installed
in the zeolite layers between each soil mixture layer.
The soil mixture layers were composed of soil (Andisol,
i.e. humus-rich volcanic ash soil, Kurohoku), saw dust,
granular iron and charcoal at the ratios of 7 1.6%, 10.5%,
11.9% and 6.0%, respectively, on a dry weight basis.
The void spaces (permeable layers) between each block
and block sides were filled with zeolite particles 35 mm in diameter. A detailed description of the MSL
system used in this study can be found in Fig.1 of the
report of Sat0 et al. (2005).

Research on quantitative processes of treatment in the respective layers of the system.

Domestic wastewater from a nearby community dispos-

Aeration pipe (Air supply:3.3 X 104 L m3day-')

MSL system
under aeration

MSL system in the

absence of aeration

Outlet of water collection pipe : front side

Outlet of water collection pipe : back side

Fig. 1. Comparison of the MSL system under aeration and in

the absence of aeration in the studies on treatment processes. In
the MSL system under aeration, an aeration pipe was installed.

a1 plant was diluted three times with tap water and introduced into the system for studying water purification
processes inside the MSL system. Two types of MSL
systems were prepared (Fig. I). The effect of aeration
was determined by comparing the MSL system under
aeration and without aeration. Loading rate of 1,OOO L
m-? d-' was continuously applied for 212 d (28 May
2002-26 December 2002), except during the period for
the preparation of the wastewater and maintenance of
the water pump. Mean chemical properties of the inflow
water were as follows : COD 70 mg L-', T-N 12 mg L-'
and T-P 0.9 mg L-' . An aeration pipe (1.O cm in diameter) was installed between the first and the second soil
mixture layers (MSL under aeration). Rate of aeration of
3.3 X lo4L mp3d-' was the same as that used in a MSL
system for domestic wastewater treatment (Wakatsuki et
al. 1993).
Water samples under the wastewater treatment process in the system were collected from each water collection pipe of the MSL system under aeration and
without aeration, starting from the bottom to the upper
layer one by one, to prevent the influence of water sampling on the flow of water in the subsequent layers. A
sufficient amount of water was collected for the analysis
(at least over 60 mL) for about 1-50 h. Except for water
sampling, the water collection pipes were closed by a
plug. The water samples, wastewater and treated water
(i.e. final effluent of the system) were analyzed for the
COD concentration by the potassium dichromate method, NH,+-N concentration by the Nessler method,
NO,--N and N02--N concentrations by ion chromatography (DIONEX OX-120) and for the PO4"-P concentration by the ascorbic acid method (APHA 1992).

Treatment Processes and Mechanisms inside MSL System

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RESULTS AND DISCUSSION

Quantification of the degree of treatment in
each layer of the MSL system
Figure 2 shows the fluctuations of the mean concentrations of COD, PO,3--P, NH,+-N, NO,--N and NO,-N of the treated water in each layer of the system during
the 0- I80 d period of operation. Figures 3-5 show the
treatment processes and mechanisms for the removal of
organic matter (COD), phosphorus and nitrogen on the
7th and 170th d of the experimental period. The mean
values of the concentrations in the soil mixture layers
and permeable layers of the MSL system under aeration
and without aeration are also shown in Figs. 3-5. The
values on the 7th d represented the total mean in the
MSL system under aeration and without aeration,
because they did not differ at the initial stage.
Process of organic matter (COD) removal
In the soil mixture layers, the values of COD were
lower than those in the permeable layers (Fig. 2a),
which indicates that the efficiency of COD removal was
higher in the soil mixture layers. Table 1 shows the
mean outflow rate from each water collection pipe and
cumulative COD removal rate in each layer. This cumulative COD removal rate was estimated by measuring
the amount of water outflow from all the water collection pipes and the COD concentration in each layer.
Although the whole amount of the wastewater input was
not collected from the pipes, the flow rate per total area
occupied by the soil mixture layer and the permeable
layer in each layer was estimated, based on the flow rate
of the collection pipes and the area they occupied. Then
after, the flow rate was corrected by the ratio the flow
rate and the loading rate, assuming the existence of a
uniform vertical flow without lateral water movement
under the soil mixture layers and under the permeable
layers. Most of the COD in the wastewater was removed
in the top soil layer at the rate of 74.3% for the MSL
system under aeration and 80.6% for the MSL system
without aeration, and the removal rates increased as
water moved down, and finally reached a value of 90%.
At the initial stage of the experiment, it was considered that physicochemical reactions such as filtration
and adsorption in the upper part of the system were the
major processes. It appeared that the organic matter
referred to as COD or BOD was easily trapped in the
soil mixture layers, because of the amount of pore
space, large surface area and enhanced hydrophobic
properties by the addition of charcoal. After 170 d, the
quality of the treated water remained satisfactory (Figs.
2a, 3). Biological process of COD removal seemed to
occur, in addition to the physicochemical reaction. COD

215

values were lower on the 170th d than on the 7th d in the

upper part of the system, indicating the existence of
microbial activity, i.e. organic matter decomposition was
enhanced with time through the accumulation of various
microorganisms. On the effect of aeration on organic
matter (COD) removal, the COD concentration of the
treated water of the MSL system may not differ appreciably regardless of the presence or absence of aeration
and the mean values were 5.5 and 6.6 mg L-', respectively. In contrast, in the 2nd-4th soil mixture layers,
the COD values of the MSL system under aeration were
lower than those in the MSL system without aeration
(Figs. 2a, 3). This indicates that aeration enhanced the
microbial activity for the decomposition of organic matter in the soil mixture layers of MSL system. In the
absence of aeration, the accumulation of organic matter
may be enhanced in the upper layers of the MSL system, as shown in Fig. 3. In fact, in the absence of aeration, the MSL system was clogged on the 203rd d. The
clogging due to the accumulation of organic matter,
however, could be dissolved by interrupting the operation during a period of 2 to 3 months (Wakatsuki et al.
1998, 1999). To avoid the formation of a thick biofilm,
the control of aeration is important. The lifetime of the
MSL system for organic matter treatment could be semipermanent if the irreversible formation of impermeable
layers could be avoided through the selection of suitable
materials and appropriate construction of a non-compacted MSL structure (Luanmanee et al. 2002b).

Process of phosphorus removal

The PO,"--P concentration was lower in the soil mixture layers and fluctuated less than that in the permeable
layers (Fig. 2b). The trend of PO,"--P concentration
changed in the permeable layers, especially in the upper
first and second layers, which showed a similar pattern
to that of the fluctuations in wastewater. The concentration in the soil mixture layers decreased abruptly even in
the first layer, whereas the concentration in the permeable layers gradually decreased in the lower layers. In
both soil mixture layers and permeable layers, these
were areas where PO,"--P could be adsorbed. The
mechanism of phosphorus removal is based on phosphorus adsorption on the active aluminum hydroxides contained in soil and also on ferric hydroxides formed from
the metal irons added in the soil mixture layers. In the
soil mixture layers, added metal irons dissolved and
leached out as ferrous ions from the inner soil mixture
layers under anaerobic conditions. And then, in an edge
of the soil mixture layers close to the permeable layers
under relatively aerobic conditions, ferrous ions were
further oxidized to ferric hydroxides and were adsorbed
on the clay particles. In the permeable layers, ferrous
ions, which leached out from the soil mixture layers,

K. SATO, T. MASUNAGA, and T. WAKATSUKI

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216

(d)tN0i-N

(e):NO,--N

Fig. 2. Dynamic mean concentrations of COD, PO,'--P, NH4+-N,NO,--N and NO,--N of the treated water under the process in
each layer of the system. SML: soil mixture layers, PL: permeable layers.

Treatment Processes and Mechanisms inside MSL System

217

a b l e 1. Mean outflow rate from each water collection pipe and cumulative COD removal rate (%) in the layers of the MSL
system.
Mean outflow rate (mL h-I)

Mean cumulative COD removal rate (%)

Absence of aeration

Aeration
Layer

Under SML

Under PL

Under Sh4L

Under PL

14.5
40.4
64.2
96.3
77.9

64.6
42.7
52.8
82.7
73.4

33.2
22.0
38.9
59.2
52.8

41.5
33.5
68.6
144.4
173.7

2
3
4
5
Treated water

Aeration

Absence of aeration

74.3
84.9
88.4
89.4
90.1
92.1

80.6
77.4
83.9
84.0
88.3
90.6

SML: soil mixture layers. PL: permeable layers.

170th day

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7th day

Fig. 3. Treatment process of COD on the 7th and 170th d. The mean values of the concentration (mg L-I) in both soil mixture layers (circles) and permeable layers (squares) at each position of the MSL system under aeration and in the absence of aeration are also
shown in the figure. The values on the 7th d represent the total mean in the MSL system under both conditions, because they did not
differ at the initial stage.

were further oxidized to insoluble ferric hydroxides.

Consequently, the surface area of ferric hydroxides
expanded by these processes and was able to remove
effectively phosphorus in the MSL system. The mechanisms of phosphorus removal were described in detail in

a previous report (Wakatsuki et al. 1993). It was eventually concluded that the maintenance of proper redox
conditions through appropriate aeration control is an
important factor for effective phosphorus removal in the
MSL system.

K. SATO, T. MASUNAGA, and T. WAKATSUKI

218

170th day

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7th day

aeration

absence of aeration

Fig. 4. Treatment process of phosphorus on the 7th and 170th d. The mean values of the concentration (mg L-I) in both soil mixture layers (circles) and permeable layers (squares) at each position of the MSL system under aeration and in the absence of aeration
are also shown in the figure. The values on the 7th d represent the total mean in the MSL system under both conditions, because they
did not differ at the initial stage.

Physicochemical reactions were the main processes

involved in phosphorus removal and they took place
from the initial stage of treatment for effective P removal. The effect of aeration appeared with the passage of
time in the MSL system under aeration. The PO,3--P
concentration of treated water was lower in the MSL
system under aeration than in the MSL system without
aeration during the later period of the experiment (Figs.
2b, 4). As mentioned above, it appeared that the ferrous
ions which were dissolved from the inner soil mixture
layers were more oxidized under aeration and became
insoluble ferric hydroxides at the edge of the soil mixture layers and permeable layers, as shown in Fig. 4.
However, it was reported that phosphorus removal by
adsorption decreased because of the formation of a
highly passive Fe,O, surface coating by excessive aeration (Nishiguchi 1990).Therefore, further improvements
are necessary for the phosphorus treatment under aeration conditions. Since the main process of phosphorus
removal consists of physicochemical adsorption, effective contact between the wastewater and soil mixture

layers is a major factor for P removal. Reducing the size

and increasing the number of soil mixture layers may
enable to achieve such an effective contact by the
increase of the surface area of the soil mixture layers.

Process of nitrogen removal

At the initial stage of the experiment, although NH,+N was detected in the permeable layers in the upper part
of the system, the concentration was very low in the soil
mixture layers (Fig. 2c), presumably because both
NH,+-N adsorption and nitrification took place in the
soil mixture layers. The concentration of NO,--N was
higher in the soil mixture layers than in the permeable
layers in the top layers, especially at the onset of the
operation before 60d, due to previous increase of the
nitrification activity in the soil mixture layers. In addition to physicochemical adsorption by soil and zeolite,
the nitrification activity developed with time in the
upper permeable layers, as evidenced by the decrease in
the NH,+-N concentration and increase in the NO,--N
concentration in the MSL system under aeration and

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Treatment Processes and Mechanisms inside MSL System

219

Fig. 6. Treatment process of nitrogen on the 7th and 170th d. The mean values of the concentration (mg L-I) in both soil mixture
layers (circles) and permeable layers (squares) at each position of the MSL system under aeration and in the absence of aeration are
also shown in the figure. The values on the 7th d represent the total mean in the MSL system under both conditions, because they did
not differ at the initial stage.

without aeration at the later stage of the experiment,

compared with the initial stage (Figs. 2c, e, 5). Since the
NH,+-N concentration decreased in the upper part of the
system, the nitrification of NH4+ mostly occurred in the
upper part. NH,+ adsorption by zeolite and soil was also
likely to have contributed to the decrease in the NH,+-N
concentration and the enhancement of nitrification in the
MSL system associated with the increase of the duration
of the presence of NH,+-N in the system. NO,--N, the
intermediate product of transformation of ammonia to
nitrate, was generated in the upper layers only at the initial stage of the experiment (Fig. 2d).
At the initial stage, NO,--N was formed in the upper
part of the system and the concentration increased further in the middle part and remained at the same level in
the lower part. With the passage of time, the NO,--N
concentration decreased in the lower part, as shown in
Fig. 5 and Fig. 2e, indicating that denitrification proceeded. The concentration of NO,--N was significantly

low in the soil mixture layers, especially in the absence

of aeration, indicating that denitrification mainly
occurred in the soil mixture layers. It is suggested that
the supply of NO,--N, decrease of the oxygen concentration and/or optimum supply of organic matter (i.e.
added saw dust and organic matter from wastewater) in
the upper part of the system may enable to enhance the
denitrification process in the lower layers.
Absence of aeration of the system enhanced the nitrogen removal. The concentration of NO,--N in the MSL
system without aeration was lower than that in the MSL
under aeration, especially in the lower part of the system. As shown in Fig. 5, it was assumed that an anaerobic environment was generated and that organic matter
as an electron donor accumulated more in the MSL system without aeration, as reflected in the COD concentration (Fig. 3). These conditions were suitable for
denitrification. Since nitrification was satisfactory in the
MSL system both under aeration and without aeration,

220

K. SATO, T. MASUNAGA, and T. WAKATSUKI

Table 2. Comparison of the relative concentration of

each pollutant at each position of the system under soil
mixture layers and permeable layers.
7th d
Part of

system SML PL
COD

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PO,-P

170th d
Aeration
SML PL

Absence of aeration
SML

PL

<

<

Lower

Lower

<<
<

<<
<

<<
<<

<

<
<

Upper

NH,-N

Upper
Lower

NO,-N

Upper
Middle
Lower

<
-

>
<
-

SML: soil mixture layers. PL: permeable layers.

denitrification was the limiting factor for nitrogen

removal in this MSL system. This was because of the
insufficient availability of organic matter as an electron
donor, due to the high decomposition rate of organic
matter, as evidenced by the effective COD removal
(Wakatsuki et al. 1990).The implication is that the MSL
system could introduce oxygen by natural gas exchange
through the top of the system even in the absence of aeration.

Conclusion
The results of the present study showed that the processes of the treatment of organic matter, phosphorus
and nitrogen were different (Figs. 3-5 and Table 2).
Treatment process of COD was relatively simple, while
that of phosphorus and nitrogen was more complicated.
The location where each pollutant was removed was
also different in the MSL layers. COD and phosphorus
were removed mainly in the upper part of the system,
while nitrogen was removed throughout the upper to
lower parts of the system because two steps, i.e. nitrification and denitrification were involved. Moreover, the
treatment conditions such as aeration affected the treatment process and effectiveness of each pollutant. Some
of the mechanisms underlying the treatment processes in
the MSL system were elucidated in the present study, as
described above. However, for the practical application
of the results obtained in this study, it is still necessary
to accumulate more quantitative data and analyses of the
treatment process of each pollutant. This includes studies on the effect of structural differences in the MSL
system such as size, shape and material composition of
the soil mixture layers, and differences in the treatment
conditions of the system, such as wastewater quality,
loading rate and aeration, as shown in the present study.

These studies are currently being conducted or planned.

Based on the results obtained, we plan to set up guidelines for the planning and design of operational conditions and structure of the MSL system depending on the
quality and quantity of target wastewater as well as
treatment target in the near future.

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