w a t e r r e s e a r c h 6 0 ( 2 0 1 4 ) 7 5 e8 1

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Removal of coagulant aluminum from water

treatment residuals by acid
Tetsuji Okuda a,*, Wataru Nishijima a, Mayo Sugimoto b, Naoyuki Saka b,
Satoshi Nakai b,**, Kazuyasu Tanabe c, Junki Ito d, Kenji Takenaka d,
Mitsumasa Okada e
a

Environmental Research and Management Center, Hiroshima University, Japan

Graduate School of Engineering, Hiroshima University, Japan
c
Department of Architecture and Civil Engineering, Fukuyama University, Japan
d
Agricultural Technology Research Center in Hiroshima Prefectural Technology Research Institute, Japan
e
Open University of Japan, Japan
b

article info

abstract

Article history:

Sediment sludge during coagulation and sedimentation in drinking water treatment is

Received 28 November 2013

called water treatment residuals (WTR). Polyaluminum chloride (PAC) is mainly used as a

Received in revised form

coagulant in Japan. The recycling of WTR has been desired; one method for its reuse is as

17 April 2014

plowed soil. However, WTR reuse in this way is inhibited by the aluminum from the added

Accepted 22 April 2014

PAC, because of its high adsorption capacity for phosphate and other fertilizer compo-

Available online 4 May 2014

nents. The removal of such aluminum from WTR would therefore be advantageous for its
reuse as plowed soil; this research clarified the effect of acid washing on aluminum

Keywords:

removal from WTR and on plant growth in the treated soil. The percentage of aluminum

Coagulation

removal from raw WTR by sulphuric acid solution was around 90% at pH 3, the percentage

Nutrient

decreasing to 40% in the case of a sun-dried sample. The maximum phosphate adsorption

Plowed soil

capacity was decreased and the available phosphorus was increased by acid washing, with

Polyaluminum chloride

90% of aluminum removal. The enhancement of Japanese mustard spinach growth and the

Recycle

increased in plant uptake of phosphates following acid washing were observed.

2014 Elsevier Ltd. All rights reserved.

Sludge

1.

Introduction

Coagulation followed by sedimentation is a common technology in drinking water treatment. Polyaluminum chloride
(PAC) and aluminum sulphate (alum) are common coagulants;
coagulation can efficiently increase the size of suspended
solids by producing flocs. Flocs can easily settle during

sedimentation and be removed as sedimentation sludge; purified supernatant can then be obtained. Sediment sludge is
known as water treatment residuals or WTR; its 2010
output from waterworks in Japan was 329,628 DS-t as dry soil
(JWWA, 2013). Recent literature suggests that Europe and the
United States respectively produce several hundred thousand
and over 2 million tons of solid residuals each year, and that

* Corresponding author. 1-5-3 Kagamiyama, Higashi-Hiroshima, Hiroshima 739-8513, Japan. Tel.: 81 82 424 6197; fax: 81 82 424 4351.
** Corresponding author.
E-mail address: aqua@hiroshima-u.ac.jp (T. Okuda).
http://dx.doi.org/10.1016/j.watres.2014.04.041
0043-1354/ 2014 Elsevier Ltd. All rights reserved.

76

w a t e r r e s e a r c h 6 0 ( 2 0 1 4 ) 7 5 e8 1

global sludge production might total 10,000 t/day (Gibbons and

Gagnon, 2011; Sengupta and Prakash, 2004). In most cases, the
WTR generated is disposed of via landfilling or through land
application, but both options, among others, are now subject
to close scrutiny. The increasing generation of WTR, coupled
with environmental restraint regarding its current disposal
outlets, has prompted increased research toward its reuse.
WTR recycling has been desired in Japan as well, especially
given its shortage of landfill sites. Japans Ministry of Health,
Labour and Welfare in 2004 introduced a water supply service
policy, called the Water Service Vision (Ministry of Health
(2004)). This policy sets forth concrete solutions for dealing
with serious future issues relating to water supply services
(Ministry of Health (2003)), and calls for a WTR recycling percentage increase from 52% (in 2011) up to 100%. There are
many ways in which WTR is being reused, mostly in building
and construction, land applications and other uses
(Babatunde and Zhao, 2007).
Concentrations of heavy metals such as lead (Pb), cadmium (Cd) and chromium (Cr) in WTR are commonly at
satisfactorily low levels, unlike in soils and plants, so WTR
recycling is not so difficult; one of the major reuse applications
is as raw material for cement and athletic field sand. Another
application is as a component of tilled soils, including horticultural soils. However, WTR contains aluminum originating
from coagulants, which has a damaging effect on plants
(Lombi et al., 2010; Panda and Matsumoto, 2007; Tang et al.,
2007; Fuller and Richardson, 1986). Furthermore, because
aluminum has high adsorption capacity for phosphates and
other anionic ions (Dayton et al., 2003; Ippolito et al., 2003), the
aluminum in WTR inhibits plant utilize to anionic fertilizer
components containing phosphate. For example, Novak and
Watts (2004) determined the maximum phosphate sorption
capacity of WTR (P-max) to be 85-175 mgP/g, which is more
than 85 times that of some natural soils.
Gibbons et al. (2009) studied the phosphate-adsorptive capacity (Qmax) of several WTRs (from plant-treated raw water
with low and high alkalinity) using P-spiked de-ionized water
and secondary municipal wastewater effluent. The results
show that ferric residuals had the highest phosphateadsorptive capacity (Qmax 2960 mg/kg), followed by lime
(Qmax 1390 mg/kg) and alum (1110 mg/kg and 1030 mg/kg).
Because of WTRs high phosphorus sorption capacity, its use
as an adsorbent in water treatment has also been suggested.
Makris et al. (2004) reported the potential of WTR as a longterm immobilizer of sorbed phosphorus, showing that WTR
drastically reduced soluble phosphorus with non-equilibrium
characteristics, even after 80 d of reaction. Because of this
strong phosphate-adsorption capacity, the limitation of WTR
use in agricultural plowed soil has also been indicated.
Codling (2008) also reported that mixing of WTR reduced the
extractable phosphorus in soils, and that water-extractable
phosphorus immobilized by WTR did not recover even under
weak acidic conditions.
As in these cases, indiscriminate addition of WTR could
result in excessive immobilization of soluble phosphorus,
leading to crop deficiencies. Oladeji et al. (2007) evaluated the
influence of applied concentration of WTR with aluminum
coagulants on plant yields using Bahiagrass (paspalum notatum fluggae); phosphorus concentrations in plant tissue and

phosphorus uptake were then determined. Soil phosphorusadsorption capacity increased with the WTR application
rate, indicating that lower soil phosphorus storage capacity
value is suitable for preventing negative agronomic impact.
Therefore, the WTR mixing ratio of WTR cannot be increased
from around 10%.
This study also investigated the technique of WTR reuse as
a sewerage system coagulant. Miyanoshita et al. (2009) evaluated the treatment cost of WTR for sewerage system in
Japan, concluding that the construction cost is much lower for
combined treatment with sewerage system than for individual treatments. The additional sewer charge is less than the
increase in cost for constructing an individual sludge treatment system, sensitive parameters being the sewer charge
and the distance between the drinking water treatment
plants. However, to assure the safety of treated water it is only
necessary to extract coagulant aluminum for WTR reuse as
coagulant for drinking water treatment. In a previous study
investigating the regeneration of PAC from WTR, the two-step
method for PAC regeneration was proposed for selective
extraction of aluminum from manganese (Sekine, 2001). The
two-step method represents the extraction of aluminum and
manganese, and the purification of aluminum by precipitation
at pH 4.5e6.5. The cost analysis also conducted in the research
showed potential; however, WTR reuse was not considered.
The combination of coagulant regeneration and agricultural
reuse of its residue would yield greater cost performance and
accelerate WTR reuse. Therefore, the optimum extraction pH
for WTR reuse should be studied, as should the effect of WTR
type, i.e., dry or wet. This research also studied the effect of pH
in acid washing and of the sun-drying process on aluminum
removal from WTR; the properties of washed sludge as
plowed soil were also investigated. As well, the plant growth
potential of washed sludge was also determined by pot experiments, using Japanese mustard spinach (Brassica rapa var.
perviridis, Komatsuna).

2.

Materials and methods

2.1.

Acid washing of WTR

The WTR sample used in this study was obtained from a

drinking water treatment plant in Hiroshima, Japan, whose
influent water source is the Ootagawa river. The water treatment facility uses PAC as coagulants, with pH adjustment
using NaOH and HCl; coagulation is conducted after sedimentation of bigger suspended solids without use of chemicals. WTR is generated by concentrating the sample in a
thickener, without belt pressing or added chemicals. The WTR
is then sun-dried for a few months. The thickened sludge and
sun-dried sample with 85% and 15% water content respectively, were used for this study.
Sulfuric acid was used for the acid washing to remove the
aluminum from WTR, on the basis of the results of preexperiments using several kinds of acid. Washing was conducted using a solid/liquid ratio of 3:100 (6 g of sludge in
200 ml). During washing, pH was adjusted to a specified value
(between 1 and 5), maintained by an automatic pH controller
(TOKO Chemical Corporation, model TPD-51) with sulfuric

w a t e r r e s e a r c h 6 0 ( 2 0 1 4 ) 7 5 e8 1

acid. After 2 h of acid extraction, the sludge was collected by

centrifugation and decantation. The collected washed sludge
was then suspended in 200 ml of distilled water, and the
suspension was manually neutralized by sodium hydroxide
solution to around pH 7.0  0.5, using a pH meter (HORIBA, F51). The sludge sample, collected by centrifugation and rinsed
with distilled water, then dried in an oven (ISUZU, Muffle
Furnace) for 12 h at 100  C for use in subsequent experiments.
The permeability of sludge decrease with acid washing at
pH 1 as will be described later, so granulation was conducted.
The washed sludge was mixed while controlling moisture
content, to produce particle diameter of around 10 mm; the
particles were then heated and hardened for 1 h in the oven at
100  C.

2.2.

Soil property analysis

The amount of aluminum removed from WTR was calculated

as the ratio of aluminum concentration in the extracted solution to the aluminum content in the sludge. The aluminum
concentration in the solution was determined using inductively coupled argon plasma atomic emission spectrometry
(ICP-AES; Nippon Jarrell-Ash, ICAP-575II), after filtration with
a 0.45 mm membrane filter. The aluminum content in the
sludge was determined by extraction with 1 N hydrochloric
acid solution, based on the standard method of the soil
contamination countermeasures law in Japan. The mass balance of aluminum could be confirmed within 20%.
To evaluate the effect of aluminum removal on the
phosphorus-adsorption capacity of the sludge, the maximum
adsorption capacity for phosphorus (P-max) was determined
on the basis of phosphorus sorption isotherm (Dayton and
Basta, 2005). Phosphorus sorption isotherms were generated
by batch equilibration with standard phosphorus (KH2PO4)
solutions of 10e500 mg/L with 10 mM CaCl2 (ionic regulation)
and 67 mM CHCl3 (sterilization). One gram of sludge sample
was added into a vial with 10 mL phosphoric acid solution;
sorption equilibrium was achieved by mixing with a mechanical shaker for 24 h at 25  1  C. The filtrate was obtained
with a 0.45 mm membrane filter, and soluble phosphorus in the
filtrate was analyzed using a spectrophotometer (Shimadzu,
UV-1800) at a wavelength of 880 nm. P-max was determined
on the basis of Langmuir model fit. Total organic carbon (TOC)
was determined using a TOC analyzer (TOCe5000, Shimadzu).
To evaluate other soil properties relevant to plant growth,
the soil pH, electric conductivity (EC), hydraulic conductivity,
cation exchange capacity (CEC) and available phosphorus
(soluble phosphorus) of the sludge sample were determined as
common soil properties (Asagi and Ueno, 2008). In addition,
arsenic (As) and cadmium (Cd) contents in sludge were also
determined, because they were detected in WTR at concentrations close to environmental standards in some cases
(Mctigue et al., 1992). Soil pH was determined by pH meter
(HORIBA, F-51) in a sludge slurry with a solideliquid ratio of
1:2.5; EC was determined by conductivity meter (HORIBA, DS8F) in a sludge slurry with a solideliquid ratio of 1:5 (Dayton
et al., 2003). Hydraulic conductivity was measured as the
ability of water to pass through the sample (Lange and
Antohe, 2000). CEC is defined as the degree to which a soil
can adsorb and exchange cations, as determined by the

77

method of Rhoades (Ippolito et al., 2003; Rhoades, 1982). In this

procedure, exchangeable sites were replaced by NH
4 with
then
being
extracted
by
potasammonium acetate, the NH
4
sium chloride solution. The amount of extracted NH
4 was
determined by the indophenol method, with CEC expressed as
meq/kg. The available phosphorus (soluble phosphorus) in
sludge was measured by Truogs method (Puchooa et al.,
1999). For the analysis, 40 ml of 0.76 M ammonium phosphate solution was added to 10 g of sludge in an Erlenmeyer
flask. As an extracting solution for available phosphorus,
0.1 mol/L of hydrochloric acid was added to the sludge at the
solid/liquid ratio of 1:200. The mixture was shaken for 1 h with
a mechanical shaker, then filtered with a grass fiber filter
(Whatman GF/B of approximately 1 mm pore size). The
available phosphorus concentration in the filtrate was then
determined. For the phosphorus analysis, 2 mL of filtrate, 5 mL
of distilled water and 2 mL of chromogenic reagent (consisting
of 40 mL 2.5 mol/L sulphuric acid, 15 mL ammonium molybdate, 5 mL potassium antimonytartrate, 0.53 g ascorbic acid
and 40 mL distilled water) were mixed (Mohee et al., 2008).
This mixture was left for 30 min; the absorbance of the colored
filtrate obtained was determined at 660 nm using the spectrophotometer. The contents of As and Cd in sludge with and
without washing were determined on the basis of the standard method of the soil contamination countermeasures law
in Japan. The ICP-AES was used to determine As and Cd; other
multivalent metals were also determined for mechanism
analysis of P-max reduction by acid washing. Their analytical
error was within 10%.

2.3.

Pot experiment

Plant growth experiments with sludge samples were also

conducted for Japanese mustard spinach, in order to study the
accumulation of phosphates in plants and the effects on plant
growth. This experiment was conducted during autumn in a
greenhouse in Japan. At 20 days after seeding in a seedbed, the
Japanese mustard spinach plants were transferred to pots
containing a mixture of sample sludge and peat moss (50:50).
For sun-dried sludge and its washed sample, 3 pots each were
examined for 25 days and the average value was used for
evaluations. Plant growth was conducted with a phosphate
application ratio of 10 and 100 mg/stock. Above-ground plant
weight and leaf phosphate content after 25 days were determined to evaluate the effect of acid washing. In addition,
a control experiment was conducted without sludge.
The component substrates and their corresponding ratios
for this control sample were as follows: a horticultural
substrate consisting of bark compost:dam dredged soil:peat
moss:expanded-vermiculite:perlite:Kanuma-pumice:Hyuga
soil 32:18:10:10:10:10:10, was used here.

3.

Results and discussion

3.1.

Aluminum removal from sludges

To study the effect of various pH acid washings on aluminum

removal from sludges, the percentage removal (extraction) of
aluminum was determined for both thickened sludge and

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w a t e r r e s e a r c h 6 0 ( 2 0 1 4 ) 7 5 e8 1

sun-dried sludge. The aluminum contents of each untreated

thickened sludge and sun-dried sludge were 34 and 69 g/kg,
respectively; the percentage removal was calculated based on
this amount in the untreated sludges. Theoretically,
aluminum is mostly ionized and dissolved as aluminum ion at
pH 3.5 (Panias et al., 2001), as shown in the presence of Al(OH)
2
and Al3, the main soluble aluminum speciation, at different
pH in Fig. 1 (Mortula et al., 2009). However, as shown in Fig. 1,
the removal percentage of aluminum from the sun-dried
sample was only 5% even at pH 3, and pH 1 is necessary to
achieve over 80% removal. In contrast with the thickened
sludge sample, around 70% of aluminum removal was
possible even at pH 3.
Fig. 2 shows the change in efficiency of aluminum removal
from sludge by acid washing at pH 3, following 5 days of sun
drying. The percentage of aluminum removal by acid washing
decreased with increased drying time of sludge. Mortula et al.
(2009) reported the effects of three drying methods on leachability of aluminum from WTR and concluded that drying had
no effect. However, their pH condition was around 5 and there
was very low leachability in our result, with no difference
between thickened and sun-dried sludge (Fig. 1). This indicates that the difference in leachability can be attributable
to the aluminum leachable at certain pH. The water content
change in the sample sludge is also shown in Fig. 2; the
decrease in percentage removal seems to occur with decrease
in water content. Okuda and Inoue (1959) reported fixation of
adsorbed aluminum on kaolin, and Ashimura et al. (2005) reported the formation of Boehmite (Al(OH)O) from PAC in WTR
by storage or autoclave treatments. Such strong adsorption of
aluminum onto solid particles in WTR and/or aluminum
mineral (crystal) could be achieved by sun drying, and would
inhibit the acid extraction of aluminum from WTR. Although
there is the possibility of aluminum complexing with organics. Therefore, removal of organic materials from sundried sludge by oxidation with H2O2 (6 h reaction at solid/
liquid ratio of 3:100 with 10% H2O2 solution) was conducted at
pH 2.5; it decreased ignition loss to 1% from 19%. However, the
aluminum removal percentage was 6.6%, almost the same as
the 7.3% for sludge before oxidization. This indicates that the
decrease in aluminum removal percentage by sun drying does

Fig. 1 e Percentage removal of aluminum from thickened

sludge and sun-dried sludge by acid washing at several pH
values.

Fig. 2 e Change of aluminum removal by washing at pH 3

and water content during sun drying.

not result from complexing with organics. PAC directly

adsorbed to solid particles during coagulation, not through
organic materials (Budd et al., 2004), which supports the main
reason other than binding by organic materials. Here, the TOC
concentration of washed solution at pH 2.5 was 165 mgC/L,
representing TOC removal from the sun-dried sludge at 3% of
extractable TOC by 1 N acid. The organic contamination in
washed solution may not be problematic in reusing regenerated PAC for wastewater, but it should be removed in PAC for
drinking water treatment; the two-step purification method
(Sekine, 2001), as shown previously, could be used for that.
To evaluate the effect of aluminum removal onto the
improvement of phosphorus supply from washed sludges, Pmax was compared in sludge samples with and without
washing. Results are shown in Fig. 3, and the P-max of
thickened sludge was decreased to 22 and 3 mg/g from initial
23 mg/g by washing at pH 3 and 1, respectively. The trend was
same in sun-dried sludge having 30 mg/g of initial P-max, and
it decreased to 26 and 12 mg/g after washing at pH 3 and 1,
respectively. Almost no reduction of P-max by washing at pH 3
was observed for the sun-dried sludge, while 70% of
aluminum was removed at pH 3 in case of thickened sludge
(Fig. 1). Codling et al. (2002) reported the WTR based on ferric

Fig. 3 e P-max change of thickened sludge and sun-dried

sludge washed at different pH.

79

w a t e r r e s e a r c h 6 0 ( 2 0 1 4 ) 7 5 e8 1

coagulant shows low phosphorus availability (expecting high

P-max), and Gibbons and Gagnon (2011) suggested that calcium contributes to phosphate adsorption to WTRs, in addition to aluminum. Fig. 4 shows the removal percentage of Ca,
Fe and Al by washing, and P-max value at pH 2.5 and 3.0 where
the drastic P-max difference was observed in thickened
sludge. There was good relation only between iron removal
and P-max decline, indicating iron would be the main
component in controlling phosphate adsorption (Gibbons
et al., 2009; Codling et al., 2002). P-max of sun-dried sludge
at pH 1 was about 4 times that of the thickened sludge sample,
even though the residual aluminum content was almost the
same (Fig. 1). This indicates that sun drying increases the
phosphate-adsorption capacity of sludge. It would be caused
by the chemical and/or physical effects. Sun-dried sludge
might have higher residual iron than thickened sludge after
washing at pH 1, because of the fixation of iron with similar
mechanism with the aluminum stabilization by drying. One
possibility is the decrease in specific surface area of sludge
particles by aggregation. Makris et al. (2004) reported the
reduction of sludge specific surface area through significant
structural changes in a WTR after thermal incubation at 70  C.
Subsequently, Agyin-Birikorang and OConnor (2009) determined the decrease in Al reactivity, i.e., removal ability from
WTRs by 5 mM oxalate, with aging time, explaining it as a
result of the decrease in specific surface area. Another possibility is the production of adsorption sites for phosphate
during sun drying, i.e., sun drying increases sludge particle
fixation and the space between particles might function as
phosphate adsorption sites.

3.2.

Properties of washed sludge

Properties of sun-dried sludge and sludge washed at pH 1 were

determined for the use in plant husbandry. Sun-dried sludge
was selected for this evaluation in order to evaluate the more
difficult sample for such use; reports showed 40% lower yield
of Japanese mustard spinach at 50% addition of sun-dried
sludge obtained in the same prefecture as granite soil

(Masunaga et al., 2013). Lower pH was necessary for the sundried sludge (Fig. 1) and it had higher P-max (Fig. 3 and
Table 1) after washing at pH 1 than did thickened sludge. The
results are summarized in Table 1. At first, the available
phosphorus increase from 2.2 to 8.2 mg/g by acid washing was
obtained by the decrease of P-max. This available phosphorus
represents the supply capacity of phosphorus added as fertilizer to plants, and was found to confirm the increase in
phosphate supply capacity by acid washing. This fourfold increase in available phosphorus is big advantage for the reusability of washed sludge, because it can be efficiently used as
fertilizer. As to reusability of washed sludge, another important property is hydraulic conductivity, because it affects
growth and development of every plant. Hydraulic conductivity was drastically decreased by acid washing, from
9.32 mm/s to 0.03 mm/s. This could be due to the decrease in
particle size of agglomerate in sun-dried sludge. This value is
comparable with that of silt particles of 5e75 mm diameter
(Abeele, 1986). The carbon amount in sludge was decreased to
40% by the acid washing, indicating another possibility of a
binder role of some organic materials, and it can be removed
by acid washing. Even though the appropriate value depends
on the kind of plant, hydraulic conductivity should generally
not be lower than 0.1. Therefore, permeability control was
tried using the granulation technology. Results showed that
permeability could be recovered to 9.32 mm/s by the granulation of washed soil to around 10-mm size by mixing with 1 h
heating at 100  C and 300  C. This indicates that permeability
can be controlled to a suitable value by the granulation technology during drying, even after decrease by acid washing.
Because of acid washing, As content in sludge decreased
from 8.8 to 1.3 mg/kg and Cd content decreased from 0.5 to
0.1 mg/kg. Even though both values before washing were
lower than the standards of the Fertilizer Control Law (FCL) of
Japan, the decrease to less than 1/10 of FCL increased the
safety for use on garden plants. Soil pH decreased from 6.5 to
6.0, and EC increased from 0.3 to 1.2. Because soil pH and EC
above 7.0 and 1.5 mS/cm, respectively, cause excessive accumulation of nutrients, and have an adverse effect on plants,
these values were in appropriate ranges. CEC is associated
with fertilizer response for cationic nutrients like ammonium
and calcium ion, and there was a 20% decrease. Both values
before and after washing were in generally appropriate
ranges.

Table 1 e Properties as soil before and after acid washing.

Fig. 4 e Difference in percentage removal of three metals by

acid washing at pH 2.5 and 3.0, and P-max of washed
sludge (thickened sludge).

P-max (mg/g)
Available
phosphorus
(mg/100g)
Permeability
(mm/sec)
As (mg/kg)
Cd (mg/kg)
Soil pH
EC (mS/cm)
CEC (meq/100g)

Standards
in FCL

Before acid
washing

After acid
washing

e
e

29.2
2.2

12.2
8.2

e
50
5
e
e
e

9.32
8.8
0.5
6.5
0.3
17

0.06
1.3
0.1
6.0
1.2
12

80

w a t e r r e s e a r c h 6 0 ( 2 0 1 4 ) 7 5 e8 1

Table 2 e Leaf size and fresh weight of plant top and phosphate content in plant body after 25 days growth in soil-mixed
sludge with acid washing (at pH 1) or without (sun-dried). Values in parentheses show standard deviation in three
samples.
Application rate (mg-P/stock)
Acid washing
Plant weight of above-ground (g/stock)
Average leaf width (cm)
Phosphate content of leaves (mg/100 g)

3.3.

10

100

With
washing

Without
washing

With
washing

Without
washing

7.8
(2.3)
6.9
(1.8)
0.44

6.5
(0.5)
5.7
(0.0)
0.31

8.6
(0.9)
7.5
(0.4)
0.56

7.6
(1.1)
5.9
(0.1)
0.37

Pot experiments

Finally, the effect of sun-dried sludge acid-washed at pH 1 on

Japanese mustard spinach growth was studied. After 25 days
of growth with 100 mg/stock of phosphate application, using
sludge with and without acid washing, larger leaf area can be
observed in the group receiving sludge with acid washing, as
compared to that without washing. Table 2 shows leaf size,
plant weight of above-ground portion after 25 days of plant
growth in the soil mixed sludge with and without acid
washing; their standard deviations are also shown. The
average weight per stock with washed sludge was also heavier
than that without washed sludge, and the average width of
leaves in the washed sludge was wider than in unwashed
sludge. On the basis of Students t-test, the average width of
leaves with a phosphate application ratio of 100 mg/stock with
acid washing differed significantly from those obtained
without acid washing (p < 0.01), while there was no significant
difference in the other series. The phosphate content in the
leaves with acid washing was 40% higher than in leaves
without washing (only one analysis, so standard deviation
cannot be obtained). In addition, these plant properties (leaf
width, plant weight and phosphate content) in soil-mixed
sludge without acid washing are worse than those in the
control pod without sludge, even though the difference was
not significant. These results indicate that the decrease of
aluminum and the increase (improvement) of available
phosphorus in WTR were caused by the acid washingenhanced plant growth (Dayton et al., 2003; Ippolito et al.,
2003; Novak and Watts, 2004).

4.

Conclusions

The purpose of this study was to evaluate the effect of acid

washing pH and sun-drying process on aluminum removal
from WTR, and to evaluate the properties and plant growth
potential of washed sludge for a Brassicaceae vegetable, Japanese mustard spinach. The specific conclusions derived from
this study are as follows:
1) With thickened sludge, washing at pH 3 was sufficient to
reduce aluminum content by 80%, whereas sun-dried
sludge required washing at pH 1 for the same result.
2) The percentage of aluminum removal by acid washing
decreased during one week of sun drying.

Control
(without sludge)

6.9
(1.2)
6.1
(0.4)
0.50

3) The properties of the washed sludge were sufficient for

use in plowed soils; the inhibition of plant growth was
eliminated.

Acknowledgments
The authors thank Dr Esteban R. Min
o (Hiroshima University)
for his assistance, and Cervinia Manalo (Hiroshima University)
for her English check. The authors also greatly appreciate the
cooperation of the staff of the drinking water treatment plants
supplied sample WTR. This research was funded by a scientific
research fund (project) of the Association for Sustainable Material Cycles and Management of Hiroshima, Japan.

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