Journal of Environmental Management 270 (2020) 110869

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Journal of Environmental Management

journal homepage: http://www.elsevier.com/locate/jenvman

Research article

Recycling dredged harbor sediment to construction materials by sintering

with steel slag and waste glass: Characteristics, alkali-silica reactivity and
metals stability
Yee Cheng Lim a, b, Yu-Jen Shih c, Kuang-Chung Tsai d, Wein-Duo Yang e, Chiu-Wen Chen b, **,
Cheng-Di Dong b, *
a
Institute of Maritime Science and Technology, National Kaohsiung University of Science and Technology, Kaohsiung City, Taiwan
b
Department of Marine Environmental Engineering, National Kaohsiung University of Science and Technology, Kaohsiung City, Taiwan
c
Institute of Environmental Engineering, National Sun Yat-sen University, Kaohsiung City, Taiwan
d
Department of Safety, Health and Environmental Engineering, National Kaohsiung University of Science and Technology, Kaohsiung City, Taiwan
e
Department of Chemical and Materials Engineering, National Kaohsiung University of Science and Technology, Kaohsiung City, Taiwan

A R T I C L E I N F O A B S T R A C T

Keywords: This work recovered the dredged sediment around Kaohsiung Harbor, Taiwan, for preparing lightweight ag­
Dredged sediment gregates (LWA), of which physicochemical properties as affected by the addition of basic-oxygen-furnace (BOF)
Basic-oxygen-furnace slag slag and waste glass were investigated. LWA properties included water absorption, particle density, compressive
Waste glass
strength, shrinkage, and microstructure of sintered pellets were evaluated to ensure feasibility of dredged harbor
Lightweight aggregates
Metal stability
sediment reutilization technique. Results showed that adding appropriate amount of glass powders (~7%) to the
Waste reduction mixtures of sediment and slag significantly reduced the water absorption (as low as 2.2%) of the sintered pellets
and increase the compressive strength (as high as 23.1 MPa) of LWA, which were found to be controlled by open
porosity and shrinkage. Excessive addition of glass (>10%) led to increase in internal pore sizes of the sintered
pellets, and thus reduced the compressive strength. The alkali–silica reactivity (ASR) of the LWA was innocuous
according to the ASTM C289 test. Sintering and glass addition improved the stability of heavy metal and
environmental compatibility of the LWA. The recycling of waste sediment, slag, and glass for LWA production
can provide an alternative for the disposal of dredge harbor sediment and has positive impact on waste reduc­
tion, which not only can reduce secondary contamination to the environment, but also can contribute to circular
economy.

1. Introduction
Sediment dredging is important routine harbor operation to main­
tain water ways for shipping (Lirer et al., 2017; Mymrin et al., 2017).
Annually about one million tons of sediments are dredged and disposed
from Kaohsiung Harbor, which is a largest international harbor in
Taiwan (Chen et al., 2017a, 2017b; TIPC, 2018). Low-polluted sandy
sediments can be directly used for land reclamation. Dredged materials
are mostly limited in construction applications due to poor bearing ca­
pacity, high chloride content, and high risk in secondary contamination.
Thus, dredged harbor sediments are commonly dumped into designated
ocean disposal site nearby, which potentially causes negative effects on
the marine environment (Chen et al., 2018, 2016; Manap and Voul­
voulis, 2015). An eco-friendly alternative plan for the disposal of
dredged sediments is needed. In previous studies, dredged materials
from river, lake and reservoir sediments have been well studied as raw
materials of lightweight aggregate (Chen et al., 2012; Huang et al.,
2016; Liu et al., 2018; Liu and Coffman, 2016; Peng et al., 2017; Tang
et al., 2011). However, few researches focused on marine sediments or
dredged materials from harbor. Therefore, in this study, the dredged
sediment from Kaohsiung Harbor, the fifteen largest international har­
bor worldwide was recycled and mixed with two other wastes, such as
basic-oxygen-furnace (BOF) steel slag and waste glass, to synthesize
lightweight aggregate.

* Corresponding author.
** Corresponding author.
E-mail addresses: cwchen@nkust.edu.tw (C.-W. Chen), cddong@nkust.edu.tw (C.-D. Dong).

https://doi.org/10.1016/j.jenvman.2020.110869
Received 6 March 2020; Received in revised form 6 May 2020; Accepted 27 May 2020
Available online 5 June 2020
0301-4797/© 2020 Elsevier Ltd. All rights reserved.
Y.C. Lim et al.
Lightweight aggregates (LWA) have been increasingly used in con­
crete for high rise buildings and large-scale construction. The use of
LWA in concrete can reduce the dead weight of structures due to low
density, thereby saving construction costs. The porous LWA can make
room partition, which is superior in thermal and acoustic insulation
(Boarder et al., 2016). Conventional LWA are composed of natural
minerals with low density; however, the sintering of expandable clay
could generate LWA (Aslam et al., 2017). Since raw material sources for
LWA production are becoming limited, wastes, recycled materials, and
industrial byproducts were recovered as alternatives. Recently, sewage
sludge, reservoir sediment, incinerator fly ash, bottom ash, and slag
have been reused as raw materials for the manufacture of LWA
(Gonza �lez-Corrochano et al., 2016; Han et al., 2015; Kockal and
Ozturan, 2011; Tang et al., 2011; Zhang et al., 2015). Among the above
materials, dredged harbor sediment is an ideal choise because of its
typical content of quartz, feldspar, and aluminosilicate minerals, which
are rich in SiO2, Al2O3, and alkaline earth oxides, essential ingredients
for manufacturing high quality LWA (Ayati et al., 2018).
With an increase in global steel demand for urban and industry
development, the generation of steel slag has become a critical issue
nowadays (Shi, 2004). Up to 3 million tons of steel slags, including
basic-oxygen-furnace (BOF) slags and electric arc furnace (EAF) slags,
are annually generated in Taiwan (CSC, 2017). These slags require
further disposal, but there are not enough places enough to treat or stack
those these industrial byproducts. Reuse and recycle of steel slags will
bring about economic benefits and reduce potentially negative impacts
to the environment. Steel slag, commonly rich in calcium oxides, can be
a suitable fluxing material for LWA manufacturing. Mixing ratio of
harbor sediment and EAF slag of 10/100 to 50/100 was found to suc­
cessfully manufacture the brick-like products and LWA (Wei et al.,
2014). Moreover, waste glass has also been reused as additives for LWA
manufacturing. The addition of glass powder, which contain Na2O, can
reduce required sintering temperature and enhance bloating ability of
LWA during sintering process (Kang et al., 2012; Wei et al., 2016). Tuan
et al. (2013) added waste glass into sewage sludge to make LWA and
showed increase of bulk density and failure point loading, and decrease
in water absorption of LWA. In our previous study (Lim et al., 2019),
waste glass powder was used as an additive for the manufacture of LWA
sintered from dredged harbor sediment mixed with BOF slags. However,
the effects of glass amount added on the physical properties of the LWA
were not well examined. The role of glass addition in the LWA
manufacturing remains relatively unknown especially for metals sta­
bility and alkali-silica reactivity.
This study aimed to study the effect of waste glass on the engineering
properties of LWA, which was made by waste sediment and slag
including water absorption, particle density, compressive strength as
well as microstructure of the core fragment. The potential of alkali–silica
reactivity of the LWA was evaluated using rapid chemical test. The
stability of heavy metals in LWA was examined by sequential extraction
to ensure that the LWA products are environmental friendly in further
practical applications. Economic consideration was also discussed to
evaluate the reuse technology for harbor sediment as construction ma­
terials, which make a win-win benefit in waste reduction and circular
economy.
2. Materials and methods
2.1. Raw materials
The recovered waste sediment, slag and glass powders were applied
to prepare green compact. The sediment sample was collected around
Kaohsiung Harbor (No. 63 Pier), Taiwan. The basic-oxygen-furnace
(BOF) slag was provided by CHC Resources Corporation, Taiwan. The
glass powder was obtained from crushed waste laboratory glass
container. All raw materials were oven-dried at 105 � C, sieved under 1.0
mm standard mesh, and stored in PE bottles for subsequent experiments.
2
Journal of Environmental Management 270 (2020) 110869
A Bruker S8 TIGER Series 2 wavelength dispersive X-Ray fluorescence
spectrometer was used to analyze the composition of sediment, slag and
glass samples. The thermal property was determined by a Hitachi STA
7200 simultaneous thermogravimetric/differential thermal analyzer
from 30 to 1100 � C in a N2 atmosphere with a heating rate of 20 � C
min 1. The grain size of raw materials was determined using a Beckman
Coulter LS230 laser diffraction particle size analyzer.
2.2. LWA preparation
The mass ratio of sediment/slag/glass was from 11/4/0 to 8.5/4/2.5,
in which mass content of BOF slag in each green pellet was fixed at 27%,
and glass mass content varied from 0 to 17%. The sample preparation
and firing procedure selected were based on Lim et al. (2019). A PET
tube was used as cylindrical mold. After well-mixed all raw materials,
15 g mixture for each green pellet was filled into the PET mold, and
shaped as cylinder with a dimension of 2.0 cm in diameter and 2.2 cm in
length using the pressure around 25 psi. The sequence of heating steps of
LWA included 24 h of curing at 105 � C, 10 min of preheating at 500 � C,
and 15 min of sintering at 1175 � C in a SNOL 6,2/1300 LSM01
program-controlled muffle furnace. Lim et al. (2019) suggested that
sintering at 1175 � C for 15 min after preheating at 500 � C for 10 min was
an optimal firing procedure to produce a sediment-based LWA with low
water absorption and high mechanical strength. Moreover, in the pre­
vious study (Lim et al., 2019), the LWA sample with 27% of BOF slag had
lowest values of water absorption, comparable low dry particle density
and highest compressive strength. Therefore, in this study, the BOF slag
contents was fixed at 27% in each green pellet, and the effects of glass
amount added on the performance of the sintered samples were
examined.
2.3. LWA physical properties
The engineering properties of sintered pellets, including particle
density, water absorption, compressive strength, open porosity,
shrinkage, and microstructure of core fragment, were studied. Water
absorption (W24h) was determined according to the standards method
(ASTM C127, 2015) and calculated using Eq. (1). Archimedes’ principle
was used to determine dry particle density (ρd) and apparent density (ρa)
(Cheeseman et al., 2005; Gonza �lez-Corrochano et al., 2016) using Eq.
(2) and Eq. (3), respectively. Open porosity (Po) was calculated using Eq.
(4).
Water absorption : W24h ¼
M1 M2
� 100 (1)
M2
M2
Dry particle: ρd ¼ (2)
M1 M3
M2
Apparent density: ρa ¼ (3)
M2 M3
� �
ρd
Open porosity: Po ¼ 1 � 100 (4)
ρa
where M1 is the weight of saturated-surface-dry sintered pellet (after
immersing in water for 24 h), M2 is the weight of oven-dry sintered
pellet, and M3 is the weight of immersed sintered pellet in water.
Compression testing machine (Summit, Taiwan) was used to test the
strength of sintered pellet at a 25 kN capacity in terms of the fracture
loading force per pressing area of sample (Wei et al., 2016). A digimatic
caliper was applied to measure the volume shrinkage of cylindrical
pellet after sintering (minimum indication 0.01 mm; Mitutoyo, Japan).
A FEI Quanta FEG 200 environmental scanning electron microscope was
used to observe the internal pore size and microstructure of sintered
pellet. The potential alkali-silica reactivity was assessed based on the
ASTM chemical method (ASTM C289; 2007).
Y.C. Lim et al. Journal of Environmental Management 270 (2020) 110869

The leaching concentrations of heavy metals was determined by Table 1

toxicity characteristic leaching procedure (TCLP) according to the Chemical composition of harbor sediment, BOF slag and waste glass.
standard method of Taiwan Environmental Protection Administration Harbor Sedimenta BOF slaga Waste Glassa
(Chen et al., 2015; NIEA R201.15C, 2007). Extraction fluid was 0.1 M
SiO2 53.9 9.86 65.3
acetate acid solution (pH 2.88). Leaching of sample with 20/1 of liquid Al2O3 17.4 2.25 –
to solid (L/S) mass ratio was performed for 18 h at 30 rpm using a rotary Fe2O3 7.15 22.6 –
agitation apparatus. The concentration of Ag, Ba, Cd, Cr, Cu, Ni, Pb, and Na2O 1.91 –c 11.4
Zn in the TCLP leachate were determined by a Thermo Scientific iCAP K2O 3.66 0.07 4.05
MgO 2.46 2.51 6.95
7400 Duo MFC inductively coupled plasma optical emission CaO 1.91 43.1 12.3
spectrometer. MnO 0.06 1.88 –
The stability of heavy metals was assessed by a modified Tessier’s SO3 1.82 0.27 –
five-step sequential extraction (Chen et al., 2013; Tessier et al., 1979). Cl 1.56 0.04 –
TiO2 0.94 0.39
The operating conditions and corresponding metal fractions are sum­ –
P2O5 0.26 1.76 –
marized as the following: Cr2O3 0.04 0.17 –
ZnO 0.05 – –
1. Exchangeable fraction (F1): sample was extracted using 1 M MgCl2 LOIb 6.8 15 <0.1
solution (pH 7) for 1 h. a
Unit: wt %.
2. Carbonate-bound fraction (F2): F1 residue was treated with 1 M b
Weight loss at 1000 � C using TGA/DTA.
sodium acetic solution (adjusted to pH 5 with acetic acid) for 5 h. c
–: non-detectable.
3. Fe–Mn oxides-bound fraction (F3): F2 residue was extracted using
0.04 M hydroxylamine hydrochloride in 25% (v/v) acetic acid at 96 3.2. Grain size distribution of raw material
� 3 � C for 6 h.
4. Organic matter-bound fraction (F4): Extraction of F3 residue was Fig. 1 shows the grain size distribution of the raw materials. The
conducted within 0.02 M nitric acid and 8.8 M H2O2 solution harbor sediment was sandy mud with a mean particle size of 27.9 μm,
(adjusted to pH 2 with nitric acid) at 85 � 2 � C for 2–3 h (twice), and D10, D50 and D90 of 3.0, 23.2 and 285 μm, respectively. The mean
followed by dilution with 3.2 M ammonium acetate in 20% (v/v) particle size of BOF slag was 131 μm with D10, D50 and D90 of 13.1, 190
nitric acid. and 626 μm, respectively. Previous studies suggested that raw materials
5. Silicate-bound fraction or called residual fraction (F5): microwave grinding into finer particles is beneficial to LWA manufacturing (Dondi
was applied to assist digestion with a mixture of concentrated acids et al., 2016). However, the BOF slag is hard and low abrasion with a
(HNO3/HCl/HF/H2O2 ¼ 9/3/3/2) using a CEM MARS-6 microwave hardness of 7.0–8.0 and a Los Angeles abrasion value of 17.6% (CSC,
system. 2017); thus, excessive grinding will result in additional energy con­
sumption. The waste glass was also crushed into powders with a mean
A Hitachi ZA-3300 polarized Zeeman flame atomic absorption particle size of 246 μm, and D10, D50 and D90 of 41.7, 345 and 973 μm,
spectrophotometer was used to determine the concentrations of Cd, Cr, respectively. Coarser waste glass powders readily melt, flow around the
Cu, Ni, Pb, and Zn collected in sequential extraction. sediment particles, and form continuous viscous phases that improve the
sintering reaction (Wei et al., 2011).
3. Results and discussion

3.1. Chemical composition of raw material 3.3. Thermal behavior of raw material

The mass ratio of sediment/slag/glass in the raw material affects the Fig. 2 shows the thermal behavior of the raw materials. The initial
content of SiO2, Al2O3 and flux in the mixture for LWA manufacturing, weight loss of harbor sediment was 1.1% from ambient temperature to
which are important factors of LWA (Liu et al., 2018; Tsai et al., 2006). 200 � C, which was attributed to the loss of remaining moisture (Fig. 2A).
Raw materials containing 52–78% of SiO2, 10–25% of Al2O3, and 8–28% Removals of organic matters and structural water from the mineral
of fluxing contents (the sum of Fe2O3, MgO, CaO, Na2O, and K2O) have
been proposed to be suitable for LWA manufacturing (Cougny, 1990;
Riley, 1951). Table 1 lists the primary chemical composition, expressed
in oxide form, of the raw material used in this study. The main
composition of harbor sediment was SiO2 (53.9%) and Al2O3 (17.4%),
followed by Fe2O3 (7.15%) with minor components such as K2O
(3.66%), MgO (2.46%), CaO (1.91%), and Na2O (1.85%). The loss on
ignition (LOI) of the harbor sediment was 6.8%. Therefore, this work
fabricated LWA with density higher than those made from organic
matter-rich sewage sludge because of low LOI (Franus et al., 2016;
Gonza �lez-Corrochano et al., 2016). The BOF slag was mainly composed
of CaO (43.1%), Fe2O3 (22.6%), and SiO2 (9.86%). Its LOI was 15.0%.
The role of BOF slag in the LWA manufacturing is a fluxing material (Lim
et al., 2019). The waste glass powder used in this study was soda-lime
glass, which was abundant in SiO2 (65.3%), CaO (12.3%), and Na2O
(11.4%). Thus, the addition of glass powders in raw materials decreased
sintering temperature because Na2O lowered the melting point of
aggregate, and promoted the formation of silicate structure inside LWA
during sintering (Wei et al., 2017).

Fig. 1. Grain size distribution of dredged sediment, BOF slag, and waste glass.

3
Y.C. Lim et al. Journal of Environmental Management 270 (2020) 110869

(Fig. 2B): one at 450–550 � C with a 1.3% weight loss due to dehy­
droxylation of Ca(OH)2 (Khachani et al., 2014), and other in the
700–825 � C range as result of CaCO3 decomposition (Garea et al., 2003),
with an 7.6% weight loss. The weight loss of waste glass was less than
0.1% from ambient to 1100 � C (Fig. 2C).

3.4. Characteristics of sintered LWA

The key engineering properties of LWA are dry particle density,

water absorption, and compressive (crushing) strength. Typically, dry
particle density not higher than 2.0 g cm 3 is commonly classified as
LWA (Ayati et al., 2018). As shown in Fig. 3A, the dry particle density of
the sintered pellets showed an increasing trend from 1.72 to 2.07 g cm 3
when the glass addition was increased from 0 to 17%. Except those with
17% of glass addition (i.e. the samples with a mass ratio of sed­
iment/slag/glass of 8.5/4/2.5), dry particle density of the sintered pel­
lets prepared in this study all keep in value lower than 2.0 g cm 3, which
are qualified as LWA. The sintered pellets which contain more glass
would be denser and relatively higher in dry particle density because the
waste glass contains less LOI than the harbor sediment.
A general water absorption of LWA used in concrete was less than
18% (Ayati et al., 2019; Wei et al., 2014). The absorbed water in LWA
strongly affected the pozzolanic reaction of the cement, as well as the
curing time and concrete performance (Amorim et al., 2012). As shown
in Fig. 3A, all LWA samples prepared in this study showed water

Fig. 2. TGA and DTA curves of (A) dredged sediment, (B) BOF slag, and (C)
waste glass.

(weight loss of 1.0%) accompanied with a broad exothermic peak

occurred in the 200–450 � C range (Qi et al., 2010). Decomposition of
carbon and sulfur compounds with a weight loss of 4.4% occurred from
450 to 900 � C, accompanied by endothermic changes extended to 1100
�
C (Xu et al., 2008). Further weight loss (0.73%) from 900 to 1100 � C
may be caused by alkali metal sulfate decomposition (Bethanis et al.,
2002). A small exothermic peak at temperature up to 1050 � C may be
evidence for the formation of spinel-type aluminosilicate phase and
primary mullite (Conconi et al., 2019). In contrast, two major weight Fig. 3. Variation of the physical properties of LWA with different glass content.
losses accompanied with endothermic peaks were observed for BOF slag (A) Apparent density, dry particle density and water absorption; (B)
Compressive strength and shrinkage.

4
Y.C. Lim et al.
absorption less than 18%. Among those, the LWA sample without glass
addition had a relatively higher water adsorption of 14.6%. When the
glass addition was increased to 7% (i.e. the samples were prepared from
a mass ratio of sediment/slag/glass of 10/4/1), the water absorption
dropped sharply to 3.45%. The lowest value of water absorption
(2.24%) was for the LWA sample with 17% of glass addition. It is
concluded that increasing percentage of glass would eliminate water
absorption. Wei et al. (2011) suggested that the LWA to be incorporated
in concrete should have minimum water absorption, even though water
absorption promotes internal curing and benefit to concrete mechanical
properties (Bogas et al., 2012). The waste glass contains up to 11.9% of
Na2O and the eutectic mixture of Na2O and SiO2 has a relatively lower
melting point (Meshalkin and Kaplun, 2003), which can effectively
generate more viscous glassy phases to smoothen the LWA surface
roughness and seal the pores, consequently shielding external water
from entering into the interior of the LWA. Therefore, there are good
linear relationship between water absorption and open porosity (r ¼
0.99, p < 0.01, n ¼ 18) (Fig. 4A). Moreover, when the addition of glass
was increased to 7%, the apparent density sharply decreased (Fig. 3A),
indicating gradually close-up of pores inside the sintered pellets (Dondi
et al., 2016).
Fig. 4. Correlation of the physical properties of LWA. (A) Water absorption vs.
open porosity; (B) Compressive strength vs. shrinkage.
5
Journal of Environmental Management 270 (2020) 110869
Compressive strength is another important engineering property of
LWA, which affects its practical application in engineering construction.
High-strength LWA can be used for structural buildings and bridges,
while LWA with weaker strength can be applied to non-structural room
partition with great sonic and fire resistance, soilless cultivation in
agriculture, or filter bed for water treatment (Ducman and Mirti�c, 2009).
As shown in Fig. 3B, the compressive strength for the LWA sample
without glass addition was relatively low at 19.2 MPa; meanwhile, the
strength obviously increased with the addition of waste glass, and
reached the highest level (23.2 MPa) when the glass added was up to
7%. A relatively high amount of SiO2 in the waste glass can promote
complete silicate structure formation inside of LWA; moreover, the glass
readily melts to form a viscous phase around the sediment particles,
consequently thickening the inter-pore crystalline phases and shrinking
the pores inside of LWA (Mao et al., 2019; Wei et al., 2011). However,
when the addition of waste glass was increased from 7 to 17%, the
compressive strength of the LWA samples decreased noticeably. For the
LWA sample with 17% of glass addition, its compressive strength
decreased to16.3 MPa, which was lower than those LWA without glass
addition (Fig. 3B).
Fig. 5 shows the ESEM morphology of the core fragment of the LWA
samples. Fine pores were evenly distributed in the LWA sample with 7%
of glass addition (Fig. 5C), while the core fragment of the sintered pellet
without glass addition was relatively rough (Fig. 5A). When the glass
addition was greater than 10%, the pores inside the LWA were inter­
connected and formed larger pores (Fig. 5D–F). As shown in Fig. 5D,
some pores inside the LWA sample with 10% of glass addition reached
800 μm, and as large as 1.7 mm inside the sintered pellet with 17% of
glass addition (Fig. 5F). Thus, the LWA with more glass would have
expanded pore sizes. More glass addition can generate more viscous
phases with lower viscosity to effectively trap the bloating gases,
thereby resulting in more porous structure inside LWA (Tuan et al.,
2013). Wei et al. (2011) reported that sintered pellets prepared under
higher sintering temperature and more glass additive led to the forma­
tion of larger pores inside the LWA products, while the LWA prepared
with less glass additive were characterized by finer internal pores in the
fractured cores. With respect to compressive strength of the LWA in this
study, an increase in internal pore sizes appear to have caused a decrease
in compressive strength. A strong linear relationship between the
compressive strength and the shrinkage (r ¼ 0.89, p < 0.05) was
observed in this study (Fig. 4B). Some studies also showed that the
compressive strength of LWA was positively correlated to the dry par­
ticle density (Gonza �lez-Corrochano et al., 2016), however, no such
relationship was observed in the present study.
3.5. Assessment of alkali-silica reactivity
Most artificial LWA contain poorly crystalline silica and/or other
glassy alkali-sensitive minerals which rendered LWA potentially alkali-
reactive (Li et al., 2018). In particular, waste glass, which contains
high content of SiO2 and Na2O, may provide additional alkali to promote
the alkali-silica reaction. The possibility of alkali–silica reactivity must
be considered for all artificial aggregates, especially those prepared with
waste glass (Rajabipour et al., 2015). High silica content (~70%) and
amorphous structure of waste glass make the glass-based aggregates
potentially deleterious, and consequently spalling and loss of strength of
concrete in further construction application (Bumanis et al., 2013).
Therefore, the evaluation of the alkali-silica reactivity of LWA prepared
from mixtures of harbor sediment, BOF slag, and waste glass is impor­
tant for further use of LWA in construction structures. In this study, the
potential of alkali-silica reactivity of LWA were assessed according to the
rapid chemical method defined in ASTM C289 (2007). The Rc and Sc
values of the LWA sample are shown in Table 2 and Fig. 6. The Rc value
denotes the reduction of alkalinity of the NaOH solution due to
alkali-silica reactivity. The Sc value is the concentration of dissolved
silica.
Y.C. Lim et al.
Fig. 5. Microstructure of the core fragment of LWA prepared with different glass content. (A) 0%; (B) 3%; (C) 7%; (D) 10%; (E) 13%, and (F) 17%.
As listed in Table 2, the Rc and Sc values of the LWA samples with
different BOF slag contents (glass content fixed at 7%, BOF slag content
varied from 7 to 47%) decreased with increase in BOF slag content, in
which the Rc ranged from 150 to 45.1 mmol L 1, and the Sc ranged from
72.8 to 43.0 mmol L 1. Similarly, the Rc values of the LWA samples with
different glass content (BOF slag content fixed at 27%, glass content
varied from 0 to 17%) ranged from 130 to 70.2 mmol L 1, showing a
decreasing trend with increase of glass addition. The Sc values were
slightly varied in the range between 52.9 and 64.4 mmol L 1. According
to Fig. 6, it can be clearly seen that the LWA manufactured from the
mixture of harbor sediments, BOF slags and waste glass were all
innocuous from the point-view alkali–silica reaction. However, the
LWA, either prepared with sediment only or with a mass ratio of sedi­
ment/glass ¼ 14/1, showed considerably high sensitivity to alkalis
corresponding to relatively high Sc values. The above two LWA were
potentially deleterious for the alkali–silica reaction based on ASTM
C289 (Fig. 6). Unlike harbor sediment and waste glass, the BOF slag
contains lower content of SiO2, Na2O and K2O, thus the addition of BOF
6
Journal of Environmental Management 270 (2020) 110869
slag can contribute to reduce silica and alkali contents, leading to low
alkali-reactive of LWA.
In comparison, Table 2 shows the Rc and Sc values of the LWA, made
from perlite, expanded vermiculite, expanded clay, and waste glass,
investigated in Ducman et al. (2002) and Mladenovi�c et al. (2004).
Mladenovi�c et al. (2004) mentioned that the LWA made from expanded
glass and perlite showed high sensitivity to alkalis and serious decom­
position of the aggregate texture due to alkali-silica reaction corre­
sponding to much higher Sc values. The Sc value was considerably
higher in LWA made from expanded clay also; only the LWA made from
expanded vermiculite had low Sc value. Some researchers have also
observed that alkali-silica reaction often occurs in some artificial LWA,
especially in the case of perlite, expanded glass and expanded clay
(Collins and Bareham, 1987). However, Ducman et al. (2002) reported
that even though the reactivity of waste glass-based LWA in some cases
may cause alkali-silica reaction, no deleterious expansion was observed
in the accelerated mortar bar test. Chiou and Chen (2013) also reported
that when up to 20% of glass powder was added, the potential of
Y.C. Lim et al. Journal of Environmental Management 270 (2020) 110869

Table 2 alkali-silica reaction of reservoir-sediment based LWA increased, but

The Rc and Sc values of the studied LWA. Sc/Rc ratio all showed in the harmless zone.
Raw materials in mass ratio Rc (mmol Sc (mmol Reference
L 1) L 1)
Sediment BOF Glass
3.6. Assessment of heavy metals stability
Slag

15 0 0 85.0 88.2 This study Table 3 shows the concentration of Ag, Ba, Cd, Cr, Cu, Ni, Pb, and Zn
14 0 1 79.8 78.5
13 1 1 150 72.8
in the leachate were <0.005, 0.02–0.23, <0.005, 0.70–1.08, 0.06–0.14,
12 2 1 135 68.2 0.12–0.16, 0.05–0.07, and 0.20–0.34 mg L 1, respectively, which were
11 3 1 110 65.4 all far below Taiwan regulatory standards for waste recycling and
10 4 1 120 58.4 harmful materials management. Results show that the LWA prepared in
9 5 1 65.2 56.0
this study are safe for practical construction application. Except barium,
8 6 1 60.3 49.2
7 7 1 45.1 43.0 the leaching concentration of Cd, Cr, Cu, Ni, Pb, and Zn almost
decreased with increase in the amount of waste glass powder content of
11 4 0 130 64.0 This study
10.5 4 0.5 105 64.4
the LWA samples. The heavy metals in the LWA can be strongly bound to
10 4 1 120 58.4 the aluminosilicate or silicate frameworks during sintering, which
9.5 4 1.5 80.4 52.9 consequently lowered the leachability (Chang et al., 2007; Xu et al.,
9 4 2 75.1 62.3 2013). High SiO2 content in waste glass promotes formation of silicate
8.5 4 2.5 70.2 57.5
frameworks, which contributes to the stabilization of most toxic metals
Expanded clay 82.5 101.9 Mladenovic et al. in recycled materials, making them safe for reuse as construction ma­
Expanded glass 917.9 2890.0 (2004) terials (Mao et al., 2019).
Expanded vermiculite 671.9 17.3
Perlite 198.1 1420.4
A modified Tessier’s five-step sequential extraction (Chen et al.,
Waste glass (derived from 708.0 2366.6 Ducman et al. 2013; Tessier et al., 1979) was conducted to examine the partitioning of
bottles and window glass) (2002) heavy metals in the LWA before (green pellet) and after sintering.
Generally, the bioavailability and eco-toxicity of heavy metals associ­
ated with the different fractions generally decreases in the following
order: F1 (exchangeable fraction) > F2 (carbonate-bound fraction) > F3

Table 4
The percentage of each partition fraction of heavy metals in the LWA before and
after sintering.
Cd Cr Cu Ni Pb Zn
(%) (%) (%) (%) (%) (%)

Green pellet F1 100 0.04 0.5 0.3 2.1 2.3

before F2 ND 1.1 13.6 4.6 15.1 24.0
sintering F3 ND 43.5 16.1 23.7 56.9 44.8
F4 ND 3.6 56.5 6.0 7.2 4.5
F5 ND 51.8 13.3 65.4 18.6 24.4
Σ 100 48.2 86.7 34.6 81.4 75.6
F1–F4
Sintered LWA F1 ND ND ND ND ND ND
with 7% glass F2 ND 0.9 1.7 ND 0.4 2.2
F3 ND 19.5 2.7 3.9 1.8 2.7
F4 ND 1.8 3.4 ND ND 1.4
F5 ND 77.9 92.2 96.1 97.8 93.6
Σ ND 22.1 7.8 3.9 2.2 6.4
F1–F4
Sintered LWA F1 ND 0.4 ND ND ND ND
Fig. 6. The Rc-Sc diagram of LWA prepared from different proportion of with 17% glass F2 ND 1.3 1.5 0.5 ND 2.3
dredged harbor sediment, BOF slag and waste glass. F3 ND 4.6 2.5 0.3 ND 2.9
F4 ND 0.4 1.6 1.1 ND 0.5
F5 ND 93.3 94.4 98.1 100 94.4
Σ ND 6.7 5.6 1.9 ND 5.6
F1–F4

ND: non-detectable.

Table 3
The TCLP leaching concentration of heavy metals for the LWA with different glass content.
Sediment Slag Glass Leaching concentration in leachate (mg L 1)

(in mass ratio) Ag Ba Cd Cr Cu Ni Pb Zn

11 4 0 ND 0.02 ND 1.08 0.14 0.16 0.07 0.34

10.5 4 0.5 ND 0.05 ND 0.91 0.11 0.16 0.07 0.28
10 4 1 ND 0.14 ND 0.88 0.10 0.15 0.07 0.27
9.5 4 1.5 ND 0.21 ND 0.84 0.09 0.13 0.06 0.27
9 4 2 ND 0.22 ND 0.77 0.07 0.13 0.06 0.21
8.5 4 2.5 ND 0.23 ND 0.70 0.06 0.12 0.05 0.20

Taiwan legal limit for waste recycling 5 100 1 5 15 – 5 –

ND: non-detectable.

7
Y.C. Lim et al.
(Fe–Mn oxides-bound fraction) > F4 (organic matter-bound fraction) >
F5 (residual). As shown in Table 4, the non-residual concentrations (the
sum of F1, F2, F3, and F4) of the green pellets (sample was prepared
from a mass ratio of sediment/slag/glass of 10/4/1) were 0.18, 139,
58.2, 7.8, 20.9, and 159 mg kg 1 for Cd, Cr, Cu, Ni, Pb, and Zn,
respectively. In particular, Cd has the highest concentration in F1, Cu
has the highest concentration associated with the sum of F2, F3, and F4,
Cr and Ni have the highest concentration in F3 and F5, Pb and Zn have
the highest concentration associated with the sum of F2 and F3. When
the LWA after sintered at 1175 � C, the concentration of Cr, Cu, Ni, Pb,
and Zn in the sintered pellet were mainly associated with the residual
fraction (78–100%). Cd also fell below the detection limit. Sintering at
high temperature is effective immobilizing heavy metals, both in
forming part of the residual fraction of the LWA and volatizing some
elements, especially Cd (Gonzalez-Corrochano et al., 2012). Compared
to the green pellets, the non-residual fraction (the sum of F1, F2, F3, and
F4) of the LWA after sintering was significantly reduced, 100%–0% for
Cd, 48%–22% for Cr, 87%–8% for Cu, 35%–4% for Ni, 81%–2% for Pb,
and 76%–6% for Zn, indicating that the sintering process enhanced the
stabilization of heavy metals. Gonzalez-Corrochano et al. (2012) re­
ported that part of heavy metals merge into the residual faction of LWA
and formed crystalline structure of neo-formed feldspars and minerals of
spinel group during sintering. However, Cr proportion (~19%) is high in
the fraction of Fe–Mn oxides (F3). Chang et al. (2007) reported that Cr
compounds in LWA were converted to more soluble or more extractable
forms after sintering. It is probably that chromium compounds need a
higher temperature to reconstitute its crystallinity and bonding phase
into a residual structure. When the glass content of LWA was increased
to 17% (i.e. the sample was prepared from a mass ratio of sed­
iment/slag/glass of 8.5/4/2.5), the residual fraction of heavy metals in
the LWA were higher than those of LWA with 7% of glass addition,
especially Cr which residual fraction increased from 78% to 93%,
indicating that glass addition enhanced the stability of heavy metals in
the LWA, which improved the environmental compatibility in further
practical application of LWA.
3.7. Economic considerations
Current the cost of ocean dumping for dredged sediment is approx­
imately US15/ton including government official fee and disposal
expense. It is expected to increase significantly in the future, which
becomes a significant potential cost for harbor operation. Landfill
disposal cost also is as high as US250/ton. On the other hand, there have
no commercial production of LWA in Taiwan. The import price of LWA
is typically US80-US150/ton depending on grade, quantity and appli­
cation. Based on the lab work in this study, total cost of LWA production
is approximately US 170/ton. However, the lab work is limited in the
scale and efficiency of raw material treatment and LWA production.
Considering the manufacturing process of the actual factory scale, the
costs of milling, pelletizing and sintering could be reduced. Therefore,
the cost of LWA production in Taiwan local factory is estimated about
US40-US60/ton. These costs will vary depending on energy demand and
processing methods of milling, pelletizing and sintering. Also, the cost
for environmental protection such as air pollution control devices
should be considered. Due to sulfur and organic compounds were existed
in the harbor sediment and BOF slag (Table 1), the emissions of CO, CO2
and SO2 will be occurring during the sintering process up to 1000 � C
(Anagnostopoulos and Stivanakis, 2009). Air pollution control devices
should be installed to comply with government regulations. Moreover,
according to Wei et al. (2014), although the harbor sediment and steel
slag contain Cl , there is no environmental concern regarding the po­
tential hazard of dioxins/furans, probably destruction of dioxins/furans.
at high temperature. Although the cost of LWA production is 2–4 times
more than ocean dumping, LWA production from dredged sediments
will become increasingly viable when the disposal costs continue to
increase and the demand for lightweight concrete products increases.
8
Journal of Environmental Management 270 (2020) 110869
4. Conclusion
Results of this study showed the quality improvement of sediment-
based LWA by addition of waste glass. Appropriately adding glass
powders to the mixtures of dredged harbor sediment and BOF slag for
LWA manufacturing can effectively increase the compressive strength
and lower water absorption of LWA. High strength and low water ab­
sorption are highly desirable properties of LWA for further construction
application of lightweight concrete. But, excessive addition of glass led
to increase in internal pore size and reduced compressive strength.
Moreover, LWA made from harbor sediment and/or waste glass alone
may be potentially deleterious due to alkali–silica reaction. The addition
of BOF slag can reduce the alkali–silica reactivity, and improve the
safety in cement concrete application of LWA. Sintering process also
improve the heavy metals stability of LWA and enabled the recycling of
dredged harbor sediment, BOF slag and waste glass into LWA as non-
hazardous construction materials. Overall, making LWA using dredged
harbor sediment, BOF slag and waste glass is a national waste man­
agement which brings economic benefits and reduces secondary
contamination to the environment.
Declaration of competing interest
The authors declare that they have no known competing financial
interests or personal relationships that could have appeared to influence
the work reported in this paper.
CRediT authorship contribution statement
Yee Cheng Lim: Investigation, Data curation, Writing - original
draft. Yu-Jen Shih: Writing - review & editing. Kuang-Chung Tsai:
Validation, Resources. Wein-Duo Yang: Validation, Resources. Chiu-
Wen Chen: Conceptualization, Methodology. Cheng-Di Dong:
Supervision.
Acknowledgment
The authors appreciate CHC Resources Corporation for providing the
analytical instruments for TGA/DTA and compressive strength test as
well as BOF slag samples. We also thank Dr. T.H. Wang (Yuan Ze Uni­
versity, Taiwan) to help XRF analysis. Thanks also go to Shih-Kai Lin for
his works in lab. We sincerely appreciate reviewers’ comments and
suggestions in making this manuscript better. This work was sponsored
by ROC Ministry of Science and Technology (MOST-107-2622-E-992-
015-CC2).
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