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Long 2021
Long 2021
Recycled use of municipal solid waste incinerator fly ash and ferronickel
slag for eco-friendly mortar through geopolymer technology
Wu-Jian Long a, b, c, *, Jun-kai Peng a, c, Yu-cun Gu c, d, Jin-lin Li a, c, Biqin Dong a, b, c, Feng Xing a, c,
Yuan Fang a, b, c
a
Guangdong Provincial Key Laboratory of Durability for Marine Civil Engineering, Shenzhen, 518060, Guangdong, PR China
b
Key Lab of Coastal Urban Resilient Infrastructure, MOE, Shenzhen University, Shenzhen, 518060, Guangdong, PR China
c
College of Civil and Transportation Engineering, Shenzhen University, Shenzhen, 518060, Guangdong, PR China
d
Department of Civil, Architectural and Environmental Engineering, Missouri University of Science and Technology, Rolla, MO, 65401, USA
A R T I C L E I N F O A B S T R A C T
Handling editor: Cecilia Maria Villas Bôas de Due to the rapid urbanization and increased population, the production of municipal solid waste incineration fly
Almeida ash (MSWI-FA) has become enormous and attracted attention worldwide. This study feasibly utilizes MSWI-FA as
an immobilization host to co-dispose of ferronickel slag (FNS) through geopolymer technology. Due to the high
Keywords: content of heavy metals in MSWI-FA and FNS, the leachate of the geopolymer was tested with two leaching
Municipal solid waste incineration
methods, in terms of acetic acid buffer solution method (AAM) and sulphuric acid & nitric acid method (SNM).
Fly ash
Results showed that the leaching concentrations of heavy metal ions in geopolymers were less than the upper
Ferronickel slag
Co-disposal limit of Chinese landfill standard. For instance, the value of Cu, Zn, and Cr leachate in geopolymers are far lower
Geopolymer than 100, 100, and 5 mg/L. Furthermore, various microstructural tests were performed to evaluate the stabili
zation/solidification behavior of MSWI-FA and FNS geopolymer, including electrochemical impedance spec
troscopy (EIS) test, scanning electron microscope (SEM)/energy dispersive spectrometer (EDS), X-ray diffraction
(XRD) test, and mercury intrusion porosimeter (MIP) test. The EIS results showed that geopolymer with the
combination of 60 wt% MSWI-FA, 20 wt% ground granulated blast furnace slag (GGBS), and 20 wt% silica fume
(SF) exhibited a compact and dense microstructure, which was beneficial to the physical encapsulation of heavy
metal ions. The MIP result also confirmed that the capillary pore structure of geopolymer is also developed. The
SEM, EDS, and XRD results showed that the C-A-S-H, Friedel’s salts, and NaCl were the main hydration products
in geopolymers. The C-A-S-H was capable contributed to improve the physical encapsulation of heavy metal ions.
Friedel’s salts were observed to adsorb heavy metal ions on its surface and had the good binding capacity of
heavy metal ions. Based on these findings, the feasibility of geopolymers are confirmed, which promote the co-
disposal of MSWI-FA and FNS and provide valuable information on the MSWI-FA based construction materials.
1. Introduction mass, and nearly 100% in organic matter content; (ii) the utilization of
the energy from the waste incineration; (iii) the effectiveness on
The worldwide production of municipal solid waste (MSW) has disposing of mass MSW (Caprai et al., 2020; Zheng et al., 2014). With
reached an enormous scale due to the rapid urbanization and increased the benefits of saving valuable landfill space and promoting energy
population (Diliberto et al., 2020; Geng et al., 2020). The production recycling, municipal solid waste incineration (MSWI) has been exten
magnitude of MSW is estimated at over 2 billion tons annually which sively applied in many countries and regions (Yu et al., 2020).
needs to be properly treated (Daniel Hoornweg, 2012; Gutberlet, 2015). However, MSWI generates a huge amount of waste by-products, i.e.
In the past decades, many methods have been developed to lower the bottom ash and fly ash, accounting for 5–30 wt% of the total weight of
environmental impact of MSW, such as landfill, compositing, and municipal solid waste (Yang et al., 2019). Noticeably, the MSWI-FA has
incineration (Huber et al., 2018). The incineration process has three been considered hazardous waste due to the presence of approximately
main advantages: (i) the reduction of MSW by 90% in volume, 70% in 3–5 wt% heavy metal ions (Zhang, S. et al., 2020). The production of
* Corresponding author. College of Civil and Transportation Engineering, Shenzhen University, Shenzhen, 518060, Guangdong, PR China.
E-mail address: longwj@szu.edu.cn (W.-J. Long).
https://doi.org/10.1016/j.jclepro.2021.127281
Received 25 November 2020; Received in revised form 8 March 2021; Accepted 22 April 2021
Available online 4 May 2021
0959-6526/© 2021 Elsevier Ltd. All rights reserved.
W.-J. Long et al. Journal of Cleaner Production 307 (2021) 127281
municipal solid waste incineration fly ash (MSWI-FA) is estimated to major advantages. Firstly, the cost of dispose of MSWI-FA and FNS
reach 6 million tons annually in China (Sun et al., 2016). Therefore, the decrease a lot since manufacturing this eco-friendly geopolymer does
disposal of MSWI-FA becomes urgent. Some treatments including ther not consume too much energies and resources (Zhang et al., 2020; Zhang
mal treatment, chemical and physical separation, and solid et al., 2020). Then, this work provides guide information on MSWI-FA
ification/stabilization (S/S) have been proposed to properly dispose of and FNS based construction materials which is a potential substitution
MSWI-FA (Luo et al., 2019). Among these methods, S/S is the most of Ordinary Portland Cement. It is valuable because he magnitude of
widely applied in the treatment of MSWI-FA due to the effective newly construction industry dramatically increased yearly and many
immobilization of heavy metals and low cost at disposing of mass haz raw materials such as stone, sand, and other mineral resources have
ardous waste. The S/S works through physically encapsulated and become overexploited (Wang et al., 2020).
chemically fixed hazardous materials inside the matrix in hydraulic Therefore, this study aims to co-dispose of MSWI-FA and FNS into
binders (Fan et al., 2018). Although ordinary Portland cement is the eco-friendly mortar through geopolymer technology. The mortar was
commonly used hydraulic binder in S/S practice, its production release prepared with a binder of alkali-activated MSWI-FA and fine aggregate
0.7t CO2 per tons and is responsible for global CO2 emissions by of FNS. Furthermore, the GGBS and SF were partly replaced MSWI-FA to
approximately 5–8% (Scrivener, 2014). Consequently, it is urgent to strengthen the performance and to assure the immobilization. Two kinds
find alternative low-carbon and high-efficiency methods to dispose of of toxicity characteristic leaching procedures including AAM and SNM
MSWI-FA. were employed to reveal leaching performance in acid rain environment
Geopolymer, also known as alkali-activated cementitious materials, and landfill leachate environment. The mechanical performance was
has been proposed to dispose of MSWI-FA (Cristelo et al., 2020b; Shiota accessed by a compressive strength test. The microstructural charac
et al., 2017; Tian et al., 2020; Xuan et al., 2019). The concept of geo teristic was analyzed by scanning electron microscopy (SEM)/elemental
polymers is to activated raw materials with high alkaline activators, spectral scanning (EDS), X-ray diffraction (XRD) analysis, and mercury
which form binders similar to ordinary Portland cement (Wang et al., intrusion porosimeter (MIP) analysis. Electrochemical impedance
2020). The high alkaline activator is usually selected with NaOH or spectroscopy (EIS) analysis was carried out to get the electrochemical
Na2SO3 and the raw materials are usually selected with aluminosilicates properties of geopolymers. The S/S mechanism of MSWI fly ash-based
ash with fine particle size (Zhang, P. et al., 2020). It has been proved that geopolymer as an immobilization host was discussed by synthetically
geopolymers can stably encapsulate heavy metal ions inside the analysis obtained results. The study can promote the application of
three-dimension network of cementitious hydration products (Cristelo MSWI-FA as an immobilization host material and provide a valuable
et al., 2020b; Huang et al., 2019). guide on the co-disposal of MSWI-FA and FNS.
Since the MSWI-FA exhibits pozzolanic properties, the MSWI-FA is
considered as the potential raw material of geopolymer (Liu et al., 2. Materials and methods
2020). One approach is to make geopolymers by co-disposing MSWI-FA
with other solid waste, such as red mud, sewage sludge, dehydrated 2.1. Raw materials
pyrophyllite, (Chen, P. et al., 2019; Cyr et al., 2012; Geng et al., 2020; Li
et al., 2019; Shiota et al., 2019), or with other pozzolanic waste, such as In this study, MSWI-FA and FNS were collected from a municipal
blast furnace slag (GGBS), fly ash, metakaolin, silica fume (SF) (Jin et al., waste incineration plant in Huizhou, Guangdong Province, China, and a
2016; Liu et al., 2018; Qian et al., 2006). The other approach (Cristelo smeltery in the same region, respectively. The GGBS and SF (Weishen
et al., 2020a; Kan et al., 2020; Liu et al., 2020; Zheng et al., 2010) is to Co., Ltd., China) were added as supplementary cementitious materials
directly use MSWI-FA as raw material (also known as precursors in and the deionized water was applied as mixed water in this study. The
geopolymer). Cristelo et al. (2020a) has reported that the overall per appearance of MSWI-FA, FNS, GGBS, and SF are presented in Fig. 1. The
formance including mechanical properties, durability, and leachability chemical composition of MSWI-FA, GGBS, and SF was determined by an
properties of MSWI-FA based geopolymer paste was better than X-ray fluorescence spectrometer (XRF, S4 PIOMEER, Germany’s Bruker
cement-based reference. And the main hydration products of AXS) and listed in Table 1. The physical properties of MSWI-FA, FNS
alkali-activated MSWI-FA hardened paste is combined phases of hydrous were listed in Table 2. The particle size distribution of MSWI-FA, GGBS,
alkali-aluminosilicate and calcium silicate hydrate (C–S–H) (Tian et al., and SF were determined by Mastersizer (Mastersizer 2000, Malvern, UK)
2020). Therefore, manufacturing the geopolymers based on MSWI-FA and were plotted in Fig. 2.
can not only immobilize the heavy metals of MSWI-FA but also bene The fineness modulus of FNS fine aggregate is 3.0 and ranges from
fits the utilization of MSWI-FA as construction materials. 0.1 mm to 4.75 mm. The gradations of FNS fine aggregate was matched
Ferronickel slag (FNS) is considered as the third-largest solid waste to standard sand according to Chinese standard GB/T 6003 (2012) and is
in China and the annual production exceeds 30 million tons in china (Gu showed in Fig. 2. The chemical composition of FNS mainly includes 49.1
et al., 2020; Saha et al., 2018). However, the utilization rate of FNS is wt% SiO2, 28.2 wt% MgO, and 10.1 wt% Fe2O3. The heavy metals in
only 10% and the rest is mostly sent to landfills (Xi et al., 2018). In the FNS are MnO and Cr2O3 with a mass content of 0.93 and 2.08,
nickel-metal melting plant, the course mineral, such as sulphide ores and respectively.
garnierite ores, is melted to extract nickel and then the residue is The alkali activation was selected with a mixture of sodium hy
naturally air-cooled or water quenched to form FNS (Polyakov, 2013). droxide (Guanghua Technology Co., Ltd., Shantou, Guangdong, China)
Previous studies (Nuruzzaman et al., 2020; Sun et al., 2019) showed that and liquid sodium silicate solution (Shengjing Ceramic Materials CO.,
FNS was feasibly used in concrete or mortar as aggregate, which showed Ltd., Zhaoqing, Guangdong, China). The chemical and physical prop
superior performance in workability, mechanics, and durability. For erties of the sodium silicate solution are presents in Table 3.
instance, Nuruzzaman reported that FNS was used in high strength
self-compacting concrete as fine aggregate. The concrete can meet the 2.2. Mix design and preparation
workability criteria of self-compacting concrete, and the mechanical and
durable properties were increased by the addition of FNS (Nuruzzaman The mix proportions of geopolymer are listed in Table 4. After pre
et al., 2020). It should be noticed that metals including Ni, Cr, and Mn liminarily mixing the raw materials, the alkali activation was added into
containing in FNS exhibit potential risk to the environment and human the mixture and stirred well to obtain a uniform paste. Then the paste
health (Cao et al., 2020). Therefore, it is feasible to use FNS as the was cast into a mold and was demoulded after curing for 24 h at stan
aggregate in construction materials, which effectively dispose of the dard curing condition with relative humidity no less than 90% and
solid waste. temperature of 25 ± 2 ◦ C according to ASTM C305. The samples were
Manufacturing MSWI-FA and FNS based geopolymer mortar has two then moved to a standard curing room for a specific time at 7 days and
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W.-J. Long et al. Journal of Cleaner Production 307 (2021) 127281
Table 1
Chemical composition of MSWI-FA, FNS, GGBS, and SF (wt%).
CaO SiO2 Al2O3 Fe2O3 MgO SO3 K2O Na2O Cl ZnO PbO CuO P2O5 TiO2 BaO
MSWI-FA 40.66 3.42 0.73 0.62 0.88 5.13 6.34 12.18 27.43 1.05 0.12 0.13 0.24 0.21 0.14
GGBS 39.81 31.86 16.53 0.43 6.89 0.04 0.54 0.33 0.01 1.23
SF 0.49 92.26 0.89 1.97 0.96 0.33 1.31 0.42
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W.-J. Long et al. Journal of Cleaner Production 307 (2021) 127281
Fig. 2. Particle size distribution: (a) MSWI-FA, GGBS, and SF and (b) aggregate gradations of FNS and standard sand.
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W.-J. Long et al. Journal of Cleaner Production 307 (2021) 127281
3.2.1. Compressive strength analysis MF80S20. This indicates that the synergistical use of GGBS and SF were
Fig. 4 shows the compressive strength of geopolymers at 7 and 28 better than their single addition. This effect may attribute to the syn
days. The reference mixture made with 100 wt% MSWI-FA had a ergistic effect by GGBS and SF.
compressive strength of 3.1 and 5.9 MPa at 7 and 28 days, respectively.
The low compressive strength could attribute to two reasons: 1) The 3.2.2. Leachates analysis
high w/b ratio of geopolymer. The high specific surface of MSWI-FA Two leaching methods including SNA and AAM were performed to
shown in section 2.1 requested more amount of water to ensure work simulate the leachate of geopolymer in acid rain pollution and landfill
ability, which may lead to the reduction of compressive strength. 2) The leachate, respectively. The heavy metals leaching of geopolymer is
amount of hydration product in geopolymer. MSWI-FA container less shown in Table 5 and the upper limit of three Chinese standards is also
amount of SiO2 and Al2O3 compared to slag. It may lead to less C–S–H presented to evaluate the leaching of heavy metal ions. As shown in
hydration product and reduction of compressive strengths. Table 5, the concentration of all the heavy metals species was far below
The compressive strength was significantly increased with the the upper limit of Standard GB18598-2019(2020) and GB5085.3–2007
increasing replacement of MSWI-FA at both 7 and 28 days of age. For (2020), indicating the geopolymer effectively stabilize the heavy metals
example, replacing MSWI-FA with the 20 wt% GGBS and SF increased leaching. Physically, the geopolymer is formed by the three-dimensional
28 d compressive strength by 155% and 201%, respectively. This can be aluminum silicate network structure, which consists of AlO4 and SiO4
attributed to the formation of C–A–S–H and the development of pore tetrahedral structure units. In the cavity of these units, the contaminants
structure. Adding GGBS supplement the essential Si and Al source. These could be seal stably. Furthermore, the network skeleton of geopolymer
aluminosilicate oxide dissolved as Al(OH)4- and SiO2(OH)2− 2 or SiO was reported to be of perfect stability under strong acid-base conditions.
(OH)3- and react with the Ca2+ in MSWI-FA to form C-A-S-H hydration (J.G.S. van Jaarsveld, 1998; Luna Galiano et al., 2011). Other than this
products, which contributes to the compressive strength (Chen et al., physical encapsulation, various double-layered hydroxides of calcium
2019; Cyr et al., 2012; Luna Galiano et al., 2011). Furthermore, SF has alumino/ferric hydrates such as ettringite (AFm) were reported to
been reported to enhance compressive strength by the pore filling effect chemically interact with metals and replaced these heavy metals with
due to the fine particle size, which can promote the development of interlayer hydroxyl.
compressive strength (Li et al., 2014). Moreover, the leachate pH value of geopolymer is showed in Fig. 5.
With the 20% replacement of MSWI-FA, the compressive strengths at Leachate pH value is the key factor for immobilizing heavy metal ions in
7 and 28 days of MF80G10S10 mixture were better than MF80G20 and cementitious materials. The relation between the leachate pH value and
leaching concentration of heavy metal ions is shown in Fig. 5. It should
be noticed that the pH value of the buffer solution of method AAM was
2.88 ± 0.05. After immersion and tumble, the pH values of the leachate
for all the specimens ranged from 4.5 to 4.9 which can be attributed to
the buffering capacity of alkali environment in geopolymer (Luo et al.,
2019; Zhang et al., 2016).
Overall, the pH value of the leachate was increased with the increase
in the replacement of MSWI-FA. The relations between leaching con
centration and pH values are the pH-dependent leaching. According to
previous work (Luo et al., 2019; Zhang et al., 2016), the elements such as
Zn, Pb, and Cr followed a cationic leaching pattern where the leached
concentrations decreased with an increased pH environment. The
leaching of this cationic pattern is controlled by the dis
solution/precipitation mechanism of corresponding hydroxides, car
bonate, or sulfate solids which is soluble in acid-stage and indissolvable
in alkalinity (Guo et al., 2017; Jiao et al., 2016; Luo et al., 2019).
Moreover, as shown in Fig. 5(a)–(c), the Zn, Pb, and Cr leaching
concentration were reduced with the increased pH value. However, the
leaching concentrations in MF80G20 and MF80S20 were higher than
those of MF80G10S10, which was due to the more compacted matrix in
MF80G10S10. The combined use of GGBS and SF in geopolymer can
facilitate the formation of C-A-S-H, which is beneficial to the physical
Fig. 4. Compressive strength of geopolymer.
encapsulation of heavy metals. This corresponding to compressive
5
W.-J. Long et al. Journal of Cleaner Production 307 (2021) 127281
Table 5
Leachability of geopolymer and the upper limitation in standard (mg/L).
Metal Type Concentration with Method SNA Upper Limitation Concentration with Method AAM Upper Limitation
a b
Standard 1 Standard 2 Standard 3c
Fig. 5. Leaching concentration of heavy metal ions according to pH value: (a) Zn; (b) Pb; (c) Cr; (d) Mn.
strength results. Fig. 5(d) shows that the leachate of Mn is independent benefit the physical encapsulation of heavy metals.
with the pH value. It should be noted that the electrochemical impedance of the overall
specimen cannot accurately estimate the internal microstructure of
3.2.3. EIS analysis geopolymer. Hence, the values of the electrochemical parameter Rct1 of
The EIS responses in the Nyquist format of geopolymer and the geopolymer were obtained by fitting with model Rs (Q1(Rct1W1))
electrochemical parameter Rct2 are shown in Fig. 6 and Table 6, (Q2(Rct2W2)). This model uses two individual elements (Rs (Q1
respectively. In Fig. 6, the diameters of the semicircles of the Nyquist (Rct1W1))) to simulate the charge interactions in both the pore solution
curves increase with the replacement of MSWI-FA by GGBS and SF. The and solid/liquid double phase, which precisely reflect electric response
relationship between electrochemical response at high or low fre inside the geopolymer. Rct1 represents the resistance of the charge
quencies in cementitious materials and physical properties have been transfer between the solid and liquid phases of geopolymer, which is
discussed in previous studies (Lizarazo-Marriaga et al., 2014; Song, affected by several physical factors including the type and concentration
2000). The electrochemical responses at high, intermediate, and low of ions in pore solution, porous structure, and the compactness of the
frequencies are respectively related to the solid phase (including hy matrix (Ball et al., 2011; Dong et al., 2014, 2016). In Table 6, the value
drated products and fine aggregate), pore network, and of Rct1 is increased with the increasing replacement of MSWI-FA by
electrode-electrolyte interface. Hence, the increased diameter of the GGBS and SF. This can be attributed to two reasons: (i) adding GGBS and
semicircle of the Nyquist curve corresponds to the dense pore structure SF firstly consume a large amount of OH− due to the pozzolanic effect
and compact matrix. This indicates that the pore structure and matrix of (Korde et al., 2020) and OH− is reported to be the most significant
specimens are effectively densified by the adding of GGBS and SF, which contributor to the pore solution conductivity (Snyder et al., 2003). (ii) as
6
W.-J. Long et al. Journal of Cleaner Production 307 (2021) 127281
7
W.-J. Long et al. Journal of Cleaner Production 307 (2021) 127281
Fig. 7. SEM image and EDS results of geopolymer: (a) ITZ of MF100; (b) ITZ of MF60G20S20; (c) halite crystal and corresponding EDS results in MF100; (d)
hydrocalumite and corresponding EDS results in MF80G20; (e) amorphous gel and corresponding EDS results in MF60G20S20.
and the porosity of geopolymer decrease. Meanwhile, the variation the heavy metals but also benefits from developing eco-friendly substi
trend of heavy metals leachate is correspondingly related to that of tute construction materials.
compressive strength. This indicates that compressive strengths and
porosity characterize the physical encapsulation of heavy metals, which 4. Conclusions
reflect on leaching performance. The microstructure performance shows
no clear difference which indicates the chemical binding effect of heavy This study investigates the feasible utilization of MSWI-FA as an
metals does not play the major roles in anti-leaching. Hence, the per immobilization host to dispose of FNS through geopolymer technology.
formance evaluation shows the feasibility of geopolymer. By recycled The GGBS and SF were used to partly replace MSWI-FA to strengthen the
use the MSWI-FA and FNS, it can not only decease the cost on dispose of performance of geopolymer. The mechanical performance, leaching
8
W.-J. Long et al. Journal of Cleaner Production 307 (2021) 127281
Fig. 9. Cumulative intrusion curve and particle pore distribution of geopolymer: (a) Cumulative intrusion curve; (b) Particle pore distribution.
Table 7
Summarization of performance of geopolymer.
Mix. ID MF100 MF90G10 MF90S10 MF80 MF80G20 MF80S20 MF60
G10S10 G20S20
9
W.-J. Long et al. Journal of Cleaner Production 307 (2021) 127281
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