Accepted Manuscript

Utilization of Red Mud in Geopolymer-based Pervious Concrete with Function of

Adsorption of Heavy Metal Ions

Xiao Chen, Yugang Guo, Song Ding, Hao Yu Zhang, Fei Yue Xia, Jie Wang,
Mingkai Zhou

PII: S0959-6526(18)32999-8

DOI: 10.1016/j.jclepro.2018.09.263

Reference: JCLP 14398

To appear in: Journal of Cleaner Production

Received Date: 05 May 2018

Accepted Date: 29 September 2018

Please cite this article as: Xiao Chen, Yugang Guo, Song Ding, Hao Yu Zhang, Fei Yue Xia, Jie
Wang, Mingkai Zhou, Utilization of Red Mud in Geopolymer-based Pervious Concrete with
Function of Adsorption of Heavy Metal Ions, Journal of Cleaner Production (2018), doi: 10.1016/j.
jclepro.2018.09.263

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 ACCEPTED MANUSCRIPT

Preparation of red mud-granulated blast furnace based geopolymer

pervious concrete and its adsorption of heavy metal ions

Xiao Chen1,*, Yugang Guo2, Song Ding3, Hao Yu Zhang4, Fei Yue Xia5, Jie Wang6, Mingkai Zhou7
1. State Key Laboratory of Silicate Materials for Architecture, Wuhan University of Technology, Wuhan 430070, China

School of Materials Science and Engineering, Wuhan University of Technology, Wuhan 430070, China

Email: chenxiao1981@whut.edu.cn

2. School of Materials Science and Engineering, Wuhan University of Technology, Wuhan 430070, China

Email: 9493118@qq.com

3. School of Materials Science and Engineering, Wuhan University of Technology, Wuhan 430070, China

Email: 1048350580@qq.com

4. School of Materials Science and Engineering, Wuhan University of Technology, Wuhan 430070, China

Email: 1322817519@qq.com

5. School of Materials Science and Engineering, Wuhan University of Technology, Wuhan 430070, China

Email: 236352641@qq.com

6. State Key Laboratory of Silicate Materials for Architecture, Wuhan University of Technology, Wuhan 430070, China

School of Materials Science and Engineering, Wuhan University of Technology, Wuhan 430070, China

Email: 358569956@qq.com

7. State Key Laboratory of Silicate Materials for Architecture, Wuhan University of Technology, Wuhan 430070, China

School of Materials Science and Engineering, Wuhan University of Technology, Wuhan 430070, China

Email: zhoumingkao@163.com
 ACCEPTED MANUSCRIPT

1 Utilization of Red Mud in Geopolymer-based Pervious Concrete with

2 Function of Adsorption of Heavy Metal Ions

3 Xiao Chena,b,*, Yugang Guob, Song Dinga, Hao Yu Zhanga, Fei Yue Xiaa, Jie Wanga,b, Mingkai Zhoua,b
4 a State Key Laboratory of Silicate Materials for Architecture, Wuhan University of Technology, Wuhan 430070, China

5 b School of Materials Science and Engineering, Wuhan University of Technology, Wuhan 430070, China

6 Abstract. Red mud (RM) is a kind of industrial solid waste that is difficult to utilize，but it
7 contains much alkali and has the ability of adsorbing some heavy metal ions. Due to these
8 characteristics, red mud could be used as a raw material to develop a geopolymer based pervious
9 concrete having rainwater purification function with granulated blast furnace slag (GBFS).
10 Following this, influence of different factors including RM content, the sodium hydroxide to
11 silicate (Na2O/SiO2) mole ratio, and the alkali concentration of the activator on the mechanical
12 properties and ability of adsorbing heavy metal ions were investigated. XRD, SEM and EDS were
13 then used to characterize the microstructure and morphology in attempt to reveal the mechanisms
14 on the strength formation and on the adsorption of heavy metal ions. The results show that both
15 the Na2O/SiO2 mole ratio and the alkali concentration of the activator had an obvious effect on the
16 strength of the RM-GBFS-based geopolymer pervious concrete, but little effect on the adsorption
17 of heavy metal ions. Moreover, with the increasing content of RM, the strength of the RM-GBFS-
18 based geopolymer pervious concrete decreased, while the adsorption of heavy metal ions
19 improved significantly. The possible reason for the excellent ability of adsorbing heavy metal ions
20 can be attributed to the composition of the hardened RM-GBFS-based geopolymer system
21 including geopolymeric gel, C-S-H gel with a lower Ca/Si ratio and some raw RM particles that
22 have great ability of adsorbing heavy metal ions. As the compressive strength at 28 d of the RM-
23 GBFS based geopolymer pervious concrete (containing 30 wt% RM in the geopolymer) can reach
24 18.53MPa, it can applied in the light road pavement in China, and this pervious concrete has been
25 demonstrated to have the function of rainwater purification due to its higher removal of heavy
26 metal ions from solution that can reach 53 % to 77 %. Therefore, it can be concluded that it is
27 feasible to employ RM for manufacturing geopolymer-based pervious concrete with function of
28 rainwater purification.
29 Key words. Pervious concrete; Geopolymer; Red mud; Adsorption; Heavy metal ions
30
31 1. Introduction
32 Red mud (RM) is the byproduct of alumina extraction via the Bayer process (Ke et al., 2015)
33 and the amount of its discharge is huge (Brunori et al., 2005). For each ton of alumina produced,
34 up to 1.5 tons of RM is generated (Liu et al., 2016). The aluminum production of China ranks first
35 in the world, therefore, China is also the largest RM producer in the world. The cumulative
36 amount of RM in China has exceeded 350 million tons. In 2016, China’s RM discharge was about
37 80 million tons (Liu et al., 2014). The pH of RM is always between 9.2 and 12.8 because of the
38 addition of hydroxide (NaOH) in this process (Grafe et al. 2011; Liu et al., 2017). The high alkali
39 content makes it possible to use the RM in alkali-activated materials or geopolymer. Some studies
40 investigated the use of RM as a part of an aluminosilicate material to prepare a geopolymer (Li et
41 al., 2017; Ye et al., 2016; Geng et al., 2017; Hajjaji et al., 2013; Ye et al., 2016; Kaya et al.,
42 2016). Furthermore, RM always has a large specific surface area, which is between 11.65 m2/g
43 and 30.72 m2/g (Liu et al., 2016), thus it can also be used as adsorbent. Many studies have

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1 indicated that RM has a significant adsorption effect for pollutants in aqueous solution, such as
2 heavy metal ions (Khan et al., 2015; Zhou et al., 2017; López-García et al., 2017; Lata et al.,
3 2015 Skin et al., 2016 ) and dyes (Hu et al., 2018; Wang et al., 2005).
4 Pervious concrete will be widely used for urban pavement in the future because it reduces the
5 risk of flash floods (Rahman et al., 2015) and increases water runoff (Nnadia et al., 2015)0. Thus,
6 pervious concrete can be used as part of an effective storm water management strategy
7 (Chandrappa et al., 2016) to collect, store, treat, redistribute, and recycle water (Scholz et al.,
8 2007). However, nonpoint pollution can be caused by stormwater and the pollutants (both natural
9 and man-made) will be carried into natural water bodies, such as seas, rivers or lakes (Thomle,
10 2010). It has been reported that the runoff contains COD (Chemical Oxygen Demand), TSS (Total
11 Suspended Solids), TN (Total Nitrogen), TP (Total Phosphorus) and some heavy metal ions (Fe,
12 Zn, and Cu) (Li et al., 2015). A study by Ellis showed that the contents of Cd, Cu, Pb, and Zn in
13 water bodies that come from rainwater are 46 %, 78 %, 47 %, and 13 % of the total contents of the
14 corresponding elements in the water bodies, respectively (Ellis et al., 1987).
15 Fortunately, pervious concrete can improve the quality of stormwater thanks to its porous
16 characteristics (Thomle et al., 2010). Some studies have investigated the water purification effects
17 of pervious concrete in recent years. The abilities of coarse aggregate, Portland cement, and fly
18 ash for the removal of heavy metal ions in solution were studied by Holmes et al., 2017. A study
19 focused on the pollutant adsorptive capacity of cement, silica sand, and aggregate found that
20 cement had the highest adsorptive capacity for road runoff pollutants (Wang et al., 2016). Soto-
21 Perez et al., 2016 studied the pollution control potential of pervious concrete with fly ash and
22 found that it could remove 72.4-77.9 % of fecal coliform and 40.5 %- 9.8 % of phosphorus. Wu et
23 al., 2015 added diatomite into pervious concrete as an adsorbent to improve its heavy metal ions
24 removal ability. Kim et al., 2017 carried out a comparative study of the reduction ratios of
25 nitrogen and phosphorus by pervious concretes fabricated with Portland cement and calcium
26 sulphoaluminate cement and indicated that the binder was a crucial factor in determining the water
27 purification characteristics of pervious concrete. Shabalala et al., 2017 investigated the potential
28 use of pervious concretes consisting of Portland cement CEM I 52.5R with or without 30 % fly
29 ash (FA) as a reactive barrier for the treatment of water polluted by mine waste and reached the
30 same conclusion that the absorptivity of the binder is directly related to the water purification
31 performance of the pervious concrete. Therefore, it can be seen that, compared with aggregates,
32 the adsorption of the binder has a more significant effect on the water purification performance of
33 the pervious concrete.
34 Although ordinary Portland cement is the most commonly used binder for pervious concrete
35 (Sheth et al., 2015), there have also been reports of the use of geopolymers for the preparation of
36 pervious concrete (Jo et al., 2015; Tho-in et al., 2012 and Fu et al., 2014) owning to their
37 environmental friendliness and excellent properties (such as high early strength(Davidovits, 1994),
38 excellent mechanical properties (Hardijito et al., 2014), low creep and shrinkage (Bakharev,
39 2005), and good resistance to acid (Hu et al., 2008) and sulfate attacks (Kong et al., 2008)). In
40 addition to the above advantages, a series of studies also indicated that geopolymer has excellent
41 adsorption properties. Al-Zboona et al., 2011 used a fly ash-based geopolymer as an adsorbent to
42 remove the Pb2+ from aqueous wastewater and found that the synthesized geopolymer exhibited
43 remarkable removal capacity for Pb2+. Cheng et al., 2012 investigated the adsorption features of a
44 metakaolin-based geopolymer for Pb2+, Cu2+, Cr3+ and Cd2+, and verified that the geopolymer
45 could adsorb heavy metals. Wang et al., 2007 indicated that the adsorptive capacity of a fly ash-
46 based geopolymer was much higher value than those of FA and natural zeolite. Therefore,
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1 pervious concrete prepared with geopolymer is expected to have excellent water purification
2 characteristics.
3 Based on the above, this work aims to use RM to replace some granulated blast furnace slag
4 (GBFS) to prepared RM-GBFS-based geopolymer, and use this geopolymer as the binder to
5 prepare a pervious concrete of good mechanical properties and of an adsorption of heavy metal
6 ions. In this work, some RM-GBFS-based geopolymers with different RM contents, Na2O/SiO2
7 mole ratios, and activator alkali concentrations are used to prepare a series of pervious concretes
8 (with constant the aggregate grading and the ratio of binder to aggregate). The strength, void
9 ratios, permeabilities, and heavy metal removal abilities of these samples are tested to analyze the
10 effects of the varied factors on the relative performances of RM-GBFS-based geopolymer
11 pervious concretes. XRD (X-ray diffraction) and SEM-EDS (scanning electron microscopy-
12 energy dispersive spectroscopy) are used to explore the water purification mechanism of RM-
13 GBFS-based geopolymer pervious concrete.
14
15 2. Materials and methods
16 2.1. Materials
17 The GBFS (used as the aluminosilicate material for the geopolymer) used in this experiment
18 was purchased from Wuhan Iron and Steel Company (Wuhan, China). The RM (derived from
19 alumina refineries through the Bayer process) was obtained from the red mud yard of Zhaofeng
20 Aluminum Company (Shanxi, China). Type I Portland cement (according to ASTM C150 (2016))
21 is used. The chemical compositions and physical properties of the above materials are shown in
22 Table 1. The alkali activator consists of sodium silicate and sodium hydroxide. The sodium
23 silicate (Na2SiO3•3.2H2O; pH=11.0-13.0; relative density: 2.614 g/cm3; purity: 34 %) was
24 purchased from Qingdao Best Line Chemical Technology Co., Ltd (Qingdao, China). The sodium
25 hydroxide (NaOH, pH>11; relative density, 2.130 g/cm3; purity, 96 %) is purchased from
26 Sinopharm Chemical Reagent Co., Ltd (Shanghai, China).
27 Table 1 Chemical compositions and physical properties of granulated blast furnace slag (GBFS), red mud (RM)
28 and Portland cement (PC)
Chemical composition (wt %) Physical properties
GBFS RM PC GBFS RM PC
CaO 37.51 16.49 55.56 Apparent density (kg/m3) 2.931 2.781 3.101
Al2O3 15.01 22.72 6.31 Specific surface area (m2/g) 4.245 10.854 3.264
SiO2 34.58 21.43 21.91 Initial setting time (min) 126
Fe2O3 0.27 9.98 2.95 Final setting time (min) 228
MgO 9.02 0 2.92
SO3 2.03 0 1.80
Na2O 11.51
0.68 0.85
K2O 0.42
LOI 1.10 13.41 6.34
29
30 2.2. Preparation of specimens
31 In order to remove the influence of different void ratios and permeabilities of the pervious
32 concrete on the adsorption of heavy metal ions, the mass ratio of water to GBFS was fixed at 0.37,
33 the amount of powder material was fixed at 320 kg/m3, and limestone gravel with a particle size of
34 4.75-9.5mm was used at a fixed dosage of 1600 kg/m3 to ensure that the target void can is
35 maintained at 25 v/v% (Currently, the designing void ratio of pervious concrete is general between
36 15 % and 33 % (Kia etc., 2017), and a bigger void ratio (or a larger permeability) is a designing
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1 trend of pervious concrete (Chandrappa etc., 2016), so the 25 v/v% of void ratio was chosen in
2 this work). The mix ratio of the binder is consistent with that in the corresponding permeable
3 concrete. A0 represents the GBFS-based geopolymer pervious concrete. A1 and A2 represent the
4 RM-GBFS-based geopolymer pervious concrete (the proportions of GBFS replaced by RM are 30
5 wt% and 50 wt%, respectively). A1-1 and A2-1 use raw RM, while A1-2 and A2-2 use washed
6 RM to investigate the effect of alkaline in the RM on the strengths of the pervious concrete and its
7 corresponding binders. RM is washed by immersing in distilled water for 24 hours and then
8 determining the pH of the leachate; if the pH is greater than 7, then leachate is filtered off and the
9 RM is immersed in fresh distill water for another 24 hours; this is repeated until the pH of the
10 leachate is around 7 for 3 consecutive days. The leachate is then poured off and the soaked RM is
11 dried at 100°C for 24 hours, then crushed before use. A1-1, A3, and A4 have alkali activator mole
12 ratios of 0.8, 0.4, and 1.2, respectively. A1-1, A5, and A6 contain alkali activator concentrations
13 of 6.0 wt%, 4.0 wt%, and 10.0 wt%, respectively. PC (Portland cement) indicates pervious
14 concrete and the corresponding binder is prepared using Portland cement. The specific
15 compositions of the prepared pervious concretes and their corresponding binders reported in
16 Table 2.
17 Table.2 Compositions of prepared pervious concretes and their corresponding binders
Binder
No. GBFS Alkali activator (kg/m3) Aggregate(kg/m3)
PC (kg/m3) RM (kg/m3)
(kg/m3) NaOH Water Na2SiO3
A0 0 0 320 19.55 80.51 57.41 1600
A1-1 0 96 224 19.55 80.51 57.41 1600
A1-2 0 96 (washed) 224 19.55 80.51 57.41 1600
A2-1 0 160 160 19.55 80.51 57.41 1600
A2-2 0 160 (washed) 160 19.55 80.51 57.41 1600
A3 0 96 224 22.68 99.46 28.70 1600
A4 0 96 224 16.42 61.57 86.11 1600
A5 0 96 224 13.03 93.14 38.27 1600
A6 0 96 224 26.06 67.88 76.54 1600
PC 320 0 0 0 118.40 0 1600
18
19 Using the ratios shown in Table 2, the sodium hydroxide (NaOH), sodium silicate (Na2SiO3),
20 and water (the PC group only uses water) are first mixed together to form a solution, while the
21 GBFS, RM (the PC group uses cement) and aggregate are dry-mixed for 1 min. After that, the
22 above-prepared solution is poured into the dry mixture, and stirred for 2 min until a uniform
23 mixture is obtained. The mixture is then put into a 150×150×150 mm cube trial mold and
24 immediately covered with plastic film. After curing for 1 day in the mold, the samples are
25 removed from the mold and place in a standard curing room at a temperature of 20±1 °C and a
26 humidity of 95 %. There are twelve samples for each group. Three samples are used for 7d
27 compressive strength testing and three samples for 28d. Three samples are used for void and
28 permeability testing and the remaining three samples are subjected to dynamic adsorption testing
29 (described in section 2.4.1) after curing for 28 days. Before the dynamic adsorption testing, these
30 three samples were washed by distill water until the pH of washed water is around 7, and then
31 dried these sample for adsorption testing. After the dynamic adsorption testing, a portion of
32 aggregate coated with binder is removed from the middle of the sample, vacuum dried, and
33 analyzed by SEM and EDS. The preparation of the corresponding binder is similar to for the
34 pervious concrete and the cube mold size is 50×50×50 mm. There are seven samples for each

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1 group: six are used for compressive strength testing (7d and 28d), while one sample is ground
2 finely to a particle size below 100 μm (according to Kim et al., 2017) for static adsorption
3 testing (described in section 2.4.2) and XRD analysis.
4 2.3. Experimental procedure
5 The compressive strength of the pervious concrete is tested according to BS EN 206-1:2000
6 and the compressive strength of binder is tested according to ASTM C109/C109M–11b. Three
7 samples are tested for each group and the means and standard deviations are calculated.
8 The void ratio is determined according to ASTM C1754 (2012). First, sizes of sample are
9 measured and the volume (v) are calculated; second, the samples are immersed into water
10 completely for 12 hours; then, their weights (m0) in water are measured; finally, these samples are
11 taken from the water and their weights (m1) are measured after drying. The void ratio is calculated
12 according to Eq. (1). Three samples are tested for each group and the means and standard
13 deviations are calculated.
𝑚1 ‒ 𝑚0
14 [
𝑘= 1‒ 𝑣 ] × 100 % (1)

15 The permeability coefficient is tested according to the method in ACI 552R-08 (the test
16 device is shown in Fig.1) and is calculated according to Eq. (2). Three samples are tested for each
17 group and the means and standard deviations are calculated.
𝛼1 × 𝐿 ℎ1
18 𝑘=𝛼 × 𝑙𝑛 (ℎ ) (2)
2×𝑡 2

19 where k is permeability (mm/s); L is the length of sample (mm); α1 is the cross-sectional area
20 of the tube (mm2); α2 is the cross-section area of the sample (mm2); t is the time for water to drop
21 from h1 to h2(s), h1= 260 mm and h2= 60 mm.

22

23 Fig.1. Permeability test setup (Khankhaje et al., 2017a).

24 The phase composition of the binder was analyzed using XRD (RU-200B, RIGAKU Corp.,
25 Japan). Microscopic observation was carried out using a field diffractometer emission scanning
26 electron microscope (FEI-QUANTA FEG 450, FEI Hong Kong Co., Ltd., China) and an X-ray
27 spectrometer is used for surface scanning to observe the distribution of heavy metal ions on the
28 surface of the binder.
29 2.4 Adsorption procedures
30 The adsorption in this work can be divided into two parts: dynamic adsorption (for RM-
31 GBFS-based geopolymer pervious concrete) and static adsorption (for binder powders).
32 2.4.1 Dynamic adsorption of RM-GBFS-based geopolymer pervious concrete

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1 In order to simulate the process of rainwater entering a groundwater system through pervious
2 concrete, a device for testing the heavy metal ion adsorption of pervious concrete dynamically was
3 designed, as shown in Fig.2. Each pass of the heavy metal ions solution (Volume is 1L) through
4 the pervious concrete is considered to be one adsorption cycle; after 50 adsorption cycles, 10 ml of
5 the heavy metal ion solution is removed for determination of the heavy metal ion content by
6 inductively coupled plasma (ICP) (preliminary studies showed that the concentration of heavy
7 metal ions in the solution remained stable after 50 adsorptions).
8 The heavy metal ions solution (simulated rainwater) is prepared using CdCl2, PbCl2, CuCl2,
9 and CrCl3•6H2O (chemical purity, purchased from Qingdao Best Line Chemical Technology Co.,
10 Ltd, Qingdao, China) and distilled water, and the total concentrations of heavy metal ions in
11 solution is fixed at 1×10-3 mol/L-1 (according to Holmes et al., 2017) and the concentration of
12 each heavy metal ions (Cd2+, Pb2+, Cu2+, and Cr3+) is 0.25 mol/L-1. In addition, the pH value of
13 solution has a significant effect on the adsorption of heavy metal ions by the adsorbent (Fu et al.,
14 2011; Abollino et al., 2003), therefore, the pH of heavy metal ions solution is fixed around 7 by
15 using dilute nitric acid in order to eliminate this effect.

16
(a) Schematic diagram (b) Photograph
Fig.2. Pervious concrete dynamic adsorption test device
17 2.4.2 Static adsorption of binder powders
18 In order to explore the relationship between the adsorption of binder and that of pervious
19 concrete, the adsorption of binder powders (2 g each of raw GBFS (GBFS), raw RM (RM), RM-
20 GBFS-based geopolymer binder (A0-A6) and PC binder (PC)) to Pb2+ (as an example) is also
21 investigated. Binder powders are placed separately into 250 ml of PbCl2 solution at a
22 concentration of 50 ppm, adjusted the pH of solution to around 7 by using dilute nitric acid, and
23 then stirred manually for 5min. After holding for 5, 10, 15, and 30 min, 3 ml of each liquid are
24 removed for determination of the Pb2+concentrations by ICP.
25
26 3. Results and discussion
27 3.1. Mechanical properties
28 The 7d and 28d compressive strengths of the pervious concretes and the binders are shown in
29 Fig.3 and Fig.4, respectively. As the RM content increases from 0 to 50 wt%, the compressive
30 strength of the pervious concretes decreases by 42.1 % (7d) and 36.7 % (28d). Simultaneously, the
31 compressive strength of binders also decreases by 36.8 % (7d) and 36.4 % (28d). The iron species
32 in RM hinders dissolution of aluminosilicate material in the geopolymer, which results in the
33 decreased compressive strength (Kaya et al., 2016). From the differences between the

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1 compressive strength of A1-1 or A2-2 (prepared using untreated RM) and A1-2 or A2-2 (prepared
2 using washed RM), the alkali in RM could be an activator of the aluminosilicate material in the
3 geopolymer (Pan et al., 2003). The Na2O/SiO2 mole ratio plays an important role in the
4 compressive strength of the pervious concretes and the binders (Khale et al., 2007). As the mole
5 ratio of Na2O/SiO2 increases from 0.4 (A3) to 1.2 (A4), the 28d compressive strength of the
6 pervious concrete first increases from 10.55 MPa to 18.53 MPa, and then decreases to 10.72 MPa
7 when the Na2O/SiO2 mole ratio is above 0.8. The mole ratio of Na2O/SiO2 has the same effect on
8 the binder strength. The compressive strength of the pervious concretes and binders varies with
9 alkali concentration. The highest compressive strength of pervious concrete was obtained at an
10 alkali concentration of 6 wt% ( A1-1), and then the strength decreased with further increasing in
11 the alkali concentration (A6) (Khale et al., 2007).
12 It is noted that the 28d compressive strength of RM-GBFS-based geopolymer pervious
13 concrete (the replacement rate of RM to GBFS is up to 30 wt%) is 18.53 MPa, which can be used
14 as the light road pavement in China. This is because that the pervious concrete with 28d
15 compressive strength higher than 15.0 MPa can be used for light road according to GB/T 25993-
16 2010 (2010). Compared with the PC sample (made by Portland cement), sample A1-1 (made by
17 RM-GBFS) has sufficient strength for light road pavement. Therefore, the content of RM can be
18 as high as 30 wt% in RM-GBFS-based geopolymer pervious concrete. That is, every cubic of
19 pervious concrete will consume 96 kg of RM and save the same amount of GBFS, which has
20 become a valuable mineral admixture in China, simultaneously. Moreover, due to the alkali
21 contained in RM, it is also possible to save the amount of alkali used in the alkali activated
22 materials.
25
7d 60 7d
28d 28d
Compressive strength(MPa)

20
50
Compressive strength(MPa)

40
15

30
10

20

5
10

0 0
A0 A1-1 A1-2 A2-1 A2-2 A3 A4 A5 A6 PC A0 A1-1 A1-2 A2-1 A2-2 A3 A4 A5 A6 PC
23
Fig.3. Compressive strength of pervious concretes: 7d Fig.4. Compressive strength of binder: 7d and 28d
and 28d
24
25 Fig.5 and Fig.6 show the relationship between the compressive strength of the pervious
26 concrete and the binder after curing for 7 and 28 days, which indicates a satisfactory trend that the
27 strength of the pervious concrete increases with increasing strength of the binder. Although the
28 aggregate size, water/cement ratio, paste/aggregate ratio, void ratio, etc. can affect the strength of
29 pervious concrete, the strength of the binder is a main and directly factor (Joshaghani et al.,
30 2015). Therefore, a significant linear positive correlation can be seen between the strength of the
31 pervious concrete and that of the binder, whether the binder is PC (Ibrahim et al., 2015) or the
32 RM-GBFS-based geopolymer, as shown in Fig.3 and Fig.4.

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20
22
Actual value Actual value
18 Fitting Curve
Pervious concrete strength(MPa) Fitting Curve

Pervious concrete strength(MPa)

20
16
18
14
16

12
14

10
12
y=0.484x-4.891
8 y=0.519x-6.639
R2=0.825 10
R2=0.91316
6 8

20 25 30 35 40 45 25 30 35 40 45 50 55
Binder strength(MPa) Binder strength(MPa)
1
Fig.5. Fitting curve for 7d compressive strength of Fig.6. Fitting curve for 28d of compressive strength of
binder and concrete binder and concrete
2 3.2. Void ratio and permeability
3 Fig.7 shows the measured total void ratios of the pervious concrete samples; the target void
4 ratios are 25 v/v%. The measured total void ratio for every sample is higher than the target void
5 ratio, which is due to the rough surface of the aggregate and the process of compaction (Kim et al.,
6 2017; Singh et al., 2014). The measured total void ratios of all samples are similar and range from
7 26 % to 29 %. Moreover, the permeabilities of all samples are also similar and range from 8.03
8 mm/s to 8.91 mm/s, as shown in Fig.8. This is because the permeability of pervious concrete is
9 well correlated with its void ratio (Neithalath et al., 2010; Chandrappa et al., 2016). Some studies
10 have shown that the contact time and area can have significant effect on the adsorption efficiency
11 of an adsorbent (Shabalala et al., 2017; Al-Zboona et al., 2011; Shin et al., 2016), in this work,
12 the contact time and area between the water and the pervious concrete are affected by the total
13 void ratio and the permeability. Therefore, the aggregate gradation and the paste/aggregate ratio,
14 which are two main factors affecting the total void ratio and permeability of a pervious concrete
15 (Pieralisi et al., 2016), are maintained to eliminate the effect of total void ratio on the concrete’s
16 strength and the adsorption of heavy metals.
35 12
Target void=25%
30
29 29 8.91
28 28 10
27 27 8.77
26 26 8.54
8.32 8.45 8.12
8.03 8.25
25
Permeability(mm/s)

8
Total void(%)

20

6
15

4
10

5 2

0
A0 A1-1 A2-1 A3 A4 A5 A6 PC 0
A0 A1-1 A2-1 A3 A4 A5 A6 PC
17
Fig.7. Total void ratio of concrete Fig.8. Permeability of concrete
18
19 3.3. Water purification characteristics
20 In order to determine the adsorption efficiency of the prepared pervious concrete samples for
21 each of the tested heavy metal ions, the reduction ratio of each heavy metal ion’s concentration
22 after 50 absorption cycles was calculated according to Eq. (2), and the results present on Fig.9.
𝛼0 ‒ 𝛼50
23 𝑅𝑒𝑑𝑢𝑐𝑡𝑖𝑜𝑛 𝑟𝑎𝑡𝑖𝑜 (%) = 𝛼0 × 100 % (2)

8
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1 where α0 represents the concentration of each heavy metal ion before the first absorption
2 cycle, and α50 indicates the concentration of each heavy metal ion after 50 absorption cycle.
100 55
Cd Pb Cu Cr
90 50

80

Concentation of Pb2+(ppm)
45
Reduction ratio(%)

70
40
60 RM
GBFS
35 A0
50 A1-1
A2-1
30 A3
40 A4
A5
25 A6
30 PC

20
20 0 10 20 30 40 50 60
A0 A1-1 A2-1 A3 A4 A5 A6 PC Time(min)
3
Fig.9. Reduction ratios of heavy metal ions Fig.10. Batch adsorption test results for binders
concentrations by pervious concrete samples
4
5 As shown in Fig.9, it can be found that all of the RM-GBFS-based geopolymers prepared in
6 this work (A1-A6) absorb heavy metal ions more strongly than the Portland cement based-
7 pervious concrete (PC). Take A2-1 and PC for example, the reduction ratios of heavy metal ions
8 concentrations after purified by A2-1 are 64.16 % (Cd2+), 84.03 % (Pb2+), 63.30 % (Cu2+), and
9 62.60 % (Cr3+); whereas, what after purified by PC are only 45.41 % (Cd2+), 66.12 % (Pb2+),
10 38.23 % (Cu2+), and 23.42 % (Cr3+).
11 Moreover, the composition (such as the content of RM, the Na2O/SiO2 mole ratio and the
12 alkali concentration of the activator) of the RM-GBFS-based geopolymer has an effect on its
13 adsorption capacity for heavy metal ions. The reduction ratio of each of the heavy metal ions
14 increases with the increasing RM content, as shown in Fig.9. As the content of RM increases from
15 0 to 50 wt%, the reduction ratios of the concentration of Pb2+, Cd2+, Cu2+, and Cr2+ increase from
16 73.35 %, 58.96 %, 53.68 %, and 47.99 % (A0) to 84.03 %, 64.16 %, 63.30 %, and 62.6 % (A2-1),
17 respectively, indicating that RM provides strong heavy metal ion adsorption in the RM-GBFS-
18 based geopolymer. This is because the RM is composed of fine particles with a high surface
19 reactivity (Gupta et al., 2011; Bertocchi et al., 2006; Rai et al., 2012), so it adsorbs heavy metal
20 ions stronger than PC or geopolymer without RM. Therefore, the RM can improve the adsorption
21 capacity of pervious concrete on heavy metal ions obviously to make the pervious concrete with
22 the function of excellent water purification.
23 The Na2O/SiO2 mole ratio and the alkali concentration of the activator for the geopolymer
24 can affect the adsorption capacity of pervious concrete to heavy metal ions to a certain extent, but
25 the impact is limited. With the Na2O/SiO2 mole ratio increasing from 0.4 (A3) to 1.2 (A4) via 0.8
26 (A1-1), the reduction ratio of Pb2+ first increases from 74.15 % (A3) to 77.38 %( A1-1) and then
27 decreases to 71.97 % (A4), which is similar to the relationship between the alkali concentration of
28 the activator and the adsorption capacity for heavy metal ions. The heavy metal ion adsorption
29 ability of the geopolymer is affected by the content of the amorphous gel (geopolymeric gel and
30 C-S-H gel with lower Ca/Si ratio), which has a high surface area and a large pore volume (Al-
31 Zboona et al., 2011; Wang et al., 2007). The formation of this gel involves the dissolution of
32 aluminosilicate materials and the condensation of an aluminosilicate gel (Buchwald et al., 2011).
33 As the alkali concentration of the activator increases, the speed of aluminosilicate dissolution
34 increases. With increasing the Na2O/SiO2 mole ratio increasing, the speed of condensation and the

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1 quantity of geopolymer gel first increases and then decreases (Khale et al., 2007; Zhang et al.,
2 2008). Therefore, the content of this gel in the geopolymer varies with the change in the mole ratio
3 of Na2O/SiO2 and the alkali concentration of the activator, which also affect the adsorption of
4 heavy metal ions by the RM-GBFS-based geopolymer pervious concrete.
5 Therefore, compared with the Na2O/SiO2 mole ratio or the alkali concentration of the
6 activator, the content of RM is the most significant factor on the water purification of the RM-
7 GBFS based geopolymer pervious concrete and can adjust it to regulate the water purification
8 capacity of the pervious concrete.
9 Fig.10 shows the static adsorption test results for the different binders (including raw RM and
10 GBFS) on dissolved PbCl2. It can be seen that the Pb2+ concentrations in the solutions are
11 remarkably reduced in the first 10 min and reach equilibrium after 30 min, which is consistent
12 with the results reported in Kim et al., 2017. The adsorption of Pb2+ by GBFS is the lowest while
13 that by RM is the highest. Furthermore, the adsorption capacity of the binders is in the same order
14 as that of the corresponding pervious concretes, which indicates that the adsorption ability of the
15 pervious concretes is mainly affected by that of the binder when the aggregate grade and the
16 paste/aggregate ratio are fixed.
17 It is worth noting that the contact time between the pervious concrete and the heavy metal
18 ions is also a main factor affecting adsorption of RM-GBFS-based geopolymer pervious concrete,
19 and this contact time can be indicated by the permeability coefficient of pervious concrete. In this
20 work, there are some minor differences on the permeability of samples, which is possible to be a
21 secondary reason for differences in adsorption of samples. For example, as shown in Fig.9, the
22 highest reduction ratios of heavy metals were observed for A2-1, which exhibits quite low
23 permeability (about 8.32 mm/s), and quite low reduction ratios were obtained for A5 with highest
24 permeability (about 8.91 mm/s). However, the above rule does not apply to all samples in this
25 work (such as A0 and A2-1) since the difference in the void ratio (or permeability) between
26 samples is much smaller than the difference in characteristic of binder between samples.
27 Therefore, the characteristic of binder is the most mainly factor for adsorption in this work.
28 In addition, Fig.9 also shows that the RM-GBFS-based pervious concrete has different
29 adsorption effects on different heavy metal ions. The strongest adsorption effect was found for
30 Pb2+ (with reduction ratios of 66.14 %-84.30 %) while the weakest adsorption effect was for Cr3+
31 (with the reduction ratios of 24.36 %-62.62 %). The adsorption capacity of the RM-GBFS-based
32 pervious concrete for different heavy metal ions is in the order: Pb2+ > Cd2+ > Cu2+ > Cr3+, which is
33 similar to the results obtained for the geopolymer in Cheng et al., 2012. The radius of the hydrated
34 metal ions, the activity of the metal ions, and the free energy of hydration of the metal ions affect
35 the adsorption selectivity (Cheng et al., 2012). The smaller the hydrated metal ion radius, the
36 lower the free hydration energy, and the easier the metal ions are adsorbed, and vice versa. The
37 radii of the hydrated metal ions and the free hydration energies of Pb2+, Cd2+, Cu2+ and Cr2+ are
38 4.01 Å, -357.2 kcal/mol, 4.26 Å, -429.8 kcal/mol, 4.19 Å, -496.9 kcal/mol, and 4.61 Å, -1005.5
39 kcal/mol, respectively (Barros et al., 1997; Hawari et al., 2007; Sanderson, 1967; Schneider et
40 al., 2007). Compared with the other metal ions, Pb2+ has the smallest hydrated metal ion radius
41 and the lowest free hydration energy; therefore, the reduction ratio of the Pb2+ concentration after
42 50 absorption cycles is the highest.
43 3.4. Mechanism analysis
44 3.4.1. Mineral compositions of binders
45 Fig.11 shows the XRD patterns for RM, GBFS and binders of A0, A1-1, and A2-1 after
46 curing for 28 days. There is a broad diffuse hump peak located at 20-38° (2θ) in the XRD pattern
10
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1 for GBFS indicating that the GBFS mainly consists of typical amorphous phases (Zhang et al.,
2 2008). After the GBFS activated by alkali for 28 days, the broad diffuse hump peak in the XRD
3 pattern of A0 (GBFS -based geopolymer binder) becomes narrower and more significant and
4 centered around 30° (2θ), which indicates the A0 sample is “completely amorphous with a clearly
5 lack of long-range order” (Lecomte et al., 2006). Some studies suggest that the amorphous phase
6 includes geopolymeric gel and C-S-H gel with a lower Ca/Si ratio (Zhang et al., 2008; Lecomte et
7 al., 2006; Yip et al., 2005). The RM contains hematite, gibbsite, cancrinite, muscovite-2 and
8 katoite (as shown in Fig.11), which is consistent with Pan et al., 2003; Ye et al., 2016; Kaya et al.,
9 2016. From the XRD patterns of A1-1 and A2-1, it can be seen that the characteristic peaks of RM
10 also appear in the RM-GBFS-based geopolymer and these peaks becomes more visible as the
11 content of RM increases from 30 % (A1-1) to 50 % (A2-2). This indicates that some of the RM
12 does not participate in the action and other studies (Pan et al., 2003; Hajjaji et al., 2013; Kaya et
13 al., 2016) also reached the same conclusion. There is also a broad diffuse hump peak centered at
14 around 30° (2θ) in the XRD patterns of A1-1 or A2-1 that indicates that an amorphous phase
15 including geopolymeric gel and C-S-H gel is also formed in the RM-GBFS-based geopolymer.
16 Therefore, RM-GBFS-based geopolymer consists of the geopolymeric gel, C-S-H gel, and some
17 raw RM.
18
C=Cancrinite(Na,Ca,K)7-8[(Si,Al)12O24](CO3,OH)22-3H2O G=Gibbsite(Al(OH)3) F=Hematite(Fe2O3)
M=Muscovite-2((K,Na)Al2(Si,Al)4O10(OH)2 K=Katotite(Ca2.93Al1.97Si0.64O2.56(OH)9.44)
RM

C F F
C M
G C K
M F K K
M K C M K
GBFS
A2-1
A1-1
A0

10 15 20 25 30 35 40 45 50 55 60 65 70
2degree
19
20 Fig.11. XRD patterns of RM, GBFS, and binders from A0, A1-1, A2-1, 28d of curing

21 3.4.2. Microscopic morphology of binders

22 The hydration products of PC are mainly Ca(OH)2, C-S-H gel and AFt (Feldman et al., 1976)
23 (Fig.12 (a),(b)) , while the GBFS-based geopolymer (A0) includes geopolymeric gel and C-S-H
24 gel (Yip et al., 2005) (Fig.12 (c),(d)), which has a much lower Ca/Si ratio compared to that of C-
25 S-H gel resulting from the hydration of Portland cement (Brough et al., 2002). Fig.12 (g), (h)
26 shows that there are also some unreacted RM particles in the RM-GBFS-based geopolymer, which
27 is in agreement with the Pan et al., 2003. Comparing Fig.12 (a) with (c), it is clear that the
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1 structure of GBFS-based geopolymer is more compact than that of cement paste, which results in
2 the strength of A0 being higher than that of PC, as shown in Fig.3 and Fig.4. The structure of the
3 RM-GBFS-based geopolymer (Fig.12 (e)) is as compact as that of the GBFS-based geopolymer
4 (Fig.12 (c)), but it contains some unreacted RM leading to defects in structure (Hajjaji et al.,
5 2013). Thus, the strengths of both the pervious concrete and the binder (A0, A1, and A2) decrease
6 with increasing RM content (Fig.3 and Fig.4). The characteristics and quantity of gel (including
7 C-S-H gel and geopolymeric gel) directly affect the binder's adsorption of heavy metal ions. The
8 geopolymeric gel in the GBFS-based geopolymer (A0) or the RM-GBFS -based geopolymer (A2)
9 has a higher surface area and a bigger pore volume (Al-Zboona et al., 2011; Wang et al., 2007)
10 (Fig.12. (d), (f)) compared with the C-S-H gel in the PC paste (Fig.12. (b)), and the C-S-H gel
11 with a lower Ca/Si ratio in the geopolymer has the same feature (Nonat, 2004; Pelisser, 2012). In
12 addition, the amount of these gels is also greater than that in PC matrix, so the heavy metal ion
13 absorption capability of the GBFS-based (A0) and RM-GBFS-based geopolymer pervious
14 concretes (A1) is stronger than that of the PC pervious concrete, as shown in Fig.9. RM has a
15 small particle radius, large porosity, and large specific surface area, which is why it can strongly
16 absorb pollutants in aqueous solution (Khan et al., 2015; López-García et al., 2017; Lata et al.,
17 2015). Therefore, with the content of RM increasing from 0 % (A0) to 50 % (A2), the adsorption
18 effect of heavy metal ions by the pervious concrete/binder gradually becomes stronger, as
19 illustrated in Fig.9 and Fig.10.

Ca(OH)2

AFt

C-S-H
100μm 10μm

20
21 (a)Portland cement (PC), 500× (b) Portland cement (PC), 5000×

C-S-H (lower Ca/Si)

Geopolymeric gel

100μm 10 μm

22
23 (c) GBFS-based geopolymer (A0), 500× (d) GBFS-based geopolymer (A0), 5000×

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Red mud
Geopolymeric gel

C-S-H (lower Ca/Si)

100μm 10μm

1
2 (e) RM-GBFS-based geopolymer (A2-1), 500× (f) RM-GBFS-based geopolymer (A2-1), 5000×

3 Fig.12. SEM micrograph of binder of Sample PC, A0, A2-1, 28d

4 3.4.3. Adsorption of heavy metals on the surface of the binders

5 Fig.13 (a), (b), and (c) show the distributions of heavy metal ions on the PC, GBFS-based
6 geopolymer (A0) and RM-GBFS-based geopolymer (A2-1) binder pieces coating aggregate,
7 respectively. In the spectral scanning area, the red pixels represent heavy metals (including of Pb,
8 Cd, Cu and Cr) adsorption, while the gray pixels represent no heavy metal adsorption. Therefore,
9 the ratio of the red to total areas can indicate the amount of heavy metal adsorption. The ratios of
10 red to total areas in Fig.13 (a), (b), (c) are 17 %, 37 % and 53 %, respectively, which means that
11 the order of adsorption capacity for heavy metal ions is: Portland cement pervious concrete (PC) <
12 GBFS-based geopolymer pervious concrete (A0) < RM-GBFS-based geopolymer pervious
13 concrete (A2-1), which is consistent with the results of the % reduction in the concentration of
14 heavy metal ions in Fig.9 and the batch adsorption test results for the binders in Fig.10. It was also
15 determined that the heavy metal ions are mainly adsorbed on the C-S-H gel in the PC binder
16 (Chen et al., 2009) (Fig.13(a)), mainly adsorbed on the geopolymeric gel/C-S-H gel in the GBFS-
17 based geopolymer binder (Al-Zboona et al., 2011; Cheng et al., 2012) (Fig.13(b)), and mainly
18 adsorbed on the geopolymeric gel/C-S-H gel/rud mud in RM-GBFS-based geopolymer
19 binder(Fig.13(c)). The color of the red area in Fig.13 (b) is deeper than that in Fig.13 (a), which
20 indicates that the gel (geopolymeric and C-S-H gel with low Ca/Si ratio) in the GBFS-based
21 geopolymer has a stronger adsorption capacity for heavy metal ions than the gel in the Portland
22 cement binder.
23 The distributions of different heavy metal ions adsorbed by the RM-GBFS-based geopolymer
24 binder segment are shown in Fig.13 (e), (f). The purple, green, red and yellow pixels represent Pb,
25 Cd, Cu and Cr, respectively, and the ratios of the different color pixels indicate the adsorption of
26 different heavy metal ions by the RM-GBFS-based geopolymer pervious concrete. Fig.13 (f)
27 shows that adsorption capacity of the RM-GBFS-based pervious concrete for different heavy
28 metal ions is in the order: Pb2+ > Cd2+ > Cu2+ > Cr3+, which is consistent with the results for the %
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1 reduction in the concentration of heavy metal ions in Fig.9.

Pb/Cd/Cu/Cr
Unallocated 17%

83%

2
3 (a) Portland cement binder (PC), after adsorption

Pb/Cd/Cu/Cr
Unallocated

37%

63%

4
5 (b) GBFS-based geopolymer binder (A0), after adsorption

Pb/Cd/Cu/Cr
Unallocated

47%
53%

6
7 (c) RM-GBFS-based geopolymer binder (A2-1), after adsorption

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48% Pb
P Cd P
24%
PP P P
18% Cu
bP P b
9% P
2b Zn P
b2
P
+2PPPbP
2+
PbP2+Pb
+ +P
B2bB2+2B
P P
2+2 +
B B 2
P
+2+ 2+P
1
BP B
2 (d) RM-GBFS-based geopolymer binder, before adsorption (e) Various metals on RM-GBFS-based geopolymer
+ +
3 binder, after adsorption 2B 2
4 Fig.13. Binder piece coated aggregate with EDS showing metal deposition +2 +
5 The adsorption mechanism of RM-GBFS based geopolymer pervious concrete has +been
6 revealed based on the analysis of the XRD, SEM and EDS; this can be used to guide the design of
7 such pervious concrete and to regulate its function of water purification.
8
9 4. Conclusions
10 In this study, RM-GBFS-based geopolymer pervious concretes with different mixtures were
11 prepared and their strength, void ratio, permeability, and heavy metal adsorption were measured.
12 The mechanisms on the strength formation and adsorption of heavy metal ions of these concretes
13 were revealed based on the analysis of the XRD, SEM with EDS results. It can be concluded as
14 follows:
15 (1) RM content played an important role in the strength and adsorption of heavy metal ions
16 in the RM-GBFS-based geopolymer pervious concrete. The strength decreased and the
17 adsorption of heavy metal ions improved remarkably as the content of RM increased
18 from 0 to 50 wt%.
19 (2) As the Na2O/SiO2 mole ratio and the alkali concentration of the activator increased, the
20 strength of samples firstly increased and then decreased. In addition, the Na2O/SiO2 mole
21 ratio and the alkali concentration of the activator also affected the heavy metal ion
22 adsorption capacity of the pervious concrete to a certain extent, but its effect was little.
23 (3) The hardened RM-GBFS-based geopolymer concrete consisted of geopolymeric gel, C-
24 S-H gel with a low Ca/Si ratio and some raw red mud particles. The main reason for the
25 significant adsorption of heavy metal ions of RM-GBFS-based geopolymer pervious
26 concrete may be that the geopolymeric gel and the C-S-H gel with a low Ca/Si ratio have
27 large surface area and high pore volume, and the unreacted raw RM in the RM-GBFS-
28 based geopolymer concrete has a great ability of absorbing heavy metal ions.
29 (4) Compared to PC pervious concrete, the 28d compressive strength of the RM-GBFS-
30 based geopolymer pervious concrete (RM content =30 wt%) was only lower by 5 %,
31 while the removal of heavy metal ions increased by 33 %-120 %, so this pervious
32 concrete can be applied in light road pavement in China.
33 (5) Although this work has demonstrated the feasibility of utilizing RM in geopolymer based
34 pervious concrete with function of adsorbing heavy metal ions and provides a technical
35 approach for boosting the utilization of RM, there are also some limitations (for example,
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1 fail to consider the effect of the initial concentration of heavy metals ions, pH of
2 solution, etc.) needing further improving in future studies. Moreover, the void ratio and
3 permeability of pervious concrete can also affect the water purification of RM-GBFS
4 based geopolymer pervious concrete, which is an important direction for future research
5 on this topic. Meanwhile, it is also necessary to study that the adsorption capacity of this
6 concrete for other pollutants (such as TN, TP) in rainwater.
7
8 Acknowledgements
9 The authors would like to thank the financial support by the Fundamental Research Funds for
10 the Central Universities (Project No. 20181049701003 and 2018-CL-A1-33), the Science and
11 technology basic work of China (Project No. 2014FY110900) and the National Natural Science
12 Foundation of China (Project No. 51402226).

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List of abbreviations
Abbreviation Complete form
RM red mud
GBFS granulated blast furnace slag
XRD X-ray diffraction
SEM scanning electron microscope
EDS energy spectrometer
red mud-granulated blast furnace slag- based
RM-GBFS-based geopolymer pervious concrete
geopolymer pervious concrete
COD chemical oxygen demand
TSS total suspended solids
TN total nitrogen
TP total phosphorus
Portland cement/ pervious concrete prepared with
PC
Portland cement
ICP inductively coupled plasma

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