Construction
Construction
Manuscript Draft
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1 Cementitious binders and reclaimed asphalt aggregates for
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2 sustainable pavement base layers: potential, challenges
4 3 and research needs
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6
a,b a a a
7 4 Juliana O. Costa , Paulo H. R. Borges , Flávio A. dos Santos , Augusto Cesar S. Bezerra , Wim Van
b b
8 5 den bergh and Johan Blom
9
10 6 a
Department of Civil Engineering, Federal Center for Technological Education of Minas Gerais (CEFET-MG),
11 7 Belo Horizonte, Brazil
12 8 b
Faculty of Applied Engineering, EMIB research group, University of Antwerp, Antwerp, Belgium
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14 9 Abstract:
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16 10 Five to seven percent of CO2 is emitted during the production of Portland cement, making it an
17 11 unsustainable binder for modern pavement base layers. If the road industry supports the global
18 12 challenge to decrease global warming, new binders should be developed and materials used with a
19 13 lower impact, leading to a more sustainable pavement structure. This review paper investigates the
20 14 possibility of incorporating recycled aggregate pavement (RAP) as an aggregate replacement, and
21 15 alternative cementitious materials as Portland cement (PC) replacement in base and subbase layers
22 16 of pavements. Special attention is given to the use of alkali-activated materials (AAM) as binder for
23 17 RAP granules. It discusses RAP as a construction material, the implications of using RAP in
24 18 pavement layers with PC and supplementary cementitious materials. It also highlights the
25 19 advantages, limitation challenges and research needs for RAP-incorporated AAM (RAP-AAM). This
26 20 study concludes that the use of RAP and AAM has a sustainable potential but also call to more
27 21 research to understand the impact of different activation systems on mechanical and durability
28 22 properties, as well as the possibility to include local wastes as a precursor. Moreover, mechanical
29 23 solutions should be supported by an LCA study to compare alkali-activated alternatives with current
30 24 solutions.
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33 25 Keywords:
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35 26 RAP; alkali-activation; pavements; base-layers; recycled aggregates
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37 27 1. Introduction
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39 28 The road infrastructure comprises 21 million kilometers worldwide [1], and the related industrial
40 29 sectors are said to be responsible for 24% of the global Greenhouse Gas (GHG) emissions worldwide
41 30 [2,3]. Natural aggregates are a non-renewable source and a major component of pavements, any
42 31 small recyclability actions may significantly reduce the environmental impact of the infrastructure
43 32 sector. Currently, pavement sustainability actions comprise the employment of several types of
44 33 recycled aggregates. The most used recycled aggregates are recycled concrete [4], steel slag [5],
45 34 waste foundry sand [6], waste glass [7], crushed brick [8] and reclaimed asphalt pavement (RAP) [9].
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35 RAP is a waste produced during the asphalt road rehabilitation, Europe and USA combined produced
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48 36 well over 100 million tons of RAP in 2017 [10]. In Europe, 68% of the reclaimed asphalt is reused in
49 37 asphalt mixes, 19% is used as granular materials in unbound layers, 1.25% finds application in other
50 38 civil engineering projects and 11% ends on landfills [10]. Most studies recommend the use between
51 39 20-50% of RAP as an aggregate replacement; in the U.S., many of the State Department of
52 40 Transportation (DOT) agencies limit the RAP content to 15% to avoid variabilities in the hot mix
53 41 asphalt [11]. Zhang et al. [12] presented a detailed review of the production process and performance
54 42 of RAP-containing asphalt hot mixes. In Belgium, RAP also finds applications in cement-stabilized
55 43 and loose bases / sub-bases [13].
56 44 Worldwide a relatively high amount of RAP is yet not recycled and therefore disposed of in stockpiles.
57 45 Other recycling actions are in place, such as the utilization of RAP as a replacement for natural
58 46 aggregates in Portland cement-based materials (mainly concrete). However, the mechanical and
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47 durability properties of RAP containing OPC are jeopardized by the poor adhesion of RAP to the
1 48 cement paste [14].
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3 49 Alkali-activated materials (AAM) emerged in the last two decades as sustainable building materials to
4 50 replace Portland cement for some applications. These new binders rely on the alkaline activation of
5 51 natural materials (mainly clay and metakaolin) and industrial residues or wastes (such as pulverized
6 52 fly ash, ground granulated blast furnace slag, mining residues, among others). AAM has been studied
7 53 as stabilizers in base-subbase layers and more recently employed in combination with RAP
8 54 aggregates [15,16]. Although the results appear to be promising, the literature on this subject is still
9 55 scarce. To the author's knowledge, there is no publication addressing the advantages and
10 56 shortcomings of alkali-activated materials containing RAP aggregates (RAP-AAM).
11 57 Most of the researches on sustainable materials for pavement sections focus on the asphalt layers
12 58 and undermine the potential of the foundation layers (base and subbase). The foundation layers are
13 59 thicker than asphalt layers and therefore, can consume higher volumes of recycled materials.
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60 However, the use of larger quantities of recycled aggregates represents, in general, a loss of
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61 mechanical properties that need to be compensated with the use of cementitious binders or
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62 stabilizers. The most used stabilizer for base layers is Portland cement (PC), a material with a high
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63 carbon footprint and therefore not sustainable. One of the possible substitutes for PC is AAM. A
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64 properly designed alkali-activated binder could contribute to a reduction on carbon footprint, high early
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65 strength, low water permeability and higher resistance to chemical attacks [17,18]. However,
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66 designing the alkaline-activated binder is not an easy task, especially when aspiring for sustainability:
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67 the type and amount of raw materials must be carefully selected.
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23 68 The objective of the present review is to give a state of the art of the use of cementitious binders with
24 69 RAP and highlight the potential and challenges of using RAP with AAM (RAP-AAM). The research
25 70 focus on the use of this material for base-subbase layers of flexible pavements or in semi-rigid
26 71 pavements.
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28 72 This literature review aims to investigate the possibility of incorporating RAP as aggregate
29 73 replacement and AAM as PC replacement on base and subbase layers.
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31 74 This review will start describing RAP, the use of RAP in road construction, the impact and challenges
32 75 of using RAP aggregates with cementitious binders. AAM will be introduced in section 2.4 and
33 76 followed by an assessment of the available literature on RAP aggregates used with AAM. The
34 77 discussion section will debate the importance of selecting local materials for alkali-activation, the
35 78 performance and durability of RAP-AAM, and how the selection of materials impacts life cycle
36 79 analysis. The final sections will discuss the future research needs, challenges facing the application of
37 80 RAP-AAM on pavements base layers and the conclusion.
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81 2. State of the art
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41 82 2.1. Reclaimed asphalt pavement (RAP) aggregates
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43 83 Reclaimed Asphalt Pavement is a material obtained during the removal of distressed pavement
44 84 sections for renovation. The EU standard NBN EN 13108-8:2016 defines reclaimed asphalt as “the
45 85 processed site-won asphalt, suitable and ready to be used as a constituent material for asphalt, after
46 86 being tested, assessed and classified according to this standard”. The assessment includes particle
47 87 size distribution, type of binder and content, presence of foreign matter (cement concrete, bricks,
48 88 subbase material, synthetic materials, metal, wood or plastics), as well as the homogeneity and
49 89 frequency of testing of the feedstock (NBN EN 13108-8:2016).
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90 Milling machines may be costly and, in some developing countries, backhoes and bulldozers are often
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52 91 used to rip and break the pavement in an uncontrolled milling procedure. Ripping and breaking the
53 92 pavement brings variations in the characteristics and quality of RAP aggregates [19].
54 93 For many years, the production of new (hot and cold) bituminous mixes incorporates some amount of
55 94 RAP. There is an indication that the replacement of virgin aggregates (VA) by RAP has a positive
56 95 effect on rutting and stiffness and contradictory reports on the fatigue resistance of pavements [20–
57 96 25]. Nevertheless, the employment of RAP in surface pavements has become common practice in
58 97 many European countries such as Germany, Netherlands, Denmark and Belgium [26]. The
59 98 employment of RAP in new asphalt mixes is beyond the scope of this review. Antunes et al. [9] and
60 99 Zhang et al. [12] recently published a comprehensive study of this subject.
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100 Despite the recent recycling activities, large quantities of unused RAP are disposed of in stockpiles or
1 101 landfills worldwide [27]. Recently, it is possible to see an effort to promote a higher use of RAP in
2 102 unbound layers and other pavement layers (base or subbase). RAP can be used as a substitute for
3 103 virgin aggregates (VA), thus reducing its disposal and demand [28]. Some studies claim that the
4 104 recycling of RAP could reduce the overall cost of pavement sections by 40%-46% [29,30].
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6 105 The biggest challenge on the use of RAP on cementitious binders is due to the thin, aged bitumen
7 106 coating on the surface of the aggregate, which leads to inferior properties [31,32]. RAP performance
8 107 is often improved by blending with VA or stabilizing with additives.
9 108 In general, RAP aggregates are inferior to VA regarding its gradation, strength and stiffness [31]. The
10 109 hydrophobic asphalt layer on the interface of the aggregate is responsible for the lower water
11 110 absorption of the material and the weak bonding between the aggregate and the cementitious mortar
12 111 [31,33–35]. According to Saride et al. [31], the exposed area of aggregates ranges from 15% to 70%
13 112 (averaging 34%), but beneficiation process can help on the partial or complete removal of the coated
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113 asphalt. Some beneficiation methods use solvents to facilitate the cleansing of the aggregates, but
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114 those are considered expensive and unviable at large scale [33].
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17 115 Singh et al. [33] studied the impact of several RAP beneficiation methods on the mechanical
18 116 properties of OPC based concrete. The authors only tested mechanical methods (i.e. did not use any
19 117 solvent) such as sieving, washing and AB&AT (abrasion and attrition). In the latter, the beneficiation
20 118 method involves a concrete tumble mixer fed with RAP along with several charging balls. The results
21 119 found a small improvement in mechanical properties from sieving to washing and more substantial
22 120 improvement for samples produced with aggregates from AB&AT method. Portland cement concrete
23 121 (PCC) produced with treated RAP aggregates presented lower water absorption, coefficient of
24 122 sorptivity and permeable voids than the ones produced with VA. Brand at al. [36] compared washed
25 123 and “dirty” coarse RAP replacement (up to 50%) and concluded that washing did not improve the
26 124 strength of the concrete.
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28 125 Screening through the 4.75 mm sieve separates the coarse and fine fraction of RAP. Fine RAP is
29 126 coarser than natural sand aggregates, likely due to the bitumen acting as an adhesive to fine RAP
30 127 particles [29,37]. Both fractions show lower specific gravity and bulk density than natural aggregates,
31 128 possibly a consequence of the low-density of the asphalt coating. The aggregates may present a
32 129 higher water absorption due to the increased water demand from the dust layer [29,30,38].
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34 130 Age may also play a role in the properties of RAP aggregates. Singh et al. [39] observed that coarse
35 131 RAP aggregates from new pavements yielded a concrete less workable and with worse hardened
36 132 properties than an old RAP. The new RAP aggregate was from 2.5 years old pavement freshly milled,
37 133 while the old aggregate was from 20 years old pavement with eight months of stockpiling. Older RAP
38 134 aggregates originated from pavements which have been a long time in service or stockpiles have
39 135 more oxidized asphalt layer. Brand and Roesler [40] suggested that chemical oxidation could
40 136 successfully modify the surface chemistry of the asphalt leading to better wettability and bonding with
41 137 cement paste. The authors used an oxidation/ pre-treatment for asphalt: nitric acid (HNO3), sulfuric
42 138 acid (H2SO4), hydrochloric acid (HCl), phosphoric acid (H3PO4), potassium permanganate (KMnO4),
43 139 maleic anhydride (C2H2(CO)2O) and ultraviolet light (UV).
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45 140 2.2. The use of RAP aggregates in pavements base layers
46 141 Pavement structure comprises several layers and all of which offers a different opportunity for the use
47 142 of more sustainable materials. Despite the overall choice of the pavement structure (flexible, semi-
48 143 rigid or rigid), lower layers present the higher prospects to incorporate high volumes of sustainable
49 144 materials (especially cement-treated subbase/base layer) [2]. The typical base layers can be unbound
50 145 granular, asphalt treated, cement treated, permeable and recycled. Whereas subbase may be absent
51 146 if there is an appropriately strong subgrade or low traffic [41].
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53 147 Figure 1 illustrates the typical/possible cross-sections of different types of pavements [2]. Sustainable
54 148 actions on materials for those pavement layers mostly consider replacing natural aggregates for
55 149 recycled ones and also replacing PC used as binder/stabilizer with greener binders.
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57 150 RAP and other recycled aggregates are a suitable alternative when opting for unbound layers (layers
58 151 GB and GS in Figure 1). However, the greatest opportunity to use a combination of RAP with AAM for
59 152 pavement layer is while considering cement-treated bases (such as layers CT and maybe GS) and
60 153 concrete layers (RC, LC and LCL).
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154 When used as unbound aggregate, studies show that 100% RAP reduces the strength and increase
1 155 the permanent potential deformation of the unbound bases [42]. Seferoğlu et al. [43] have found that
2 156 the performance significantly increases with 3% PC treatment. According to the authors, RAP- 3% PC
3 157 and 20% RAP – 80% VA have similar deformation performance, which was 50% less than that of a
4 158 conventional base course made with 100% VA.
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8 asphalt layers (AL) concrete surface layer (CS)
asphalt layers (AL)
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10 Cement treated, roller
granular base (GB) compacted or lean concrete lower concrete layer (LCL)
11 (CT/RC/LC)
12 base and subbase (B&S)
cement treated subbase (CT) granular subbase (GS)
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14 compacted subgrade
compacted subgrade compacted subgrade
15 159
16 160 (a) (b)Pavement (b)
Semi-Rigid (c) Rigid Pavement (c)
Flexible Pavement (a)
17 161 Figure 1. Typical cross-section of pavements (a) flexible, (b) semi-rigid and (c) rigid pavements. Modified from
18 162 Plati [2]
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20 163 The strain capacity appears to be also a function of the binder content present on the RAP particles
21 164 [11]. Arshad and Ahmed [28] presented results from other authors who systematically agree that RAP
22 165 addition to VA will (i) decrease the dry density, (ii) decrease the bearing capacity (measured by the
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23 166 California Bearing Ratio – CBR) and (iii) increase the resilient modulus .
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25 167 Roller compacted concrete (RCC) with RAP aggregates is also an alternative for wearing course in
26 168 semi-rigid pavements (RC in Figure 1). A 50% RAP replacement in RCC (fine and coarse aggregates)
27 169 reduced the 28 days compressive strength and conversely increased the flexural strength [44].
28 170 According to Debbarma et al. [30], RAP aggregates also help reducing the permeable voids, water
29 171 absorption in RCC, as well as lowering the cost per cubic meter of RCC mix in 46%.
30 172 The term full-depth reclamation (FDR) is found in the literature to designate stabilized bases
31 173 composed of recycled RAP together with parts of underneath aggregates [9,45]. The study of
32 174 Castañeda López et al. [46] shows that the additions of RAP in cement-treated base (CTB) as FDR
33 175 may reduce the flexural strength but leads to more ductile behavior. The fatigue life of cement-treated
34 176 RAP depends much on the composition (PC and RAP content) and the thickness of the layer.
35 177 Consequently, it is possible to use higher RAP content by playing with other variables (PC content
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178 and thickness).
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38 179 2.3. RAP as aggregate in Portland cement (PC) matrices
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40 180 Studies on RAP as an aggregate replacement choose between replacing either the fine or the coarse
41 181 fraction, with few researches replacing both fractions at the same time (see Table 1). The level of
42 182 replacement also varies, and a combination of RAP aggregates and natural aggregates is often
43 183 employed. Overall, the employment of RAP aggregates in PC based matrices has a significant effect
44 184 on both fresh and hardened state [47].
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185 Singh et al. [29] studied the incorporation of coarse and fine RAP into PC concrete and found a
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186 significant reduction in workability of samples. The strength reduction was more substantial with the
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187 employment of the fine fraction. When compared with concretes containing VA, the replacement of
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188 100% coarse RAP reduced the slump by 29%, while 100% fine RAP reduced the slump by 100%.
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189 The authors attributed this to the absorption of the mixing water by the dust that accumulated one
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51 190 RAP during stockpiling. A reduction in workability was also observed by other authors [34,47],
52 191 although opposite findings were also reported [36,48,49]. In general, it is still not clear how the
53 192 following different parameters affect the workability of the fresh product: (i) hydrophobic properties
54 193 and the high viscosity of the asphalt layer on the aggregate surface; (ii) high water demand of the
55 194 adhered dust layer and (iii) the particle shape of the aggregates.
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59 1
60 defined as a ratio of deviator stress to the resilient strain experienced by the material under repeated loading simulating traffic
load [28].
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Compressive Strength Splitting tensile strength
6 Author Type of RAP Replac. w/c Modulus (GPa)
(MPa) (MPa)
7 0% 0.5 42.06 3.38 34.8 ELAS
8 20% 0.5 31.21 2.90 26.8 ELAS
Su et al. [34] Coarse + Fine 40% 0.5 23.12 2.28 19.9 ELAS
9 70% 0.5 17.33 1.90 14.5 ELAS
10 100% 0.5 11.93 1.51 10.5 ELAS
25.84 LONG
11 Brand and Roesler [40] Fine 100% 0.42 15.89 2.42
25.98 TRAN
12 0% 0.40 33.61 4.39 32.95 ELAS
13 Shi et al. [48] Coarse (different sources) 20% 0.40 23.78-30.54 4.18-4.45 27.07-30.45 ELAS
40% 0.40 17.77-26.97 3.05-3.92 24.06-26.14 ELAS
14 0% 0.47 73.8 - -
Thomas et al. [50] Coarse
15 25%-50% 0.47 47.4-30.1 - -
Fine 0% 0.44 ~51 ˜4.9 -
16 Abraham and Ransinchung [38]
25%-100% 0.44 ~46-34 ˜3.3-2.3 -
17 Ref 0% - 17.8 - -
18 Coarse/ Old 25%-100% - ~13-9.0 - -
Singh et al. [39]
Coarse/ New 25%-100% - ~11-5.3 - -
19 Fine/ Old 25%-100% - ~11-7 - -
20 Fine/ New 75%-100% - ~5.5-4 - -
21 Ref 0% 0.38 ~43 ˜4.6 -
Singh et al. [29] 50% 0.38 35.3 ˜2.6 -
22 Fine
100% 0.38 27.2 ˜3.7 -
23 Reference 0% 0.37 ~37 ˜4.2 -
50% 0.36 ˜28 ˜3.6 -
24 Coarse
100% 0.35 ˜25 ˜3.2 -
25 Debbarma et al. [30]
50% 0.40 ~39 ˜2.6 -
Fine
26 100% 0.39 ~32 ˜2.8 -
50% 0.40 ~29 ˜2.8 -
27 Coarse + Fine
100% 0.41 ~23 ˜2.2 -
28 Reference 0% 0.5 37.7 3.21
Coarse 100% 0.5 22.1 3.06
29 Huang et al. [49]
Fine 100% 0.5 18.8 2.54
30 Coarse + Fine 100% 0.5 10.4 1.59
31 0% 0.6 30.1 3.1 31.1 ELAS
20% 0.6 23.8 2.8 28.9 ELAS
32 40% 0.6 20.7 2.3 24.6 ELAS
El Euch Ben Said et al. [51] Coarse +Fine
33 60% 0.6 16.7 2.2 22.3 ELAS
75% 0.6 13.7 2.0 20.1 ELAS
34 100% 0.6 11.4 1.7 14.5 ELAS
35 Reference 0% 0.45 ~34 28.52 ELAS
36 Papakonstatinous [52] Fine 20-100% 0.45 ~33-24 - 26.78-22.88 ELAS
Coarse +Fine 5-15% 0.45 ~30-28 - 26.94-29.97 ELAS
37 0% 0.57 ~46
Shatarat et al. [53] Coarse
38 20-100% 0.57 ~45-30
39 0% 0.53 38.58 3.73 32.95 ELAS
Hossiney et al. [54] Coarse +Fine
10-40% 0.53 34.03- 17.38 3.11- 2.34 27.57- 16.20 ELAS
40 0% 0.37 46,0 6.3 44.4 ELAS
41 Brand et al. [36] Coarse
20% 0.37 37,2 4.7 37.4 ELAS
35% 0.37 32.7 3.4 31.9 ELAS
42 50% 0.37 27.9 3.0 30.9 ELAS
43 195 Table 1. RAP replacement on OPC based matrices and strength results (28 days)
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196 Through the production of RAP-PCC, it is possible to observe the formation of three interfacial
1 197 transition zones (ITZ) in the microstructure: between (i) the aggregates and asphalt mortar, (ii)
2 198 aggregates and cementitious mortar and (iii) asphalt mortar and cementitious mortar (Figure 2). The
3 199 weakest ITZ is the one formed between asphalt mortar and cementitious mortar [29,51]. Brand and
4 200 Roesler [35] observed that ITZ changed as the samples aged; overtime the samples with RAP
5 201 developed higher porosity, larger ITZ width and fewer hydrates. The authors suggested that the high
6 202 pH of the pore solution could leach organic compounds from the asphalt, which compromises the
7 203 hydration process and formation of calcium hydroxide (CH) and calcium silicate hydrate (C-S-H). The
8 204 consequence is the weakening of the ITZ over time.
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27 205
28 206 Figure 2. ITZ SEM images x80(a) and x1000(b) magnification [51]
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30 207 Fracture samples with RAP have shown that most of the cracks propagated within the asphalt layer
31 208 on the aggregate [40] instead of an adhesive failure of the asphalt-cement paste.
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209 As a consequence, the use of fine and/or coarse RAP aggregates in the production of PCC can
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210 drastically reduce the mechanical properties, such as compressive strength, splitting tensile strength
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211 and elastic modulus, as well as increase the toughness of the material [29,34,38,39]. Abraham and
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212 Ransinchung [38] used fine RAP to produce mortars and observed a reduction of 41.7% on
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213 compressive strength, 39.3% on flexural strength and 51.5% on splitting tensile strength. Concretes
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38 214 with 20-50% coarse aggregate replacement presented 30-60% compressive strength reduction [50].
39 215 In general, a less significant reduction in mechanical properties is observed when only coarse RAP is
40 216 used [29]. However, the study of Debbarma et al. [30] on roller-compacted concrete, found that fine
41 217 RAP mixes had a better compressive strength performance than the ones with coarse RAP. The
42 218 improvement in strength was most likely due to the specific properties of the fine RAP used, such as
43 219 low asphalt content and better gradation.
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45 220 The inclusion of RAP on concretes and mortars reduces the splitting and flexural strength of the
46 221 samples, which is more prominent when fine RAP is used [30,34,38]. However, the percentage
47 222 reduction in flexural strength is lower than the compressive strength [36,48]. It is believed that better
48 223 flexural performance is due to the visco-elastic nature of the asphalt coating, which also is responsible
49 224 for an increase in the toughness of the mixes [49].
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51 225 Shatarat et al. [53] tested concrete columns and observed a 31.06% reduction in the compressive
52 226 load capacity in comparison with the control sample. The RAP samples also showed less cracking
53 227 and lower spalling. The coefficient of thermal expansion and drying shrinkage do not seem to be
54 228 impacted by the use of RAP aggregates [54].
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56 229 2.3.1. Durability
57 230 The porosity of mortars increases in the presence of fine RAP aggregates due to the more porous
58 231 and larger ITZ. Mercury intrusion porosimetry (MIP) analysis showed an increase in mesopores and
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232 macropores. According to Abraham and Ransinchung [55], the threshold diameters and large
1 233 capillaries decreased up to 50% RAP replacement, followed by an increase of both after that,
2 234 suggesting a higher risk for chemical ingression [55].
3
4 235 The use of coarse RAP was found to decrease the water absorption on concretes, the concentration
5 236 of total permeable voids and sorptivity [29,30]. However, Abraham and Ransinchung [38,56] noted
6 237 that this behavior was in contradiction with the higher porosity of the RAP aggregates. The authors
7 238 suggested that the decrease in sorptivity was due to the molten asphalt clogging the pores of the
8 239 samples during oven drying. To avoid the melting of the asphalt present in RAP, the authors have
o
9 240 adopted a different preparation procedure, and vacuum dried the samples at 35 C. Singh and
o
10 241 Ransinchung [57] suggested oven drying at 48 C for eight days.
11 242 The inclusion of fine RAP can significantly impact the abrasion resistance of concrete samples; there
12 243 is a 75% reduction on abrasion resistance when 100% RAP replacement is employed [58]. Still,
13 244 samples produced with either coarse and fine RAP mixes produced enough abrasion resistance to be
14
245 used as pavement’s wearing course [30].
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16 246 The replacement of VA with fine RAP had an impact on the pH of the hardened concrete; the pH
17 247 reduces as the replacement level increase. This reduction is reported to be subtle (up to 3.8%), and
18 248 all RAP-PCC still present pH values above 12 [58]. No carbonation was observed after 120 days of
19 249 moist curing [30,58].
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21 250 Under sulphate attack, RAP-PCC samples also showed a higher mass and strength loss than the
22 251 reference PCC, with rates increasing with RAP content [30,56]. Singh et al. [58] reported a weight
23 252 loss of nearly 11.26% for concrete samples produced with 100% fine RAP replacement under H 2SO4
24 253 exposure.
25
26 254 The freeze and thaw resistance of PCC is associated with the concrete’s ability to withstand the water
27 255 expansion inside its pores and cracks during thermal cycling. It is also directly related to the material’s
28 256 pore structure. In that sense, the higher percentage of air voids in RAP-PCC is beneficial and can
29 257 help accommodate the expanding freezing water without damage to the matrix. Guo et al. [47] and
30 258 Thomas et al. [50] reported an increase in freeze-thaw resistance when VA is replaced by RAP
31 259 aggregates, while Brand et al. [36] observed a reduction.
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260 2.4. Alkali activated materials as binders
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34 261 The term alkali activation may be applied to the reaction between any aluminosilicate precursor and
35 262 an alkali activator to produce a new binder [59–61]. Precursors are usually in powder form and may
36 263 be natural occurring pozzolans, calcined clays or industrial by-product and wastes, such as
37 264 granulated blast furnace slag, granulated phosphorus slag, steel slag, coal fly ash, volcanic glass,
38 265 zeolite, metakaolin, silica fume and non-ferrous slags [59,62]. Depending on the Al and Ca content,
39 266 AAM may be further classified as inorganic polymers or geopolymers (Figure 3), or simply as low-
40 267 calcium (low-Ca) and high-calcium (high-Ca) AAM. As for activators, the most frequently used are
41 268 sodium silicate, sodium hydroxide, sodium carbonate, potassium hydroxide and potassium silicate
42 269 [63]. Hoy et al. [64,65] observed that the presence of sodium silicate in the alkali solution increased
43 270 the speed of the alkaline activation. However, the ideal amount of activators may vary according to
44 271 the type of precursor; and excess of activator results in loss of strength [66].
45
46 272 2.4.1. Ground Granulated Blast Furnace Slag (GGBFS) and Metakaolin (MK) based AAM
47
273 High-Ca AAM is mainly represented by the alkali-activation on GGBFS, while low-Ca AAM is
48
274 commonly produced with pulverized fly ash (PFA) and metakaolin (MK). This section will compare the
49
275 activation of GGBFS and MK as examples of high and low-Ca systems.
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54
55
56
57
58
59 2
60 Threshold diameter is the pore size through which mercury penetrates the bulk of the sample, i.e. the equivalent pore size
corresponding to the steepest slope of the curve [104,105].
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63 7
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1
2
3
4 Portland
5 based
cements Calcium
6 sulfo-
7 aluminate
8 cements
9 Ca content
10 Alkali-activated
11 materials
12
Inorganic
13 polymers
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15
16 Geopolymers
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19
20
Al content
21 276
22 277 Figure 3. Classification of AAM and comparison with other systems (modified from [67] )
23
24 278
25
26 279 GGBFS is a latent hydraulic material and, as such, it requires water and a minimal amount of a
27 280 catalyst or activator to show cementitious properties. When mixed with Portland cement, GGBFS is
28 281 activated by the calcium hydroxide and alkalis formed during the hydration of the cement. In general,
29 282 the activation is carried out using an alkali solution made with an alkali hydroxide, silicate, carbonate
30 283 or sulphate, but combining sources (sodium hydroxide and sodium silicate) can yield even higher
31 284 strength results [68]. Wang, Scrivener and Pratt [69], employed individual activators and concluded
3
32 285 that sodium silicate solution with silica modulus from 1 to 1.5 achieved best mechanical performance.
33 286 When using sodium hydroxide, the authors recommended keeping the Na2O concentration within 3
34 287 and 5% by slag weight. They reported that lower Na2O percentages might delay the activation
35 288 process, while higher values may result in efflorescence and brittleness.
36
289 The alkaline activation of GGBFS is represented by blue pathway for activation of high calcium
37
290 systems in Figure 4, with the following steps: (i) dissolution of the aluminosilicate’s glassy particles; (ii)
38
291 nucleation and growth of the initial solids; (iii) boundaries binding of the formed phases and (iv)
39
292 ongoing reaction products formed. The main reaction product formed by alkaline activation of GGBFS
40
293 is calcium (alumino)silicate hydrate (also known as C-A-S-H type gel), and secondary phases such
41
294 as layered double hydroxides and/or an alkali aluminosilicate N-A-S-(H) type gel (can also show
42
295 substitution of potassium) [59,70–72].
43
44 296 According to the literature, a properly designed alkali-activated slag shows improvements in many
45 297 properties compared to OPC – higher strength, more resistant to acids, sulphates or chlorides and fire
46 298 resistance [62]. However, AAS may also present some issues such as rapid setting, high shrinkage,
47 299 the formation of micro-cracks, the possibility of alkali-aggregate reaction and high efflorescence [68].
48 300 The addition of superplasticisers and water reducers designed for PC into AAS seems to have a
49 301 negligible effect on workability and setting time [62].
50
51 302 Metakaolinite (Al2Si2O7) also known as metakaolin (MK) is a product from the dihydroxylation of an
o
52 303 aluminosilicate clay mineral kaolinite (Al2(Si2O5)(OH)4) at a temperature of between 450 - 800 C.
53 304 During calcination, the kaolinite releases OH- from its structure, which becomes amorphous and
54 305 reactive. MK has CaO as impurities; it is a system composed mainly of (Si+Al), while BFS is a
55 306 (Si+Al+Ca) system [73]. Like other pozzolans, MK does not have cementitious properties, but when
56 307 used with PC, it is a highly reactive pozzolan which reacts with the hydrated lime to form C-S-H [74].
57 308 The addition of MK to PC based systems can improve the mechanical strength, reduce the pore
58 309 structure and mitigate some chemical attacks, such as alkali-silica reaction [75,76].
59
60 3
SiO2/M2O molar ratio, where M is an alkali metal.
61
62
63 8
64
65
1
2
3
4
5
6
7
8
9
10
11
12
13
14
15
16
17
18
19
20
21
22
23 310
311 Figure 4. Process and reaction products of AAM – high and low calcium systems (modified from [70] )
24
25
312 MK is also suitable for alkali activation yielding a material with high compressive strength, elastic
26
313 modulus and lower porosity. Best properties are achieved in the presence of soluble silicates with the
27
314 silica moduli of the final solution between 1 and 2 [70]. The reaction sequence of low calcium systems
28
315 (green path on Figure 4) is similar to the one for high calcium, but the main reaction product is an
29
316 alkaline aluminosilicate hydrate (N-A-S-H gel) with zeolite-like secondary phases. The absence of (or
30
317 low content) calcium hinders the formation of crystalline phases associated with expansions (ettringite
31
32 318 and gypsum), and the end products have better chemical stability [77]. When properly designed, the
33 319 final geopolymeric product has a quicker setting time, higher compressive strength, better resistance
34 320 to seawater and sulphate attach, and higher heat resistance than PC systems [61,77].
35 321 Nevertheless, the alkaline activation of MK represents a higher environmental impact than the
36 322 activation of GGBFS. First, kaolin clay is a natural material, and its utilization represents the depletion
37 323 of natural resources. Secondly, the calcination of kaolinite demands the burning of combustible fuels,
38 324 which then releases CO2. MK activation mainly requires sodium silicate to provide the soluble silica to
39 325 accelerate the hardening; however, the production of silicates is itself a heavy environmental burden
40 326 [78]. Because of all that, GGBFS is the preferable aluminosilicate over MK, when the first is available.
41 327 The mix of GGBFS and MK (binary system) is a potential solution to achieve an end material with
42 328 high compressive strength, lower porosity [79] and lower shrinkage than ASS [80]. Binary systems
43 329 show improvement in properties while still reducing the amount of alkaline activator needed for neat
44
330 MK activation. Figure 5 shows that the activation of blended MK/GGBFS favors the formation of a
45
331 denser matrix composed of C-A-S-H and N-A-S-H gels, which improves the overall properties.
46
47 332 2.5. RAP and alkali-activated materials
48
49 333 Many researchers have successfully studied the incorporation of RAP in base/subbase layers for
50 334 pavement section; for high replacement levels, the loss on mechanical properties needs to be
51 335 compensated by using stabilizers, i.e. agents that increase the compressive and impact strength, as
52 336 well as the overall integrity of the layers (reduction of swelling, shrinkage, abrasion, etc.) [32,81]. It is
53 337 possible to stabilize RAP using materials such as lime, cement, fly ash, blast furnace slag, rice husk
54 338 ash, sugar cane bagasse ash, among others [29,66,82,83]. The stabilizer’s content varies depending
55 339 on the type of stabilizer employed, but it usually ranges from 4% to 30% in mass of RAP (see Table
56 340 2). While the high dosage of Ca-rich stabilizers is discouraged - it causes shrinkage, cracking and
57 341 failure of the pavement - the use of low-Ca stabilizer may not impair sufficient strength. Therefore,
58 342 sometimes, it is possible to employ alkali activation to meet the strength requirement for base
59 343 materials [81]. The use of alkali activation in RAP base/subbase layers may help compensate the
60 344 strength loss.
61
62
63 9
64
65
345
1
2
3
4
5
6
7
8
9
10
11
12
13
14
15
16
17
18
19 346
20 347 Figure 5. EDX spot analysis of MK+GGBFSS systems [79]
21
22 348 The literature on the alkaline activation of base/subbase pavement layers containing RAP materials is
23 349 still limited. Hoy et al. [65] and Horpibulsuk et al. [84] presented results of alkali-activated base
24 350 courses made with RAP and stabilized with high calcium (CaO >10%) pulverized fly ash (PFA). The
25 351 SEM and XRD analysis indicate that the main activation products were C-A-S-H and N-A-S-H gels
26 352 and that the coexistence of both hydrates increased the strength, which was proportional to the
27 353 Na2SiO3 content. The absence of silicates resulted in low geopolymerization for RAP-PFA systems,
28 354 as in conventional alkali-activated concretes [65]. The authors also found C-S-H as a hydration
29 355 product is systems with a higher calcium content such as those with GGBFS [64].
30
31 356 These preliminary studies also conclude that similarly to the RAP-OPC systems, the presence of the
32 357 asphalt layer is detrimental do the binding of RAP to the matrix. In other words, the RAP particles
33 358 presented better bonding to the matrix for exposed aggregate surfaces (no asphalt layer). Hence,
34 359 better performance may be achieved if a milling procedure guarantees a higher exposed aggregate
35 360 area [31].
36 361 While studying the incorporation of RAP and PFA on different types of soil for road base and subbase
37 362 layers, Adhikari [66] observed that an increase in the PFA and RAP content increased the strength of
38 363 the geopolymer mixture up to 7 times compared with untreated soil. The elastic modulus and fracture
39
364 energy also increased. However, when compared with OPC stabilized samples, the alkali-activated
40
365 ones were more flexible and presented lower compressive strength and stiffness [86]. Other authors
41
366 also observed the positive effect of increasing the PFA content [37,84]. Curing conditions also appear
42
367 to have a significant impact on the mechanical properties, since it increases de dissociation
43 o
368 (reactivity) of the phases. Alkali activated RAP samples cured for seven days at 40 C presented
44
369 approximately 70% higher strength than reference samples cured at room temperature [37]. However,
45
370 high-temperature curing is not practical for on-site applications.
46
47 371 Wet-dry cycles are commonly used to simulate weather changes over time and estimate durability.
48 372 Avirneni et al. [81] observed that activated PFA as stabilizers for RAP: VA mixes had an acceptable
49 373 performance under aggressive wet/dry cycles, with less than 10% weight loss. Alkali activated
50 374 systems presented lower weight loss on wet-dry cycling than non-activated ones. After six wet/dry
51 375 cycles, the formation of macro- and micro-cracks caused a strength reduction, which was more
52 376 significant for lower NaOH contents [87].
53
54 377
55
56
57
58
59
60
61
62
63 10
64
65
1
2
3
4
5
6 Stabiliser Akali activator UCS
Author RAP:VA
Type Quantity Type Quantity 28 days (MPa)
7
NaOH (10M) ~3.9
8
NaOH:Na2SiO3 - 90:10 ~4.0
9 Hoy et al. [65,85] 100:0 FA 20% -
NaOH:Na2SiO3 - 60:40 ~4.9
10
NaOH:Na2SiO3 - 50:50 ~5.6
11 80:20 20%-30% 2- 4% ~4.3 – 4.9
12 Saride; Avirneni; Challapalli
80:20 FA 30% NaOH 2- 4% ~4.7 – 5.1
13 [31]
60:40 20% 2- 4% ~4.6 – 5.7
14 Avirneni; Peddinti; Saride [81]
60:40 30% 2- 4% ~5.0 – 5.4
15 FA 4% NaOH:Na2SiO3 L/B =0.3-0.5 ~1.4
16 2%+2% NaOH:Na2SiO3 L/B =0.3 ~1.6
17 Mohammadinia et al. [86] 100:0 FA +BFS 2%+2% NaOH:Na2SiO3 L/B =0.4 ~1.7
18 2%+2% NaOH:Na2SiO3 L/B =0.5 ~1.6
19 BFS 4% NaOH:Na2SiO3 L/B =0.3-0.5 ~1.9
20 Mohammadinia et al. [37] 100:0 FA 4%-16% Na2SiO3/NaOH(8M)= 2.5 L/B =0.4 ˜1.2-1.4 (7 days)
21 20%, 30% NaOH (10M) - ˜4 – 5
22 20%, 30% NaOH:Na2SiO3 -90:10 - ˜4 – 4.3
Horpibulsuk [84] 100% FA
23 20%, 30% NaOH:Na2SiO3 - 60:40 - ˜5 – 5.5
24 20%, 30% NaOH:Na2SiO3 - 50:50 - ˜5.5 – 6
25 10- 20% NaOH (8M) ~1.1 – 2.0
26 10 - 20% NaOH:Na2SiO3 - 70:30 ~1.0 – 2.3
Hoy et al. [64] 100:0 BFS -
27 10 -20% NaOH:Na2SiO3 - 60:40 ~1.7 – 3.0
28 10 - 20% NaOH:Na2SiO3 - 50:50 ~1.5 – 2.2
29 0% - - - - 1.4
30 0% FA 15%-25% - 1.6-5.38
Adhikari et al. [66] NaOH (6-8M)
0% PC 5%-10% - 1.02-3.20
31 Na2SiO3/NaOH (0 -0.5)
15%-25% FA 0-25% - 1.62-4.98
32
378 Table 2. Summary of the studies on alkali-activated matrices containing RAP
33
34
35
36
37
38
39
40
41
42
43
44
45
46
47 11
48
49
379 One great environmental concern when using wastes and alkali-activated materials is the possibility
1 380 of contamination of soil and watercourses due to leaching. The durability of base layers and its ability
2 381 to sustain the pavement may also be affected by the leaching of the stabilizers during its service life.
3 382 Preliminary studies comparing the leaching of stabilized RAP with and without alkali activation have
4 383 concluded that the environmental impact on soil and groundwater is minimal. The studies assessed
5 384 the leaching of heavy metals, pH and sodium, concluding that the employment of an activator has
6 385 reduced the leachability of metals from the aluminosilicate source [65,81,84]
7
8
386 3. Reflections from literature
9
10 387 The current recycling opportunities for RAP aggregates have been unable to consume all of the
11 388 produced RAP, and more alternatives are needed. Although great success is being achieved when
12 389 RAP is recycled in asphalt layers [88–90], the same cannot be said for base and subbase layers. The
13 390 use of RAP for unbound base layers represent a reduction in strength and attempts to compensate
14 391 this reduction often means:
15
16 392 1. Blending it with virgin aggregate. Which reduces the amount of recycled materials used and
17 393 therefore the reduces the sustainability prospect of the solution.
18 394 2. Using binders or stabilization. PC will add an environmental burden to the solution, and
19 395 supplementary cementitious materials (such as pulverized fly ash, BFS and rice husk ash) take
20 396 longer time to react and may not add sufficient strength.
21
22 397 The presence of the thin asphalt coating in the surface of the RAP aggregate is the main reason for
23 398 the binder’s poor performance. The asphalt weakens the ITZ, making it larger and more porous. RAP
24 399 beneficiation methods targeting the increase of the exposed aggregate surface could represent a
25 400 significant gain in strength. While the more porous ITZ could represent a gain in freeze and thaw
26 401 resistance, it also compromises the durability by permitting the ingress of harmful substances. RAP
27 402 beneficiation methods targeting the increase of the exposed aggregate surface could represent a
28 403 significant gain in strength and durability of RAP-PCC.
29
404 The literature on RAP with AAM is very scarce, and some important factors remain unanswered.
30
405 Similarly to RAP-PPC solution, the ITZ is also a reason for concern. However, it is unclear if different
31
406 precursors and alkali solutions could improve de binding between the different ITZ sections. The use
32
407 of a properly designed AAM may promote the recycling of RAP by increasing the early strength,
33
408 creating a denser and more resistant (durability) matrix. The application of AAM is very similar to PC,
34
409 and minor changes on the construction practice are expected. However, the costs associated with the
35
410 transportation of the alkali solution must be considered.
36
37 411 3.1. Potential, challenges and research needs for future developments on RAP-AAM
38
39 412 This section covers important topics that have not been addressed so far for the future development
40 413 of RAP incorporated alkali-activated materials. Nevertheless, they are essential to determine the
41 414 potential application of those new materials by the pavement industry. The following section also
42 415 highlights future research needs.
43
44 416 3.1.1. Cost and availability of local materials
45 417 Different from the employment of lime or Portland cement as binders for stabilization of aggregates,
46 418 AAM depend on the availability and costs of the alkaline solutions and precursors used
47 419 (aluminosilicates). In that sense, the overall cost to develop RAP-AAM may surpass the benefits from
48 420 some countries. Sodium silicate and sodium hydroxide, the most common activators used in AAM,
49 421 are rather expensive chemicals in some countries, where AAM have barely become viable for most of
50 422 the possible applications [91]. Each country may have to select the available sources of
51 423 aluminosilicate. Calcium-rich materials (industrial by-products or wastes) are preferred because they
52 424 tend to reduce the demand for alkaline solutions. So, the employment of blast-furnace slag or high-
53 425 calcium PFA may be an option to consider. Agricultural residues such as rice husk ash or sugarcane
54 426 bagasse ash may be viable and inexpensive options for developing countries (Brazil, India, other
55 427 Asian countries), as they are interesting raw materials for alkaline activation [92,93]. However, they
56 428 are usually low calcium and low alumina reactive materials, which therefore depend on another
57 429 source of Al2O3 and high amounts of activators.
58
59 430 The activation may be carried out using blended (or hybrid) systems, e.g. small amounts of lime or a
60 431 reduced amount of OPC to promote the activation with a minimum amount of alkalis and enhance the
61
62
63 12
64
65
432 final properties [94,95]. The study of those blended systems with RAP aggregates is not available,
1 433 and it is a potential topic for investigation.
2
3 434 The activation of local clay materials as binders for RAP-AAM must also be considered and should be
4 435 an object of future research. After all, clay minerals are the main constituent of soils, and the
5 436 availability of this precursors should not represent an issue. The challenges of using natural clays as
6 437 binders for AAM are related to their crystalline nature and consequently, low reactivity [96]. Soil
7 438 stabilization with alkaline materials has been studied, and many publications are now found in the
8 439 literature [97–99]. The activation of soil clay minerals to bind RAP either in base or sub-base courses
9 440 for flexible pavements or in semi-rigid (concrete) bases is a topic not explored as well.
10 441 Overall, it is paramount to assess the economic viability of AAM under two completely different
11 442 perspectives:
12
13 443 Stabilization of RAP in base or subbase courses. In this case, the mechanical requirements are
14 444 low and, therefore, low-reactively materials and small amounts of alkaline activators may be
15 445 employed;
16 446 RAP-alkali-activated concrete used as a rigid base for asphalt surface layers (semi-rigid
17 447 solutions), which demands higher mechanical performance and, hence, large quantities of
18 448 activators in combination with highly-reactive precursors.
19
20 449 3.1.2. Performance and durability of RAP-AAM
21
22 450 The performance and durability of any RAP-AAM systems are closely associated with the amount and
23 451 gradation of RAP used as aggregates, together with any beneficiation methods employed to the
24 452 former. These variables determine the adhesion and ultimately, the mechanical performance of RAP
25 453 to AAM matrices. The choice of low calcium or high-calcium precursors (and consequently the
26 454 amount and type of activators) may also play an important role in the mechanical and durability
27 455 properties. None of these topics has been systematically addressed so far in the published literature
28 456 and represent essential research needs before the implementation of RAP-AAM pavement layers.
29 457 Long-term or accelerated durability tests employed to current pavement layers are also required to
30 458 determine the durability of RAP-AAM under mechanical stresses (fatigue, rutting resistance) [13] as
31 459 well as weathering conditions such as freeze-thaw cycling [87]. Needless to mention the importance
32
460 of assessing the susceptibility to delamination of RAP-AAM concrete base from the asphalt surface
33
461 layer in semi-rigid pavements, stabilizing a comparison with traditional Portland cement concrete
34
462 (PCC) [100].
35
36 463 Leaching of alkalis with consequent contamination of soil and groundwater are questions to be
37 464 answered as well. Leaching is a function of the type of precursor and amount of alkalis used; in
38 465 general, it should not present an issue if the alkali content is limited. On the other hand, alkali-
39 466 activated matrices have proven to be suitable to encapsulate heavy metals and toxic waste [101];
40 467 thus, the leaching of undesirable species could even reduce, including some contaminants in the RAP
41 468 aggregates.
42
43 469 3.1.3. Life cycle assessment of RAP-AAM
44
470 Another object of future research is the life cycle assessment of RAP-AAM pavement layers. The
45
471 environmental impact of AAM as a replacement for PC has been widely discussed [102,103] and the
46
47 472 benefits are dependent on the precursor and amount of solution employed. The same applies to RAP-
48 473 AAM, an LCA comparing RAP-AAM, traditional RAP-stabilized layers and Portland cement concrete
49 474 base layers must be subject for future studies. LCA should be combined with the cost analysis to
50 475 determine when RAP-AAM is viable. So far, it is not possible to say if the challenges to design and
51 476 specify RAP-AAM pavements would be both technically acceptable and economically feasible. Future
52 477 research should definitively address these questions.
53
54 478 4. Conclusions
55
56 479 This paper presented a review of RAP aggregates and its utilization in foundation layers of
57 480 pavements. Alkali-activated materials (AAM) were also introduced as an alternative technology to
58 481 Portland cement-based materials. According to the literature on RAP aggregates in AAM (RAP-AAM),
59 482 it is possible to observe the following conclusions and research needs:
60
61
62
63 13
64
65
483 The biggest challenge facing the use of RAP-AAM is how to overcome the binding issues caused by
1 484 the presence of asphalt. This may be addressed by pre-treating the RAP aggregates or by
2 485 improvements on the binder.
3
4 486 The amount of research on RAP-AAM is limited; few studies presented some mechanical and
5 487 durability properties, without addressing important factors, e.g. the effect of the type of aluminosilicate
6 488 (low calcium or high calcium), type and amount of activator, neat or hybrid systems, as well and
7 489 gradation, amount and beneficiation of RAP.
8 490 The employment of alkali-activated matrices to RAP aggregates depends on the availability and cost
9 491 of precursors for AAM. Local materials may include industrial and agricultural residues and wastes
10 492 and soils, which could be a source of clay materials for alkaline activation.
11
12 493 AAM may be used to stabilize RAP particles, or they could be part of an AAM-RAP concrete base.
13 494 The amount of binder and alkaline materials in the former is much lower. The choice of the system
14 495 determines the mechanical properties, durability and environmental impact, which should be carried
15 496 out via LCA and compared with current solutions.
16
17 497 Funding:
18
19 498 This research was financed in part by Coordenação de Aperfeiçoamento de Pessoal de Nível
20 499 Superior - Brazil (CAPES), Finance code 001.”
21 500 References:
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