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Materials
  • Review
  • Open Access

15 April 2023

The Obstacles to a Broader Application of Alkali-Activated Binders as a Sustainable Alternative—A Review

,
,
and
1
Department of Construction Materials and Technologies, Faculty of Civil Engineering, Budapest University of Technology and Economics, Műegyetem rkp. 3, 1111 Budapest, Hungary
2
Department of Engineering Geology and Geotechnics, Faculty of Civil Engineering, Budapest University of Technology and Economics, Műegyetem rkp. 3, 1111 Budapest, Hungary
3
Institute of Material Technology, Building Physics, and Building Ecology, Faculty of Civil Engineering, TU Wien, Karlsplatz 13, E207-2, 1040 Vienna, Austria
*
Author to whom correspondence should be addressed.
This article belongs to the Special Issue Industrial Symbiosis and Development of New Materials or Products in Building Sector

Abstract

This paper aims to raise awareness regarding the obstacles limiting alkali-activated binders’ (AABs) application as a sustainable solution in the construction industry. Such an evaluation is essential in this industry, which has been introducing a wide range of alternatives to cement binders yet achieved limited utilisation. It has been recognised that technical, environmental, and economic performance should be investigated for the broader adoption of alternative construction materials. Based on this approach, a state-of-the-art review was conducted to identify the key factors to consider when developing AABs. It was identified that AABs’ adverse performance compared to conventional cement-based materials mainly depends on the choice of which precursors and alkali activators to employ and the regionalised practices adopted (i.e., transportation, energy sources, and data on raw materials). In light of the available literature, increasing attention to incorporating alternative alkali activators and precursors by utilising agricultural and industrial by-products and/or waste seems to be a viable option for optimising the balance between AABs’ technical, environmental, and economic performance. With regard to improving the circularity practices in this sector, employing construction and demolition waste as raw materials has been acknowledged as a feasible strategy.

1. Introduction

Alkali-activated binders (AABs) are prepared from solid low- or high-calcium aluminosilicate precursors in a strongly alkaline environment, thus generating hardened binders with cement-like properties. In the contemporary literature, the issue of the necessity of distinguishing between AABs and geopolymers has been widely discussed. A geopolymer is defined as a polymer created by the partial dissolution of an aluminosilicate source in a user-friendly alkaline or acidic medium to construct three-dimensional polymeric networks. On the other hand, the mechanism for the creation of AABs is similar to that of ordinary Portland cement (OPC), where, instead of calcium silicate hydrate gel, potassium or sodium aluminosilicate hydrate is available [1]. Davidovits makes a distinction even between a geopolymer cement and a binder, stating that cement refers to a binding system that hardens at room temperature (e.g., OPC), while a binder requires heat setting [2]. Although some studies tend to use these words interchangeably, the question of differentiating between these terms will not be addressed in this study. Instead, the terms used in the articles under consideration will be primarily provided as they were in the source material.
The application of AABs was introduced due to the lack of OPC availability in the post-World-War-II period [3]. Since the late 1990s, the usage of AABs has been investigated as a sustainable solution in the construction industry [4]. In the initial investigations of AABs’ environmental impacts, Davidovits stated that 1 tonne of geopolymer cement generates 0.18 tonnes of CO2, corresponding to an about five to six times lower value than OPC [5]. In comparison, Duxson et al. emphasised that the use of geopolymer binders can result in an 80% or even greater decrease in CO2 emissions compared to OPC [6]. The trend of introducing AABs as sustainable solutions but focusing mainly on their material performance was recognised while reviewing the literature. Furthermore, there was a lack of review papers tackling the topic of sustainability that considered the technical, environmental, and economic performance of the developed materials. Regarding the adoption of novel green solutions, the evaluation of solely material properties will not result in their wider usage. This paper will address possible obstacles to the broader application of AABs based on the three pillars mentioned above, focusing on its two major ingredients: a precursor and an alkali activator (AA). It will also provide a benchmark for the more mindful selection of ingredients when developing new AABs. This could hasten the steady process of the adoption of sustainable materials in the industry, which is a much-needed change considering the requirements of the codes in place worldwide [7].
In general, selecting the suitable AA depends on the precursor’s composition [3]. Two modes of AA production have been developed:
  • One-part mixtures combine dry alkali powder, solid aluminosilicate raw material, and water. They are suitable for in situ applications due to their advantageous handling characteristics compared to two-part mixtures containing a viscous alkali solution. Since the usage and packaging of this type are similar to those of cement, its utilisation seems promising.
  • Two-part mixtures are formed by combining an aqueous alkali solution, solid aluminosilicate raw material, and water. They have been recognised as suitable for precast applications. However, they pose a disadvantage, as they require the handling of large amounts of corrosive, hazardous, and viscous alkali solutions, which has led to the development of one-part mixtures [8].
However, precursors can be naturally occurring or industrial and agricultural by-products and/or waste. They are mainly composed of SiO2, Al2O3, and CaO [9]. By-products from the energy and mining industries have received much attention with respect to their use as a potential feedstock for AABs [10]. Moreover, solid waste generated throughout mining activities has been recognised as causing severe environmental pollution, and its utilization as raw material would be highly beneficial [11]. The producers of these by-products can benefit from reductions in their required storage and rehabilitation costs if the by-product is disposed of as waste. Additionally, from their sale as raw materials, some economic profit is also possible [10]. Various types of agricultural waste have also been investigated as raw materials for producing AABs [9]. On the other hand, bulk chemicals (e.g., sodium hydroxide, sodium silicate, etc.) are commonly utilised as AAs, while there have been few investigations on the use of industrial and agricultural by-products and/or wastes as alternative alkali sources [3]. In general, alkali hydroxide (ROH), non-silicate salts of weak acids (R2CO3, R2S, and RF), and silicic salts of R2O·(n)SiO2 are widely used, where R corresponds to an alkali metal, i.e., Na, K, or Li [4]. Table 1 presents detailed information about the types of precursors and alternative AAs available in the literature according to the best of the authors’ knowledge.
As this study will also cover AABs’ environmental and economic evaluation, widely used environmental impact assessment and cost analysis methods, namely, life cycle assessment (LCA) and life cycle costing (LCC), are introduced. LCA is a methodology used to evaluate a certain product’s environmental burden during its life cycle [12]. Based on the ISO 14,040 and ISO 14,044 standards, the methodology consists of four main steps: the definition of a goal and scope, an inventory analysis, an impact assessment, and interpretation [12,13]. While LCA is based on evaluating environmental performance, LCC is focused on cost-effectiveness. In contrast with LCA, a general standard for the application of LCC is not present [14]. However, regarding the construction industry, ISO 15686-5 provides guidelines for LCC, which concerns predicting and assessing the cost performance of the constructed assets [15]. LCC generally aims to evaluate the costs of acquiring raw materials, operation, maintenance, and disposal. It can also cover the costs of environmental impacts caused by a product (the so-called “polluter pays” principle). The incorporation of both LCA and LCC seems prudent for identifying the environmental and economic trade-offs of a particular product [14].
Table 1. Types of precursors and alternative alkali activators that are covered in the literature.
Table 1. Types of precursors and alternative alkali activators that are covered in the literature.
Used Material Investigated Performance
Alkali Activator (AA) Precursor Description Used Alkali-Activated Binder’s (AAB) Description Tech. Environ. Eco.
AAS [16]Aluminium-anodising sludge (AAS) is an industrial waste produced in the anodization process of aluminium. It was used together with rice husk ash (RHA) as a precursor, while the alkali activator (AA) consisted of sodium silicate (SS) and sodium hydroxide (SH) [16].[16]
ACS [17]Air-cooled slag (ACS) is a waste material generated by the steel-making process.It was mixed with fly ash (FA) and activated by combining SH and SS [17].[17]
BL [18,19,20] Bayer liquor (BL) is generated during the Bayer process for aluminium production. Concentrated BL was used as the primary activating solution while mixed with FA and silica fume (SF) as dry powders [18,19]. FA/BL geopolymers were also produced with different levels of Ca(OH)2 or ground granulated blast furnace slag (GGBFS) [20]. [18,19,20]
BS [21]Boiler slag (BS) is a waste generated through industrial coal combustion.It was used as a part of the precursor together with metakaolin (MK) and an activator of combined potassium hydroxide (KH) and RHA or SF [21].[21]
CC [22]Calcined clay (CC) is thermally treated clay, e.g., at 700 °C for six hours. It was used as a part of a precursor with FA and activated by a combination of SH and SS [22].[22]
CKD [23][23]Cement kiln dust (CKD) is waste generated during cement manufacturing. It was used in a one-part geopolymer with GGBFS and electric arc furnace slag (EAFS) [23].[23]
CSA [24] Cotton shell ash (CSA) is generated through the combustion of cotton shells. It was dry-mixed with MK, thus forming a homogenous powder, and mixed with deionised water [24].[24]
DE [25,26,27] Diatomaceous earth (DE) is a sedimentary rock rich in amorphous silica.Activating solution using DE was prepared with water and SH, while the precursor used was a fluid catalytic cracking catalyst (FCC) [25]. FA/MK binary system [26] and GGBFS [27] used as precursors were activated by DE and SH [26,27].[25,26,27]
DG [28,29] Desulphurisation gypsum (DG) is generated in coal-fired power plants when sulphur oxide is removed from exhaust flue gases (the same as the REA gypsum). It was used as an activator in AAB together with GGBFS as a precursor [28,29].[28,29][28][28]
DM [30]Dredged material (DM) is the product of dredged sediments from ports and waterways. The AAB included a mix of FA and DM as a precursor and a combination of SH and SS as an AA [30].[30]
EAFS [23]Electric arc furnace slag (EAFS) is a waste resulting from the steel-making process. It was used in a one-part geopolymer with GGBFS and CKD [23].[23]
FA [22,28,30,31,32,33,34,35,36,37,38,39,40,41,42,43,44,45,46,47,48,49,50,51,52,53,54,55,56,57,58,59,60,61,62,63,64,65,66] Fly ash (FA) is a fine powder that is a by-product of burning pulverized coal in power plants. It can be used as a single precursor in AABs [31,34,36,38,39,42,56,61,62,63,64,65,66]. It was also utilised as a part of binary and ternary blended precursors with a variety of conventional and/or alternative precursors [17,22,28,30,32,33,35,37,40,41,43,44,45,46,47,50,51,52,53,54,55,57,58,59,60]. The ternary mix of waste brick powder (WBP), waste ceramic powder (WCeP), and waste concrete powder (WCP) was examined together with integrating FA in the precursor and activating it using a mix of SH and SS [48].[22,28,30,31,32,33,34,35,36,37,38,39,40,41,42,43,44,45,46,47,48,49,50,51,52,53,54,55,56,57,58,59,60,61,62,63,64,65,66][28,46,47,48,59,60][28,60]
FCC [25,67,68]Fluid catalytic cracking catalyst (FCC) is a waste from the petroleum industry.It was used as a precursor wherein AA was a combination of SH and RHA [25,67,68] or quartz [68].[25,67,68][67]
GGBFS [17,23,27,28,29,33,35,41,42,45,46,48,49,51,52,53,54,55,56,59,69,70,71,72,73,74,75,76,77,78,79,80,81,82,83,84,85,86]Ground granulated blast furnace slag (GGBFS) is a by-product of the iron-making process. It was utilised to produce one-part AABs [23,28,77,85,86]. One of the studies explored sodium-carbonate-activated slag glass powder [82]. It was also used as a single source for precursor and as part of binary and ternary blended precursors with a variety of conventional and/or alternative feedstocks [17,27,28,29,33,35,41,42,45,46,49,51,52,53,54,55,56,59,67,69,70,72,73,75,76,78,81,83,84]. Additionally, mixed precursors containing different ratios of rice husk (RH), RHA, MK, palm oil fuel ash (POFA), and GGBFS were investigated [79]. Moreover, the ternary mix of WBP, WCeP, and WCP was examined together with integrating GGBFS in the precursor [48].[17,23,27,28,29,33,35,41,42,45,46,48,49,51,52,53,54,55,56,59,69,70,71,72,73,74,75,76,77,78,79,80,81,82,83,84,86][28,46,48,59,81,85][28,85]
K [73]Kaolin (K) is an aluminosilicate crystalline mineral that is transformed into MK when heat-treated. As a precursor, it was investigated while being activated by KH [87].[87]
LS [88]Ladle slag (LS) is derived from the steel-refining process via arc electric furnace technology.It was either used alone as a precursor or together with MK, where AA was mixed with SH and SS [88].[88]
MK [21,42,43,44,45,48,57,63,73,79,81,85,87,88,89,90,91,92,93,94,95,96,97,98,99,100,101,102]Metakaolin (MK) is a product of calcinating kaolin.It was used as a single precursor [21,42,63,81,85,87,89,90,91,93,94,95,100]. In the case of binary [21,43,44,45,57,73,88,92,95,96,97,98,99,101,102] and ternary [101,102] precursors, it was used together with a variety of conventional and/or alternative sources [21,43,44,45,57,73,88,92,95,96,97,98,99,101]. Mixed precursors containing different ratios of RH, RHA, MK, POFA, and GGBFS were also investigated [79]. Moreover, the ternary mix of WBP, WCeP, and WCP was examined together with integrating MK in the precursor [48].[21,42,43,44,45,48,57,63,73,79,81,87,88,89,90,91,92,93,94,95,96,97,98,99,100,101,102][81,85,101,102][85]
MWIA [31,40]Municipal waste incineration ash (MWIA) is waste obtained after the incineration of municipal waste.It was utilised as a single precursor [31] but also in ternary blended precursors, including RHA and FA [40].[31,40]
MWW [103]Mineral wool waste (MWW) is generated while manufacturing mineral wool (e.g., stone and glass wool) before adding organic resins or other additives. It was investigated as a precursor, which was activated by SS, SH, sodium aluminate, or sodium carbonate solutions [103]. [103]
NP [69,104,105,106,107,108]Natural pozzolan (NP) is a powder form of volcanic rock mainly containing amorphous silica and alumina.It was utilised as a single precursor [104,105,106,107] but also as in binary blended precursor with GGBFS [69] and MK [108]. [69,104,105,106,107,108]
OBA [109,110] Olive biomass ash (OBA) results from the combustion of olive stone [109] or olive oil industrial waste, e.g., pruning debris, leaves, and second-press olive dregs [110]. It was used mixed with water as an activator in FA- [110] and GGBFS-based AABs [109,110]. [109,110]
ONS [59] Olivine nano-silica (ONS) is produced by dissolving olivine in acid at low temperatures. It was used as an AA with SH for GGBFS/FA-based AABs [59]. [59][59]
POFA [79,84,97]Palm oil fuel ash (POFA) is a palm oil production waste.In the case of binary blended precursor, it was used with MK [92] and GGBFS [84]. Mixed precursors containing different ratios of RH, RHA, MK, POFA, and GGBFS were also investigated using SH as an AA [79].[79,84,97]
PD [77]Phyllite dust (PD) is a powder waste generated while manufacturing roof tiles.It was utilised with SS, SF, and GGBFS to produce one-part GGBFS-based AABs [77].[77]
PS [76] Paper sludge (PS) is a waste product from the paper industry.It was utilised as the CaCO3 source in combination with SH to be used as AA with GGBFS as a precursor [76]. [76]
RH [79]Rice husk (RH) is agricultural waste generated through rice production. It was used as a part of mixed precursors containing different ratios of RHA, MK, POFA, and GGBFS [79].[79]
RHA [21,25,26,41,67,68,111,112,113,114,115][16,32,37,40,57,60,79,116,117]Rice husk ash (RHA) is generated through the combustion of rice husks. The activator was produced using a mix of SH and RHA [16,21,25,26,41,67,68,111,112,113,114,115]. When RHA was used as a precursor, it was a component of the binary and ternary systems with a variety of conventional and/or alternative feedstocks [32,37,40,57,60,116]. Additionally, mixed precursors containing different ratios of RH, RHA, MK, POFA, and GGBFS were evaluated [79]. On the other hand, a one-part geopolymer synthesized by mixing RHA and solid sodium aluminate with subsequently added water was studied [117]. [16,21,25,26,32,37,40,41,57,60,67,68,79,111,112,113,114,115,116,117] [60,67,114,118][60,114]
RM [28,29,119] [28,58,72,80,98,99,120,121,122,123,124]Red mud (RM) is an alkaline sludge resulting from the Bayer process, which is the production of alumina from bauxite. It was used as an ingredient of AA for GGBFS [28,29] and FA-based AABs [119]. Additionally, it was utilised in binary and ternary precursors with a variety of conventional and/or alternative feedstocks [28,58,72,80,98,99,120,122,123,124]. Moreover, a one-part geopolymer was investigated by calcinating RM with SH pellets [121,124]. [28,29,58,72,80,98,99,119,120,121,122,123,124] [28][28]
RMS [80]Refuse mudstone (RMS) is a by-product of blasting operations in open-cut mining that is usually located at the top of a coal seam.It was used as a part of a ternary precursor with RM and GGBFS while utilising SS as an AA [80].[80]
RPP [35]Rock phosphate powder (RPP) is a pulverised form of naturally sourced rock phosphates. A ternary precursor concerning the addition of GGBFS and FA activated by SH was studied [35].[35]
SA [115,125] [78]Sugarcane ash (SA) is a residue from sugar production.It was part of AA with SH for FA- [115] or GGBFS- [125] based AABs. As a precursor, it was blended with GGBFS [78].[78,115,125]
SF [28,76,126] [77,98,124]Silica fume (SF) is a by-product of smelting for the manufacture of silicon and ferrosilicon alloys. A combination of SF and SH was used as an activator for GGBFS-based AAB [28,76,126]. It was mixed with MK [97] or RM [123] as a precursor. It was also utilised as an ingredient of one-part GGBFS-based AABs [77].[28,76,77,98,124,126] [28][28]
SiMnF [72,127]Silicomanganese fume (SiMnF) is an industrial by-product resulting from the production of silicomanganese alloy via carbothermic reduction. It was used as a precursor activated by a mixture of SH and SS [127]. Additionally, it was utilised as a part of the binary blended precursor with GGBFS [72].[72,127]
SW [128] Soda waste (SW) is a by-product of sodium carbonate production that is formed through the Solvay process.It was used for the alkali activation of GGBFS [128].[128]
WBA [129] Wood biomass ash (WBA) results from the combustion of wood biomass. It was utilised with class F pulverised fuel ash as a precursor [129]. [129]
WBP [27,46,47,48,81,96,102,127,130,131,132,133]Waste brick powder (WBP) is generated from brick construction and demolition waste.It was used as a single precursor [81,102,127,130,131,132,133] or as part of binary blended precursor with a variety of conventional and/or alternative feedstocks [27,47,96]. As a part of the ternary precursor, it was mixed with FA and GGBFS [46] as well as waste glass powder (WGP) and MK [102]. Additionally, a ternary mix of WBP, WCeP, and WCP was examined together with FA in the precursor [48]. [27,46,47,48,81,96,102,127,130,131,132,133][46,47,48,102,127,130]
WCP [48,134]Waste concrete powder (WCP) is a by-product of concrete construction and demolition waste.It was used as a single precursor [134] and a part of a ternary mix with WBP and WCeP integrating FA in the precursor [48]. [48,134][48]
WCeP [28,48,81,101,135]Waste ceramic powder (WCeP) is produced from ceramic tiles discarded as construction and demolition waste.It was utilised as a single source for precursor [81,101] and as part of binary [28,135] and ternary blended precursors [101]. A ternary mix with WBP and WCP was examined together with integrating FA in the precursor [48]. [28,48,81,101,135] [28,48,101]
WGP [101,131,136,137,138][49,50,52,82,83,92,101,102,122]Waste glass powder (WGP) is generated from glass, an abundant waste product since a large portion is not recycled, e.g., due to its grain size. As an activator, it has been synthesised with SH [101,102,131,136,137,138]. As a precursor, it was employed alone or [50] as a partial replacement of MK [92,101,102] and GGBFS [83]. Furthermore, it was evaluated as a part of a ternary precursor [49,52,101,102,122]. One of the studies also explored sodium-carbonate-activated slag glass powder [82]. [49,50,52,82,83,92,101,102,122,131,136,137,138][101,102][138]

5. Conclusions

The investigation of alternative materials’ technical performance and economic and environmental benefits has been acknowledged as a crucial factor for the broader use of such materials in the building industry. However, there is still a lack of studies covering these three pillars while developing novel material solutions. Since alkali-activated binders (AABs) have been identified as a sustainable alternative in the cement industry for decades, this study aimed to validate such claims and identify the main obstacles to their broader application. The findings of this state-of-the-art review can benefit enthusiasts working on the development of AABs by identifying key concerns for the application of their products on a large scale. The adoption of green materials could be more efficiently accelerated if laboratory-scale projects were based on a robust approach.
Based on this literature review, the following conclusions could be drawn:
  • The chemical compositions of the precursor and alkali activator used highly affect the material properties of AABs. There is still a lack of studies covering a wide range of sources for alternative precursors and alkali activators, which has led to the limited application of such AABs.
  • Concentrating investigations on locally available raw materials seems to be one of the most feasible solutions for adopting AABs on a larger scale in the industry. Future studies should focus on developing tools to identify the main factors influencing the variability of AABs’ material properties based on raw materials (e.g., machine learning).
  • The interconnectivity between the most influential factors regarding AABs’ environmental and economic performance (i.e., the regional context, transportation, energy sources, raw materials, alkali activators, precursors, and the curing method employed) demonstrates the importance of the consistent definition of both functional units and system boundaries. Evaluating only part of the critical factors can lead to results that would not realistically represent the situation when the product is applied in the industry.
  • The environmental benefits of utilizing feedstocks from construction and demolition waste could substantially improve sustainable pathways in the construction industry by focusing on circularity. Hence, alkali-activated materials employing these raw materials should be the focus of future research.
  • Studies on the economic performance of AABs are the rarest of the three pillars considered herein. Expensive feedstocks constitute a critical challenge for the economic performance of AABs, which is usually connected with high transportation costs. It has been demonstrated that by using a thorough approach, the cost of AABs can be decreased without compromising the other two pillars (i.e., technical and environmental performance).
  • Future research may benefit from using the multi-criteria analysis of alkali-activated materials to assist the development of comprehensive methodologies. Overall, optimisation should be reached by considering the most challenging factors in producing alkali-activated materials, thereby achieving favourable trade-offs between technical, environmental, and economic performance.

Author Contributions

Conceptualization, A.D. and K.K.; investigation, A.D.; writing—original draft preparation, A.D.; writing—review and editing, K.K., O.F. and I.M.; supervision, K.K., O.F. and I.M.; funding acquisition, I.M. and K.K. All authors have read and agreed to the published version of the manuscript.

Funding

Open Access funding by the TU Wien.

Institutional Review Board Statement

Not applicable.

Data Availability Statement

Not applicable.

Acknowledgments

The Stipendium Hungaricum Scholarship Programme is gratefully acknowledged for supporting the PhD study of the first author. The authors acknowledge the mobility support of the Stiftung Aktion Österreich-Ungarn in the framework of the bilateral research cooperation project No. 108öu3 between the TU Wien and the Budapest University of Technology and Economics. Additionally, the authors acknowledge the TU Wien Bibliothek for financial support through its Open Access Funding Program.

Conflicts of Interest

The authors declare no conflict of interest.

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