Recent Advances in Geopolymer Technology. A Potential Eco-Friendly Solution in the Construction Materials Industry: A Review
Abstract
:1. Introduction
2. Geopolymer Cements (GCs): Chemistry, Raw Materials, and Products
- (1)
- Alkali activation. An alkaline activator is necessary for the dissolution of Si and Al from the inorganic precursor as well as for the catalysis of the condensation reaction. The reaction of alumino-silicate oxides (Si2O5, Al2O2) in strongly alkaline solution results in a breakdown of Si-O-Si bonds with the subsequent penetration of Al atoms in the original Si-O-Si structure. The resulting alumino-silicate oxide gels, based on Si-O-Al block, are the geopolymer precursor of the polycondensation reaction. The dissolution/hydrolysis reaction is reported in Figure 2.
- (2)
- Polycondensation in Geopolymer network. The alumino-silicate gel phase is a highly reactive product. Under alkaline condition, substantially fast chemical reactions occur, forming a rigid 3D polymeric and ring framework of Si-O-Al bonds (Figure 3). The proper completion of the geopolymerization process and the conferment of adequate mechanical strength properties to the material require heat curing treatment at a thermal range between 25 and 90 °C [11]. The water released by polycondensation is normally consumed during the dissolution process.
2.1. Metakaolin-Based Geopolymer Cements (MGCs)
2.2. Fly Ash-Based Geopolymer Cements (FGCs)
2.3. Natural Minerals-Based Geopolymer Cements (NCs)
2.4. Hybrid Geopolymer Cements (HGCs)
3. Recent Research Findings of Geopolymer-Based Concrete Properties
3.1. Rheological Properties
3.2. Microstructural Properties
- Particle size distribution of alumino-silicate precursors. Assi et al. [40] investigated the influence of three different FA particle grades (38.8, 17.9, and 4.78 μm) on the microstructural properties of geopolymer concrete. The finer the average FA particle size distribution, the denser and stronger the geopolymer matrix. In this regard, the increase in surface area is crucial in terms of high reactivity to alkaline dissolution, the preferential formation of geopolymer products, the high ability to fill structural micro-voids, and less free water that evaporates during the curing, causing a decrease in the formation of microcracks.
- Type of mineral precursor and Si/Al ratio. Cherki El Idrissi et al. [41] proved how the Si/Al ratio, brought by several mineral precursors, is intimately linked with the porosity distribution in GCs. In this research, three different precursors were analyzed: MK (Si/Al ratio: 2.5), GBFS (Si/Al ratio: 3.5), and FA (Si/Al ratio: 5.9). Experimental pore volume distribution, conducted by mercury intrusion porosimetry (MIP), revealed that the pore distribution of geopolymer medium shifted into smaller voids as the Si/Al ratio increases. This result is consistent with the work of Wan et al. [42]. Geopolymer compounds synthesized at a low Si/Al ratio (Si/Al ratio of 1:1) present a high content of undispersed crystalline zeolitic nuclei into a little geopolymeric binder and macropores. At a Si/Al ratio of 2:1, a proper concentration of aluminate and silicate monomers is involved in a homogeneous geopolymer binder. At a Si/Al ratio of 4:1, many micropores or mesopores are formed due to an insufficient amount of dissolved aluminosilicate monomers. SEM micrographs of GCs synthesized at various Si/Al ratios are reported in Figure 10.
- Molarity of alkali-activator. Huseien et al. [43] researched the influence of NaOH molarity (from 2 to 16M) on the water absorption tendency of GBFS-FA-based geopolymer mortars. High NaOH molarity improves the microstructure of samples in terms of density increasing and air voids reduction. The increased concentration of alkali-activator enhances the geopolymerization mechanism in terms of precursors solubility, resulting in a high compactness of the network structure and good interfacial adhesion between the geopolymer paste and mineral aggregates. However, very high alkaline solutions (generally > 16 M) can be deleterious on the microstructural and mechanical properties of geopolymer concrete. Higher NaOH concentrations hinder the polycondensation process due to the accelerated dissolution of the alumino-silicate raw materials. The excess of hydroxyls anion (OH−) in the alkali-activated matrix results in premature precipitation of geopolymeric gels, deteriorating the mechanical properties of the geopolymer produced.
- Curing time and temperature. Recent findings of the effect of curing treatment on the pore system of FGC-based materials are reported in the research of Zhang et al. [44]. The authors investigated the relationship of microstructural properties development of FGCs and its dependence on curing conditions (room temperature, 50 °C and 80 °C for 7, 28, and 49 days). For each curing temperature, the porosity rate of the samples decreased with the heat curing period. Macro-pores (50–100 μm) constituted the geopolymer matrix under 7 days curing time. As the heat treatment increased, the percentage of large pores tended to decrease, but a more significant contribution of microcracks due to the material’s drying occurred. In this regard, the greater the temporal extension of the thermal treatment, the higher the geopolymer reaction degree, increasing the inorganic gel formation that constructed a more compact microstructure [39]. Curing temperature is crucial to the overall pore volume. Similar pore content was observed at room and middle curing temperatures (about 5% and 4.5%, respectively, while a higher pore fraction (about 8%) was detected in the samples cured at 80 °C. Faster water evaporation and hardening process at higher curing temperature results in a less ordered medium of poorer quality having larger pores and defects. On the other hand, lower curing temperatures help the material densification, as the geopolymer gel tends to saturate the microstructural voids [45].
Effects of Mineral Aggregates: Interfacial Transition Zone (ITZ) Porosity
3.3. Mechanical Properties
Mechanical Strength Properties Optimization of GC-Based Concrete: Recent Developments
3.4. Durability Properties
3.5. Thermal and Acoustic Properties
4. Recent Applications and Upgrading of Geopolymer Technology in Construction Sector
4.1. GC-Based Mixes for 3D Printing Fabrication Technologies
4.1.1. Muthukrishnan et al. Research
4.1.2. Chougan et al. Research
4.1.3. Li et al. Research
4.1.4. Voney et al. Research
4.1.5. Xia et al. Research
4.2. Adopting Geopolymer Technology: Companies and Applications
4.3. InnoWEE Project
- ETICs-like panels. ETICs-like panels (Figure 19a) consist of sandwich panels (400 mm × 900 mm) composed of an outer high-density geopolymer layer (8 mm thin) and 70 mm-thick expanded polystyrene (EPS) insulating core. The geopolymeric binder is an FA-MK blend implemented with 50 wt % of inorganic aggregates consisting in a mixture of fired clay and concrete waste. A preliminary thermal insulation performance analysis was performed by installing these panels in some residential and urban buildings located in various European countries, such as “Don Orione” residential assistance center (Bucharest, Romania), Volua municipal building (Athens, Greece), and pilot eco-buildings (Padova, Italy). In terms of energy efficiency, the results demonstrated an annual energy saving of over 400 kW/h per year, meeting the new building efficiency requirements imposed by the EU.
- Ventilated façade cladding panels. Innovative lightweight façade panels (Figure 19b), with dimensions of 595 mm × 595 mm, were developed by bonding an outer high-density geopolymer (such as the ETICs-like one) layer to an inner wood–geopolymer panel (incorporating 40 wt % of crushed wood. The element combines the specific behavior of its components. The geopolymer layer acts as a barrier to protect the structure from adverse weather phenomena (wind load, rain, and ice). The wood–geopolymer panel provides additional strength and lightweight. As for ETICs, insulating and durability studies were performed both in the laboratory and on site by the installation of prefabricated cladding panels in European pilot buildings.
5. Discussion and Conclusions
- Reactivity, SiO2 and Al2O3 monomers concentration, and the morphological finesse of the precursors are crucial for the compaction and microstructural features of a geopolymer matrix. A finer size gradation and a high (but balanced) Si/Al ratio are favorable conditions to ensure the formation of a less porous and dense geopolymer gel, promoting the mechanical strength properties.
- Activating solution molarity should be properly balanced to obtain an efficient dissolution of the alumino-silicate precursors and proper rheology of the fresh paste in terms of setting time and slump. The addition of superplasticizers reduces the water requirement, preserving optimal mechanical properties.
- Curing at room temperature or thermal-induced provides similar performance in terms of long-term mechanical strength. High curing temperatures promote the geopolymerization process but, on the other hand, they can negatively affect the microstructure and strength of the material due to the micro-crack generation deriving from accelerated water evaporation.
- The Si-content and the specific surface of the natural inert incorporated in the geopolymer compounds affect the microstructure and mechanical properties. The very Si-rich and finer mineral aggregates promote a more compact and cohesive ITZ.
- The incorporation of reinforcement fibers and micro and nano-fillers is a novel and viable approach to improve the mechanical strength and stiffness of geopolymer concrete and mortars.
- Some current investigations on the durability performance of geopolymeric compounds revealed better characteristics than PC-based materials in terms of water sorptivity, permeability, long-term resistance to corrosion, and fireproofing.
- GFCs are an emerging class of geopolymer formulations with improved thermal insulation and sound absorption properties, resulting in attractive technologies to optimize the energy-efficiency for building application. However, the sound insulation performances of geopolymers concrete are poorly covered in the literature, and therefore, more investigations need to be conducted in this field.
- The high sensitivity of the geopolymerization process to environmental factors and synthesis parameters requires skilled and highly trained labor to obtain materials of suitable quality. The instability in the chemical composition of precursors can be another severely limiting factor.
- High costs and toxicity of activating alkaline solutions. In this regard, the study of more eco-friendly and cheap activators could be a possible way of research to optimize the geopolymer technology.
- Long-term availability of raw materials. The stringent environmental regulations adopted in many industrialized countries on the use of renewable resources as primary energy supplies have led to a slight decline in many power plants, from which geopolymeric raw materials are extracted (for example, coal-fired power stations for FA supply). If this trend continues, it may further affect the diffusion of GC as a replacement of ordinary PC. However, in accordance with current production rates, availability, and costs, possible replacements of PC concrete with geopolymer aggregates of at least 75% are feasible [100].
Author Contributions
Funding
Acknowledgments
Conflicts of Interest
References
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Oxides (%) | Yangzi Power Plant (China) [18] | Secunda Power Plant (South Africa) [19] | Mae Mao Power Plant (Thailand) [22] |
---|---|---|---|
SiO2 | 55.86 | 46.28 | 39.82 |
Al2O3 | 31.74 | 21.27 | 21.52 |
Fe2O3 | 3.28 | 4.29 | 13.68 |
CaO | 1.67 | 9.82 | 15.24 |
MgO | 0.39 | 2.62 | 2.78 |
other | 7.06 | 15.72 | 6.96 |
Formulation | FA(%) | GBFS (%) | Micro-FA (%) | d (μm) | Dry Packing Density (0–1) |
---|---|---|---|---|---|
M 1 | 5 | 25 | 10 | 33.1 | 0.483 |
M 2 | 10 | 20 | 10 | 37.7 | 0.505 |
M 3 | 15 | 15 | 10 | 42.8 | 0.517 |
M 4 | 15 | 20 | 5 | 43.5 | 0.515 |
M 5 | 20 | 15 | 5 | 48.6 | 0.528 |
Type | Variable | Investigated Range | Compressive Strength (MPa) | Flexural Strength (MPa) | Density (g/cm3) | Primary Findings |
---|---|---|---|---|---|---|
FA-based lightweight mortar [25] | Activator molarity | 10–14 M | 19–30 | 3–4 | 1.88–1.92 | 14 M optimal |
FA-GBFS-based concrete [36] | Precursors size distribution | 33.1–48.6 μm | 48–67 | / | / | Finest size gradation optimal |
FA-GBFS-based mortar [50] | Heat curing | Ambient–100 °C | 40–53 | / | 1.88–1.96 | Ambient (28 days) and 90 °C (1 h) curing similar improvement effect |
FA-GBFS-based concrete [51] | FA-GBFS replacement | 0–30% by weight of GBFS | 26–52 | 3.5–5 | 2.38–2.43 | 30% GBFS replacement optimal |
FA-based mortar [52] | Mineral aggregates grading (limestone sand) | 0–4 mm; 2–4 mm; 1–2 mm; 0–1 mm | 42–49 | 6.7 -6.9 | 2.03–2.07 | 2–4 mm gradation optimal |
Method | Process Parameter | Mix Composition | Primary Findings |
---|---|---|---|
EP | 3-axis extruder, 25 mm × 15 mm rectangular nozzle, 12 mm/s printing speed, 15 mm nozzle height | FA-GBFS geopolymer mix, coarse, and fine silica sand, PVA fibers, Na2SiO3 activating solution, no chemical admixtures | Use of microwave heating as a rapid and efficient mode to increase the filaments bond strength and improve the buildability of 3D printed elements |
Method | Process Parameter | Mix Composition | Primary Findings |
---|---|---|---|
EP | Gantry-type extruder, 20 mm circular nozzle, 20 mm/s printing speed, 10 mm nozzle height | FA-GBFS geopolymer mix, fine river sand, silica fume, KOH-Na2SiO3 activating solution, no chemical admixtures | Addition of nano additive reinforcements (attapulgite nano-clay) and PVA fibers to increase the printability and mechanical strength properties |
Method | Process Parameter | Mix Composition | Primary Findings |
---|---|---|---|
EP | 3-axis extruder, 12 mm circular nozzle, 10 mm/s printing speed, 50 mm nozzle height | FA-GBFS geopolymer mix, fine river sand, silica fume, penta-Na2SiO3, no chemical admixtures | Implementation of printing device with an automated micro-cable reinforcing method to incorporate steel fibers into the printed filaments for mechanical bearing capacity optimization |
Method | Process Parameter | Mix Composition | Primary Findings |
---|---|---|---|
PP | Powder-based system, 0.2 mm circular nozzle, 0.8 mm line spacing, 2.5 mm layer height, 0.5–1 μL/mm injection volume | MK reactive powder, silica sand, ground quarry waste, K2SiO3 activating solution | The replacement of natural aggregates with ground quarry waste preserves the print quality and the structural properties of the printed elements, resulting in a more eco-sustainable approach |
Method | Process Parameter | Mix Composition | Primary Findings |
---|---|---|---|
PP | Powder-based system, 2.5 pL drop volume, 0.1 mm layer height, 2–4 layers/min printing speed | FA-GBFS powder blend, silica sand, anhydrous Na2SiO3 activating solution | The use of GBFS in the mix design (min. 50 wt %) is always necessary to ensure an adequate material setting at room temperature and higher mechanical properties. The exclusive use of FA does not allow to reach adequate green strength due to the low reactivity of the particles. The increase in FA amount increases the binder droplet penetration time. |
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Sambucci, M.; Sibai, A.; Valente, M. Recent Advances in Geopolymer Technology. A Potential Eco-Friendly Solution in the Construction Materials Industry: A Review. J. Compos. Sci. 2021, 5, 109. https://doi.org/10.3390/jcs5040109
Sambucci M, Sibai A, Valente M. Recent Advances in Geopolymer Technology. A Potential Eco-Friendly Solution in the Construction Materials Industry: A Review. Journal of Composites Science. 2021; 5(4):109. https://doi.org/10.3390/jcs5040109
Chicago/Turabian StyleSambucci, Matteo, Abbas Sibai, and Marco Valente. 2021. "Recent Advances in Geopolymer Technology. A Potential Eco-Friendly Solution in the Construction Materials Industry: A Review" Journal of Composites Science 5, no. 4: 109. https://doi.org/10.3390/jcs5040109
APA StyleSambucci, M., Sibai, A., & Valente, M. (2021). Recent Advances in Geopolymer Technology. A Potential Eco-Friendly Solution in the Construction Materials Industry: A Review. Journal of Composites Science, 5(4), 109. https://doi.org/10.3390/jcs5040109