In this paper, we comparitvley studied acetic acid attacks on geopolymer (GP-M), calcium aluminate (CAC-M), and Portland cement (PC-M)-based mortars. Consequent formations of deteriorated or transition layers surrounding the unaltered core material was classified in these three mortars, according to different degradation levels depending on what binder type was involved. Apart from mass loss, hardness, and deterioration depth, their microstructural alterations were analyzed using test methods such as scanning electron microscopy with energy dispersive spectroscopy (SEM-EDS), mercury intrusion porosimetry (MIP), powder X-ray diffraction (XRD), and thermogravimetric analysis-differential scanning calorimeter (TGA-DSC), which showed the different mechanisms for each binder type. Elemental maps revealed the decalcification (PC-M and CAC-M) and depolymerization (GP-M) that occurred across the mortar sections. The mass loss, hardness, and porosity were the least affected for GP-M, followed by CAC-M. These results points out that geopolymer-based mortars have improved acid resistance, which can be used as a potential alternative to conventional cement concretes that have been exposed to agro-industrial environments.
Geopolymers are inorganic binders based on mixtures of an aluminosilicate powder with an alkali-silicate solution. Properties of geopolymers are strongly determined by the type of reactive solid, the liquid/solid ratio of paste and, amongst others, the Si/Al ratio of the formed geopolymer network. In this study, fly ash blended metakaolin based geopolymers with varying liquid/solid ratios (l/s), activated by potassium silicate solution, are investigated. Reactivity of metakaolin and fly ash was investigated by powder X-ray diffraction (XRD) and dissolution tests. Reactivity, mechanical properties and microstructure of hardened pastes were analyzed by setting and compressive strength tests, mercury intrusion porosimetry (MIP), capillary water absorption tests, thermogravimetric analysis-differential scanning calorimeter (TGA-DSC), isothermal calorimetry and scanning electron microscopy with energy dispersive spectroscopy (SEM-EDS). The results show that substitution of metakaolin by fly ash as well as variation of l/s brings advantages up to a certain degree, but also has a considerable influence on the pore size distribution, mechanical properties, Si/Al ratio of the geopolymer network and the content of bound water.
Geopolymers are synthesized by mixing powdery solids, rich in amorphous silicon and aluminum species, with an alkaline solution, which leads to the formation of an inorganic alumosilicate network. Their acid resistance is affected by the composition, the porosity, and pore size distribution of the hardened binder as well as the type and concentration of the acidic solution. In the present study, two geopolymer mixtures with varying liquid-to-solid ratios and Si/Al ratios were exposed to a sulfuric acid solution (pH = 1) and analyzed after different durations of exposure (7, 14, 28, 56, and 70 days) by using a light microscope and scanning electron microscopy with energy-dispersive X-ray spectroscopy (SEM-EDX). SEM-EDX elemental mapping was used to evaluate the degradation from depth profiles of silicon (Si), aluminum (Al), and potassium (K) leaching. The results clearly show the leaching kinetics of potassium and the dealumination of the network. The separate consideration of specific reaction steps in the course of degradation, namely the depth of erosion (DE), the depth of deterioration (DD), and the depth of reaction for certain elements (DR(e)), indicate a combination of chemical and diffusion controlled degradation mechanisms.
Elemental leaching of metakaolin based geopolymers was investigated by immersing hardened paste specimens in a solution. For this, pure water and 0.1 molar acetic acid solutions were replenished ten times distributed over 56 days in total. Dissolution and diffusion of the elements through and from the geopolymer paste into the surrounding solutions was investigated on cross-sections of specimens by SEM-EDS microscopy, indentation, X-ray powder diffraction analysis and measuring the eluted elements by ICP-MS when replenishing the solution over time. The presented new methodological approach thus combines the dissolution rate kinetics obtained via wet chemistry (ICP) with the complementary solid state characterisation methods to gain new insights into the complex geopolymer dissolution mechanisms. Results indicated a relatively small leachability of geopolymers, limited only to the surface layer which is directly exposed to the aggressive solution, while the more inner parts of the geopolymer framework remain intact. Elemental maps revealed dissolution of aluminates that occurred across the outermost surface parts of the sections, while potassium leached out gradually but reached deeper inner parts. However, there was still a high portion of potassium being left bonded inside the geopolymer, even for the harsh acidic conditions, limited by the diffusion-reaction mechanism which took place within the geopolymer. The obtained experimental results represent a first approach towards feeding reactive transport numerical modeling approaches still to be developed for simulating leaching and degradation of geopolymer materials when exposed to water or acidic solutions.
Geopolymers are alternative binders made solely from industrial by-products and/or natural alumino-silicates, comprising no traditional cements. Reactive transport processes in geopolymer materials play a crucial role in both the degradation process of building materials as well as in the containment of hazardous wastes. A numerical model is presented for solving transport coupled to nonlinear ion-exchange equilibria between solid-liquid phases. Bound alkalies provide the geopolymer paste with a large reservoir of exchangeable (soluble) alkalies that allow for a more gradual drop in pH of the pore solution, as compared to a sudden drop when considering only diffusion transport mechanism. The model is robust enough to handle non-linearity of the ion-exchange equations, and presents a more reliable way to obtain long term durability predictions of geopolymer materials.
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