## Materials and Methods
### Chemical and Mineralogical Characterization of the Materials  
Chemical composition of the CEM I, natural pozzolan, P, siliceous coal fly ash, V, silica fume, D, and ground granulated blast-furnace slag, S, is shown in Table 2; whereas the chemical compositions for the three tested aggregates are given in Table 3. The chemical analyses were performed by XRF with a S8 Tigger 4 kW model instrument (Bruker, Billerica, Massachusetts, USA). Loss on ignition (LOI) and chloride ion contents were determined according to the European standard EN 196-2 [34].  
The effect of equivalent sodium oxide ratio, Na\({}_{2}\)O\({}_{\text{eq}}\), of Portland cement and additions on ASR properties should be considered. The highest Na\({}_{2}\)O\({}_{\text{eq}}\) ratio was found in the coal fly ash (4.56%) followed by the silica fume (3.22%) as shown in Table 2. The role of Na\({}_{2}\)O\({}_{\text{eq}}\) ratio on the mechanical strength development and flowability of cement-based materials is well-known, but also it has a deleterious effect regarding the ASR. In addition, [PERSON] et al. [35] discussed the contribution of the alkali release from aggregates to ASR. The reactive aggregate presented the largest content of alkalis (Na\({}_{2}\)O\({}_{\text{eq}}\) = 5.89%) followed by the non-reactive one (Na\({}_{2}\)O\({}_{\text{eq}}\) = 3.51%).  
\begin{table}
\begin{tabular}{c c c c c c} \hline
**Parameter** & **CEM I 42.5 N** & **V** & **S** & **D** & **P** \\ \hline Al\({}_{2}\)O\({}_{3}\) & 3.65 & 23.16 & 12.16 & - & 13.15 \\ CaO & 64.49 & 5.75 & 41.55 & 0.60 & 12.98 \\ Cl\({}^{-}\) & 0.03 & - & - & 0.06 & - \\ Cr\({}_{2}\)O\({}_{3}\) & 0.02 & 0.17 & - & - & - \\ Fe\({}_{2}\)O\({}_{3}\) & 3.96 & 5.93 & 0.39 & 0.14 & 12.75 \\ K\({}_{2}\)O & 0.64 & 0.96 & 0.48 & 3.03 & 0.56 \\ MgO & 1.27 & 1.96 & 6.96 & 0.33 & 9.62 \\ Mn\({}_{2}\)O\({}_{3}\) & 0.05 & 13.35 & 48.97 & 40.06 & - \\ Na\({}_{2}\)O & 0.12 & 3.93 & 0.17 & 1.23 & 0.63 \\ P\({}_{2}\)O\({}_{5}\) & 0.18 & 0.67 & - & - & 1.26 \\ SiO\({}_{2}\) & 20.80 & 52.17 & 35.13 & 91.31 & 42.82 \\ SO\({}_{3}\) & 2.33 & 0.36 & 1.86 & - & 0.00 \\ STO & 0.06 & 0.10 & 0.05 & - & 0.12 \\ TiO\({}_{2}\) & 0.19 & 0.92 & 0.56 & - & 3.62 \\ ZnO & 0.01 & 0.02 & - & - & 0.02 \\ ZrO\({}_{2}\) & - & 0.03 & 0.02 & - & 0.05 \\ LOI \({}^{1}\) & 2.21 & 3.80 & 0.45 & 3.29 & 2.21 \\ Na\({}_{2}\)O\({}_{\text{eq}}\)\({}^{1}\) & 0.54 & 4.56 & 0.49 & 3.22 & 0.99 \\ \hline \end{tabular}  
* \({}^{1}\) LOI: Loss on ignition; Na\({}_{2}\)O\({}_{\text{eq}}\) = Na\({}_{2}\)O + 0.658 K\({}_{2}\)O.  
\end{table}
Table 2: Chemical composition of the CEM I, natural pozzolan, P, siliceous coal fly ash, V, silica fume, D, and ground granulated blast-furnace slag, S.  
Figure 1: Siliceous aggregates employed in the present research work: (**a**) ASJ_12 (siliceous pebbles, 4–6 mm); (**b**) VB_1 (siliceous gravel, 6–12 mm); (**c**) ASJ_2 (siliceous sand, 0–2 mm).  
Mineralogical characterization was performed by X-ray diffraction (XRD). Thus, the crystalline compounds present in the aggregates were determined by XRD. Diffraction data of the aggregates were recorded using a D8 Advance powder crystal X-ray diffractometer (Bruker) with 2.2 kW Cu anode ceramic X-ray tube. Crystalline compounds were identified with the DIFFRAC.EVA v4.2.1 software which supports a reference pattern database derived from the Crystallography Open Database (COD) for phase identification. The analyses were carried out on a representative sample of each aggregate. The test sample was ground and sieved on a sieve, either by hand or by mechanical means. Then, a grain size lower than 80 \(\upmu\)m was achieved. The identification, chemical composition and aggregate type of each aggregate are shown in Table 3.