2.2. Scale Up Pillarizations
The experiments were divided into three series. In series 1, the effect of water during the expansion of clay was studied. In series 2, the method of pillaring was studied, and in series 3, the amount of pillared clay was increased.

2.2.1. Series 1: Effect of Water
To evaluate the effect of water utilized to expand the clay, several methods were tested (Table 1). The OH/Al = 2 ratio and 15 mEq Al/g of clay were maintained in all experiments.
Methods 1, 2, and 3 were performed according to the traditional procedure, only modifying the amount of water present in the clay suspension. However, methods 4 and 5 were performed in a distinct form, with the exception of the synthesis of the pillaring solution. In method 4, after preparation of the clay suspension (10 g of clay with 1 L of distilled water), 500 mL of water was removed by centrifugation (5000 rpm for 10 min). Later, the remaining suspension was added to the pillaring solution, and the mixture was stirred for 2 h. The clay was vacuum-filtered, washed with distilled water, dried in an oven at 60 °C, and calcined at 450 °C for 3 h, as previously described.
Method 5 was performed similarly to method 4, but after the stage of hydration of the interlayer cations, 900 mL of water was removed from the clay suspension by centrifugation. The remaining 100 mL of clay suspension was added to the pillaring agent performing the pillaring stage similarly to the other experiments. This procedure (removal of water suspension) was performed to verify the influence of the amount of water utilized in the clay suspension.
All methods from this series have been performed more than once in order to check their reproducibility.

2.2.2. Series 2: Method Effect
In this series of experiments, several pillaring methods were tested (Table 2). In method 6, 150 mL of a NaOH solution and 75 mL of a AlCl3·6H2O solution, both 0.6 mol/L, were utilized to prepare the pillaring solution. The NaOH solution was dripped slowly (1 mL/min) into the Al solution under constant stirring at ambient temperature and maintained under these conditions for 6 days. Subsequently, the pillaring agent was transferred to a round bottom flask containing 3 g of dry clay and kept under reflux for 24 h at 80 °C. Then, the material was vacuum-filtered, washed with distilled water, dried in an oven at 60 °C, and calcined at 450 °C as previously described in Section 2.1.
Experiment 7 proceeded as described in the traditional method. However, after 6 days of aging, the pillaring solution was stored for a month in an amber vial to check whether the properties of the pillaring solution remained over the course of time. The pillarization procedure was performed as described in the traditional method.
An in situ pillarization, tested in method 8, was performed differently from all other methods. Ten grams of clay was added to 250 mL of an AlCl3·6H2O solution (0.6 mol/L) and stirred for 2 h. Subsequently, 500 mL of a NaOH solution (0.6 mol/L) was dripped slowly (1 mL/min) into the Al solution and stirred for 6 days at ambient temperature. After the aging time, the material was washed, filtered, dried, and calcined as previously described in Section 2.1.
Experiment 9 was performed as described previously. However, the clay was first expanded with water (3 g in 300 mL) for 2 h at ambient temperature. After the solution of aluminum chloride (250 mL of 0.44 mol/L) was added to the clay suspension, the mixture was stirred for 2 h. This solution had to be more concentrated to maintain the final concentration at 0.2 mol/L after the solution had been added to the clay suspension. The following procedures were performed as described in the previous method.
Pillaring method 10 was performed as described by Leite et al. [32]. To prepare the pillaring agent, 500 mL of a NaOH solution and 250 mL of an AlCl3·6H2O solution, both 0.2 mol/L, were utilized. However, during the dripping (1 mL/min), the solution was kept at 60 °C with stirring. Then, the solution was stirred at ambient temperature for 24 h. Subsequently, 3 g of clay was dispersed in 150 mL of water for 48 h of stirring at ambient temperature. Then, the pillaring agent was added to the clay suspension and stirred for 48 h more. Finally, the clay was filtered, washed, dried, and calcined as previously described in Section 2.1.
Method 11 was performed in the same manner as method 10. However, the stirring time was reduced from 48 to 2 h. The same procedure was performed with the cation exchange stage: the pillaring solution and the clay suspension were kept in contact for just 2 h. The pillaring agent synthesis was performed as described in method 10, without modifications.
The majority of methods from this series have been performed just once.

2.2.3. Series 3: Increase in the Amount of Pillared Clay
In this series of experiments, the amount of pillared clay was increased. Table 3 presents the modified parameters for each experiment. In all methods, 1 g of clay to 100 mL of water was utilized.
Pillaring methods 3, 12, 14 and 15 were performed in the traditional manner: the pillaring agent was stirred for 6 days at ambient temperature. The difference between the methods is the concentration of the solution to maintain the relation of 15 mEq Al/g of clay.
In method 14, solutions of 1.5 mol/L were utilized. Due to this high concentration, the pillaring solution became turbid, requiring stirring for 13 days, but even after this period, the pillaring solution still presented some turbidity.
In methods 11, 13 and 16, the pillaring solution was kept at 60 °C during the dripping (1 mL/min) of the sodium hydroxide solution into the aluminum chloride solution. Then, the pillaring agent was stirred at ambient temperature for 24 h. The following procedures were performed as described above.
All methods from this series have been performed more than once in order to check their reproducibility.

2.2.4. Characterization
The prepared materials were characterized by X-ray diffraction (XRD) on a Shimadzu-XRD-7000 apparatus (Shimadzu, Kyoto, Japan) using Cu radiation (λ = 1.54 Å) and 0.02° step size. N2 physisorption isotherms were measured using a Quantachrome-NOVA 2200e apparatus (Quantachrome, Boynton Beach, FL, USA). Prior to analysis, the samples were degassed for 3 h at 300 °C under vacuum. The surface areas were obtained using the Brunauer, Emmet and Teller (BET) method, and the micropore volumes and external areas were calculated by the t-plot method using the Harkins-Jura-de Boer t-equation [33]. The total pore volume was calculated at a partial pressure p/p0 of 0.95. The micropore area was calculated as the difference between the BET and external surface areas.