Preparation of Zeolite X (Base paper)

The silica precursor solutions were prepared using different silica sources: sodium
metasilicate anhydrous (Alfa Aesar) and sodium metasilicate pentahydrate (Alfa Aesar). The
sodium aluminate precursor solutions were prepared by dissolving sodium aluminate powder
(technical, EM Science) in aqueous solutions of sodium hydroxide (Fisher Scientific) or
potassium hydroxide (85%, Acros Organics). Both silica and aluminate precursor solutions
were filtered through 0.45 μm membrane filter (Pall Corporation). In some cases
triethanolamine (TEA Z99%, Sigma) was added to aluminate solution. The silica solutions
and TEA-containing sodium aluminate solutions were left at room temperature for a day
before mixing the aluminate solutions with the silica solutions in polyethylene (HDPE)
bottles. The bottles were then sealed, hand-shaken for a minute, and placed in an oven at 95
°C. After the crystallization was complete, as judged by microscopic examination, the
products were repeatedly washed with reversed osmosis water, filtered and dried for 24 h at
60-70°C.

Synthesis of Zeolite X from fly ash (By our method)

Pre -treatment of fly ash. 
Obtained fly ash is sieved to remove any bigger particles (mesh 60-120). It is mixed with
magnetic roller for 2 h to remove any magnetic particles and then washed with distilled water
4 times to remove any dissolved materials and acetone to remove any organic materials.
Then, calcined the sample at 800°C to remove any carbon particles in an air furnance. To this
add sodium hydroxide 1:1 and make a slurry in a PP tub heat will be generated. Add the
content to an alumina crucible and calcined it at 600°C. Dull white mass is grounded and
dissolved in distilled water so as to allow it to settle the solution for 24 h. The settling white
mass is discarded and filtered through the whatmann filter paper (grade 3). This is the mother
solution which will be used further.
XRF composition analysis of fly ash,
SiO2: Al2O3: Na2O: CaO: Fe2O3:K2O: MnO2: P2O5: TiO2: SrO: BaO: MgO
62.35:18.19: 0.37: 7.93: 5.89: 2.0: 0.06: 6.32: 1.85: 0.22: 0.12: 0.72
Based on SiO2: Al2O3 ratio, SiO2/Al2O3, from which Si/Al ratio will get 1.7 which is so close
to zeolite X synthesis composition of 1.7.

For 1 gm of fly ash purified, 62.35% is silica and 18.19% aluminum twice which is good for
synthesis. To the final treated mother solution from fly ash, 1.4 g of aluminium iso propoxide
and 0.4 g of silica gel was added to sodium hydroxide (0.6 g) and stirred to complete
dissolution. The final contents were added to the stirred and autoclaved.

Likewise for 30 gm of fly ash purified, 42g of of aluminium iso-propoxide and 12 g of silica
gel was added to sodium hydroxide (18 g) and stirred to complete dissolution. The final
contents were added to the stirred and autoclaved.
Based on SiO2: Al2O3 ratio, sodium aluminate and sodium metasilicate were added as the
alumina and silica source. Sodium hydroxide was used as extent pH regulator for the
crystallization solution. The conditions considered for the synthesis of zeolite x considered in
the above steps are continued for fly ash source.
The zeolite x was synthesized by using following gel composition,
l4.76 Na2O: 1 Al2O3: 3.5 SiO2: 454 H2O
For pure synthesis of zeolite-X, calculated content of aluminium iso-propoxide, was added to
NaOH (2.396 g) in 10 mL of deionized water and were added in polypropylene (PP) bottle
and stirred well at 40°C (Solution-A). Silica gel (3 g) in NaOH (2.386 g) was added to 9 mL
of deionised water and stirred well at 40°C (Solution-B). After complete dissolution of both
solutions, the solution-B was added to solution-A in vigorous stirring. Finally, 30 mL
deionized water was added at the final stage resulting in the formation of white milky
solution. The resulting milky solution in PP bottle was autoclaved for 24 hours at 90°C in a
vacuum oven. After cooling, the mixture was washed with double distilled water until neutral
solution of filtrate is obtained. Then, finally white mass is calculated at 550°C for 2 hours to
yield sodium form of Zeolite X (Na-X).

Synthesis of Zeolite X for anticancer activity

Zeolite X from coal fly ash was synthesised by following the method described by Tekin
et al., 2015. The batch composition for the synthesis is given by l4.76 Na2O: 1 Al2O3: 3.5
SiO2: 454 H2O. Based on SiO2: Al2O3 ratio in coal fly ash, sodium aluminate and sodium
metasilicate were added as the alumina and silica source. Sodium hydroxide was used as
extent pH regulator for the crystallization solution. After the crystallization was complete, as
judged by microscopic examination, the products were repeatedly washed with reversed
osmosis water, filtered and dried for 24 h at 90°C.