HAKIM, YUSUF MATHIINUL and Mohadi, Risfidian and Mardiyanto, Mardiyanto and Royani, Idha (2025) MODIFIKASI CLAY BENTONIT DAN DESAIN KOMPOSIT FOTOKATALIS SINAR TAMPAK SEBAGAI AGEN ADSORPSI DAN FOTODEGRADASI PADA PENGOLAHAN AIR LIMBAH. Doctoral thesis, Sriwijaya University.
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Abstract
The environmental issue of wastewater pollution containing dyes has reached a critical stage, especially in water bodies. The root of the problem partly comes from the textile and garment industry, which increases production every year but does not develop effective methods for treating wastewater containing dyes. Ironically, the dye content in wastewater is laden with hazardous compounds such as suspended solids, COD, dyes, and heavy metals that are potentially carcinogenic and mutagenic to living organisms. Currently, the long-term solution offered for this problem is the development of environmentally friendly materials based on natural substances and their application methods in wastewater treatment to achieve a broader spectrum of applications. Among the various methods of wastewater treatment, adsorption and photocatalysis have currently become trends that are widely researched and synergized into a single type of material, considering factors of economic value and ease of use. In this study, the development of natural clay-based bentonite materials has been carried out, modified into organobentonite and visible light photocatalyst composites to obtain dual functions of adsorption and photodegradation as wastewater treatment media. In its implementation, the first phase of the research involved the activation of natural Pacitan bentonite (B) using a simple intercalation method of a saturated Na+ cation solution to become Bentonit-Na (B-Na) to enhance cation exchange capacity, followed by a simple intercalation modification of a saturated NH+ cation solution to become Bentonit-NH (B-NH). Next, the material was tested for its adsorption capacity against cationic dye wastewater, namely rhodamine B (RhB), malachite green (MG), and methylene blue (MB). Next, the adsorption results are analyzed to study the increase in adsorption capacity and the process. The second phase of the research involved modifying B-Na into organobentonite (OB) to obtain hydrophobic properties and its application in the adsorption of anionic dye wastewater. The modification method was carried out by intercalating the cationic surfactant octadecylamine (ODA) using variations in the type and composition of solvents in the intercalation process, namely aquades, ethanol, and a mixture of aquades/ethanol (50%). Adsorption tests were conducted on wastewater containing the anionic dye direct yellow (DY) to analyze the increase in its adsorption capacity. The third phase of the research was conducted by modifying B-Na into exfoliated bentonite sheets (BE) using the solution-phase exfoliation method and composite design with visible-light semiconductor photocatalysts (g-C3N4 and Ag3PO4) through in-situ crystallization and co-precipitation methods by controlling the pH and temperature of the composite synthesis. The obtained results were tested on the photodegradation of RhB dye wastewater to study their dual function of adsorption and photocatalysis. The results obtained in the first phase of the research are data on the functional improvement of the adsorbent structure and the maximum adsorption capacity of the B-Na and B-NH materials towards cationic dyes overall. The improvement in the functional structure was observed from the change in surface area during BET characterization, with the initial value of B being 61.791 m²/g, which then increased to 73.089 m²/g for B-Na and 178.71 m²/g for B-NH. The comparison of the increase in adsorption capacity from B to B-Na for absorbing RhB is from 100 mg/g to 116.28 mg/g, for absorbing MG is from 109.89 mg/g to 123.46 mg/g, and for absorbing MB is from 136.99 mg/g to 158.73 mg/g. Meanwhile, the increase in maximum adsorption capacity from B to B-NH for absorbing RhB is from 100 mg/g to 526.37 mg/g, for absorbing MG is from 109.89 mg/g to 128.21 mg/g, and for absorbing MB is from 136.99 mg/g to 270.27 mg/g. In the second phase of the research, data was obtained that supports the hypothesis regarding the influence of the type and composition of the solvent on the functional changes in structure and adsorption capacity towards anionic dye wastewater. The mix solvent of aqueous/ethanol 50% has a significant effect on the elevation of the basal space with a shift in the 2θ XRD value from B-Na at 6° to 4.88°. Additionally, BET characterization data show a decrease in surface area and an increase in pore diameter from B-Na to OB, indicating intercalation that opens the agglomerated bentonite interlayer structure. The results of the adsorption data analysis show an increase in the maximum adsorption capacity on B-Na, with an initial value of 119.05 mg/g increasing to 270.27 mg/g for OB-Aq and 200 mg/g for OB-Aq/Et, but decreasing to 19.76 for OB-Et. The results of the repeated use test showed that the OB material performed satisfactorily for up to 3 adsorption cycles, with an adsorption capacity of 71.12% in the third repetition. In the third phase of the research, data analysis results showed an increase in the functional structure and degradation capacity of RhB dye wastewater using visible light-based bentonite photocatalyst composites. Material product analysis with controlled pH and synthesis temperature showed a functional structural improvement in surface area up to 11 times, with the initial BE value of 4.1 m2/g increasing to 47.3 m2/g at BE/CN/AP11.200 (exfoliated bentonite composite with g-C3N4 and Ag3PO4 at pH 11 and temperature 200 °C). Additionally, the highest increase in photodegradation capability was observed from the BE material with a degradation capability of 75.23% (adsorption mechanism) to 98.85% for the BE/CN/AP8.200 material (adsorption-photocatalysis mechanism). Based on the mechanism test, ROS species h+ play a dominant role in the photocatalysis of pollutants. Neutral-basic pH conditions and high temperatures in the composite design affect the functional improvement of the structure and photodegradation capability. The heterogeneity test proves that bentonite-based composites are heterogeneous photocatalysts. Additionally, the analysis of repeated use in the photodegradation of RhB with 3 cycles on the material with the highest photodegradation capability still shows stability in RhB removal, achieving 54.14% degradation by the third repetition.
Item Type: | Thesis (Doctoral) |
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Uncontrolled Keywords: | Air Limbah, Zat Warna, Bentonit, Organobentonit, g-C3N4, Ag3PO4 |
Subjects: | Q Science > QD Chemistry > QD146-197 Inorganic chemistry |
Divisions: | 08-Faculty of Mathematics and Natural Science > 44001-Mathematics and Natural Science (S3) |
Depositing User: | YUSUF MATHIINUL HAKIM |
Date Deposited: | 10 Mar 2025 03:07 |
Last Modified: | 10 Mar 2025 03:07 |
URI: | http://repository.unsri.ac.id/id/eprint/168070 |
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