Title Science and Technology Indonesia e-ISSN:2580-4391 p-ISSN:2580-4405 Vol. 7, No. 4, October 2022 Research Paper Improvement of Congo Red Photodegradation Performance Through Zn/Al-TiO2 and Zn/Al-ZnO Preparation Nova Yuliasari1, Amri2, Risfidian Mohadi1,3, Elfita1, Aldes Lesbani1,3* 1Graduate School of Mathematics and Natural Sciences, Faculty of Mathematics and natural Sciences, Universitas Sriwijaya, Palembang, 30662, Indonesia2Magister Program Graduate School of Mathematics and Natural Sciences, Universitas Sriwijaya, Palembang, 30139, Indonesia3Research Center of Inorganic Materials and Coordination Complexes, Faculty of Mathematics and Natural Sciences, Universitas Sriwijaya, Palembang, 30662, Indonesia *Corresponding author: aldeslesbani@pps.unsri.ac.id AbstractLayered double hydroxide (LDH) is an anionic clay material known to be effective as a catalyst for the photodegradation of dyeorganic pollutants. Zn/Al LDH was synthesized by coprecipitation then impregnated with metal oxides and calcined at 300◦Cto form Zn/Al-TiO2 and Zn/Al-ZnO as photodegradation catalysts of congo red (CR). The characterization of the catalysts afterpreparation using SEM and UV-DRS while the catalyst that have been used in 5 regeneration cycles was characterized by XRD andFTIR. Photodegradation of CR was carried out by optimizing pH, catalyst weight, and time radiation. Zn/Al LDH which was modifiedinto Zn/Al-TiO2 and ZnAl-ZnO had a better degradation percentage, rate constant, and stability than Zn/Al LDH pristine structure.Zn/Al LDH, Zn/Al-TiO2 and Zn/Al-ZnO catalyzed CR photodegradation for 120 minutes with percent degradation 68.39%, 81.24%and 71.09%, respectively. KeywordsZn/Al LDH, Congo Red, ZnO, TiO2, Photodegradation Received: 20 June 2022, Accepted: 13 September 2022 https://doi.org/10.26554/sti.2022.7.4.449-454 1. INTRODUCTION Pollution problems are often associated with global industrial waste. Waters polluted by textile dyeing can account for nearly twenty percent of the pollutants (Guzmán-Vargas et al., 2016). Layered double hydroxide (LDH) has been reported by many studies as a photocatalyst for the degradation of organic pollu- tants including textile dyes (Muhammad and Garzali, 2019). LDH is the best clay that is semiconducting, has a cation of 2+ valence at the center of an octahedral of 6 hydroxyl groups and forms lamellar. The cations with valence 2+ are partially substituted by cations with valence 3+ resulting in a positive charge on the layer of the cation structure. Negatively charged anions can be intercalated between the structure of the cation layer. LDH materials can be prepared by varying the content of cation elements to produce dierent physical and chemical properties as needed (Li et al., 2020; Contreras-Ruiz et al., 2019). Zn/Al LDH LDH materials have often been used to de- grade pollutants owing to their good semiconductor properties as photocatalysts (Li et al., 2020). Not a few studies on the degradationoforganicpollutantscatalyzedbyZn/AlLDH.Hy- drothermal methods have been used in preparing Zn/Al-based catalysts, including Zn/Al-C3N4 (Gandamalla et al., 2021), Zn/Al-TiO2 (Mourid et al., 2020), Zn/Al-ZnO (Trujillano et al., 2020), ZnBa/Al-ZnO (Elhalil et al., 2018), Zn/Al-TiO2 (Aoudjit et al., 2019), Zn/Al-ZnO (Zhang et al., 2016), and ZnCu/Al (Kimetal.,2017) asphotocatalysts in thedegradation of organic pollutants, respectively ciprooxacin, sulfamethoxa- zole, nitrophenol, caeine, dodecyl sulphate, methylene blue, and orange II dyes. LDH preparation technique by coprecipitation is often done because it is not expensive and simple to synthesize, this technique includes the deposition of two or more metal ions using a precipitating agent (Song et al., 2019). Studies have been carried out using the coprecipitation method using urea as a precipitate in the preparation of Zn/Al LDH-based materials, these studies were as follows: ZnMn/Al (Morales-Mendoza et al., 2015), ZnNi/Al (Wang et al., 2014a) and Zn/Al-TiO2 (Wang et al., 2014b) which were used in the degradation of chlorophenol,orangeGandmethyleneblue, respectively,while Zn/AlCe (Suárez-Quezada et al., 2016) and Zn/AlLa (Tzom- pantzi et al., 2014) were used for phenol degradation. The coprecipitation method using sodium hydroxide precipitate was carried out in the preparation of ZnNi/Al (Qi et al., 2018) and ZnCo/Al (Li et al., 2018) as a catalyst for rhodamine- https://crossmark.crossref.org/dialog/?doi=10.26554/sti.2022.7.4.449-454&domain=pdf https://doi.org/10.26554/sti.2022.7.4.449-454 Yuliasari et. al. Science and Technology Indonesia, 7 (2022) 449-454 B degradation, while ZnCu/Al-TiO2 (Seftel et al., 2015) in phenol degradation. The studies of coprecipitation technique that used calcination temperatures include the preparation of Zn/AlGa calcined 500◦C (Amor et al., 2018), Zn/Al LDH cal- cined500◦Cand900◦C(Abderrazeketal.,2016),Zn/Al-TiO2 calcined 500◦C (Hadnadjev-Kostic et al., 2017), Zn/Al LDH calcined 800◦C (Huo et al., 2013) which were respectively used during the degradation of methylene blue, preparation of Zn/AlCe calcined 450-900◦C (Zhu et al., 2016) and Zn/Al- TiO2 calcined 500◦C (Rudic et al., 2014) as catalysts in the degradation of rhodamine-B and the preparation of Zn/AlGa calcined at 550◦C used for phenol degradation (Prince et al., 2015). From the studies of LDH-based composites that have been carried out, it appears that not a few have prepared LDH- typemetaloxidesLDH-TiO2 andLDH-ZnOasphotocatalysts for organic pollutant degradation. LDH composited with TiO2 or ZnO has advantages. LDH is a dispersant for TiO2 owing to the surface hydroxyl group, thereby simultaneously generating and enhancing photocat- alytic properties (Contreras-Ruiz et al., 2019). Meanwhile, ZnO is often considered an alternative to TiO2 because it can absorb a wider spectrum of energy than TiO2 (Amor et al., 2018). This study is intended to prepare Zn/Al-TiO2 and Zn/Al-ZnO from the basic structure of Zn/Al LDH which has been synthesized, the catalysts used in the degradation of congo red (CR) dye. The calcination temperature of the com- posite preparation was used at 300◦C, which was relatively low compared to the calcination temperature of several previous studies. 2. EXPERIMENTAL SECTION 2.1 Materials and Instrumental The starting chemicals used in this study were aluminum ni- trate by Merck, zinc nitrate by Smart-Lab, titanium dioxide by Merck, zinc oxide by LOBA Chemie, sodium carbonate by Merck hydrogen chloride by Mallinckrodt LabGuard, and sodium hydroxide by Merck. Congo red was measured by UV- Vis Biobase BK-UV1800 PC. Characterization of morphology materials was performed by SEM Quanta-650 Oxford Instru- ment, band gap energy provided by UV-DRS Jasco V-760, diractogram by Rigaku XRD Miniex-6000, and analysis of functional groups by FTIR Alpha Bruker. 2.2 Synthesis of LDH The synthesis of Zn/Al LDH was adjusted according to the modied procedure of Yan et al. (2016) namely by coprecipi- tation. 50 mL of zinc nitrate and aluminum nitrate each with a mole ratio of Zn/Al= 3 to form a total concentration of 1 M stirred for 2 hours. To this solution, 0.5 M alkaline and 0.25 M Na2CO3 were added, each 60 mL for pH 10 conditioning. The mixture was stirred for 10 hours at 80◦C. The precipi- tate formed was ltered, washed and dried at a temperature of 110◦C, then the precipitate was weighed. 2.3 Preparation of Composite The Zn/Al-TiO2 photocatalyst was prepared according to the Zn/Al LDH synthesis procedure. A mixture of zinc nitrate and aluminum nitrate was added with alkaline and Na2CO3, after being stirred for 10 hours, it was impregnated with TiO2 using a weight ratio of LDH/TiO2= 1. The best ratio of Zn/Al to TiO2 is 1 (Djeda et al., 2020). The mixture was stirred for 3 hours and added 150 mL of 0.37 M base, then stirred again for 10 hours at a temperature of 70◦C. The mixture produced a precipitate and was ltered, washed, and then calcined at a temperature of 300◦C for 7 hours. The Zn/Al-ZnO photocat- alyst was prepared according to the same process but the oxide used was zinc oxide. 2.4 Photodegradation by Catalysts Prior to the photodegradation process, the catalyst was con- tacted with a dye model in the form of a solution of 100 mg/L CR as much as 20 mL and shaken in the dark for 60 minutes. Variations in photodegradation conditions under UV 352 nm included variations in pH, catalyst weight, and time. The rate constant (k) was determined according to the equation of the integral result of the Langmuir Hinshelwood formulation, the equation ln (C0/C) = k.t produced the value of k as the slope. C0 was the residual concentration of CR after contact in the dark room. Ct was the remainder of the CR constraint after being degraded during a certain time (t). CR was analyzed by UV-Vis at 497.8 nm. The ultrasonic desorption process and material stability were studied from a 5-cycle regeneration study. 3. RESULT AND DISCUSSSION 3.1 Eect of Photodegradation Conditions One of the things that have an eect on the photodegradation of dye is the pH condition of the media. Figure 1(a) shows the variation of pH to CR photodegradation. At pH 4, it appears that Zn/Al LDH produces the lowest C/C0 or the highest CR photodegradation. CR is an anion so it can be more compati- ble with the positive charge of the photocatalyst under acidic conditions. Figure 1(a) also shows Zn/Al-TiO2 has an opti- mum pH at pH 3 while Zn/Al-ZnO is optimum at pH 6. This study found that the optimum pH when using Zn/Al-ZnO was higher than using Zn/Al-TiO2, this was found to occur because according to Elhalil et al. (2018) under acidic conditions ZnO is at risk of being decomposed by electron holes h+ and also dissolution into Zn2+. Variations in the weight of the catalyst used can aect the photodegradation process. The more catalysts used within certain limits will provide optimum conditions. Figure 1(b) shows the eect of catalyst weight on CR photodegradation. It can be seen in the gure that the heavier the catalyst used, the better the photodegradation tendency. The decrease in the photodegradation performance of the Zn/Al-ZnO catalyst at 0.1 g according to Elhalil et al. (2018) and Yuliasari et al. (2022b) could be due to light being more dicult to penetrate into the media. © 2022 The Authors. Page 450 of 454 Yuliasari et. al. Science and Technology Indonesia, 7 (2022) 449-454 Figure 1. Eect of Media pH (a) Catalyst Weight (b) on CR Photodegradation The varied time can show the optimum condition of pho- todegradation. Figure 2(a) shows the photodegradation of CR for each catalyst over time. The photodegradation results showed that after Zn/Al LDH was modied to LDH-metal oxide, it could improve the photodegradation performance. Zn/Al catalyzed degradation of CR for 120 minutes as much as 68.39%, Zn/Al-TiO2 as much as 81.24%, and Zn/Al-ZnO as much as 71.09%. Photodegradation progresses better with an increasing rate constant. Figure 2(b) shows the rate constant for CR degra- dation in the presence of catalysts. The rate constant was increased when using a composite catalyst compared to the pristine structure LDH. The rate constants (k) using Zn/Al- TiO2 and Zn/Al-ZnO composites were 0.0158 and 0.0120, respectively, while using Zn/Al LDH was 0.0083. Several rate constants obtained by photodegradation studies of organic pol- lutants include catalyst Zn/Al-TiO2 with k 0.0060 (Contreras- Ruiz et al., 2019); catalyst Zn/AlCe with k 0.0043 (Suárez- Quezada et al., 2016) and catalyst ZnMn/Al with k 0.0013 (Morales-Mendoza et al., 2015). Figure 2. Eect of Time (a) Rate Constants of Catalysts (b) on CR Photodegradation LDH materials can be modied with metal oxides to form composites that have better structural strength (Djeda et al., 2020; Yuliasari et al., 2022a). Figure 3 shows that LDH-metal oxides, namely Zn/Al-TiO2 and Zn/Al-ZnO are better in the reuse of the material up to 5 regeneration photodegradation cycles than Zn/Al LDH as the pristine structure. Figure 3. Catalyst Regeneration Cycle 3.2 Characterization of Fresh and Reuse Materials Catalyst performance can be explained by surface conditions or surface morphology. The morphological conditions of the fresh catalysts can be seen from the 500 times magnication of SEM images in Figure 4 shows the surface of catalysts. SEM images of Zn/Al-TiO2 appear to be more homogeneous than Zn/Al-ZnO. Figure 4. SEM images of Fresh Catalysts: Zn/Al LDH (a) Zn/Al-TiO2 (b) Zn/Al-ZnO (c) LDH-based materials are classied as semiconductors if they are known to have band gap energy values below 6. Char- acterization of the band-gap energy of catalysts using UV-DRS instruments. As shown in Figure 5, the catalysts have band gap energies, namely Zn/Al-TiO2 3.20, Zn/Al-ZnO 3.18, and Zn/Al LDH slightly dierent at 3.17. The catalystst material after 5 cycles of degraded CR was analyzed byXRD. Figure 6(a) shows the XRD diractogram of the catalysts. It can be seen in the gure that Zn/Al LDH which has been used in 5 degradation cycles still has a 2\ around 10◦ which is typical for the structure of the LDH cationic layer, and a 2\ around 60◦ from the anionic interlayer (Siregar et al., 2022). This study also is in line with Contreras-Ruiz et al., © 2022 The Authors. Page 451 of 454 Yuliasari et. al. Science and Technology Indonesia, 7 (2022) 449-454 Figure 5. Band Gap Energy of Fresh Catalysts 2019 that the TiO2 peak of LDH-TiO2 appears at 2\ around 25◦, 54◦, 55◦, and 69◦. While Zn/Al-ZnO still shows the typical peak of LDH at an angle of 32◦, 34◦, 36◦, 48◦, 56◦, 63◦, and 68◦ which is in line with Bhuvaneswari et al. (2019). Analysis of the functional groups contained in the catalyst materials that have degraded the dye was carried out by FTIR. Figure 6(b) shows the FTIR spectra of catalyst materials that were used in the degradation of CR. Zhao et al. (2018) stated that the band around 3400 cm−1 is the stretching OH vibration of LDH and conveyed that the band around 1360 cm−1 is a vibration of CO32−. The band between 400 cm−1 to 800 cm−1 that appears according to Aoudjit et al. (2019) is a vibration of the bond between metal elements and oxygen. The 1620 cm−1 band is probably the vibration of the azo group or the primary amine group (Nandiyanto et al., 2019), where CR has these functional groups. Figure 6. XRD Diractogram of Reuse Catalysts (a) FTIR Spectra of Reuse Catalyst (b) After CR Photodegradation for 5 Cycles of Regeneration 4. CONCLUSION Modication of Zn/Al LDH into LDH-Metal oxides, namely Zn/Al-TiO2 and Zn/Al-ZnO increases the photodegradation performance. The percentage degradation and rate constant of congo red (CR) usingZn/Al LDH increased when usingZn/Al- metal oxides. The regeneration cycle showed that Zn/Al-TiO2 and Zn/Al-ZnO had better stability than Zn/Al-LDH. 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Page 454 of 454 INTRODUCTION EXPERIMENTAL SECTION Materials and Instrumental Synthesis of LDH Preparation of Composite Photodegradation by Catalysts RESULT AND DISCUSSSION Effect of Photodegradation Conditions Characterization of Fresh and Reuse Materials CONCLUSION ACKNOWLEDGMENT