• International Journal of Technology (IJTech)
  • Vol 11, No 3 (2020)

Synthesis of Nano-Photocatalyst ZnO-Natural Zeolite to Degrade Procion Red

Tuty Emilia Agustina, Elda Melwita, David Bahrin, Rianyza Gayatri, Indah Fitriany Purwaningtyas

Corresponding email: tuty_agustina@unsri.ac.id

Cite this article as:
Agustina, T.E., Melwita, E., Bahrin, D., Gayatri, R., Purwaningtyas, I.F., 2020. Synthesis of Nano-Photocatalyst ZnO-Natural Zeolite to Degrade Procion Red. International Journal of Technology. Volume 11(3), pp. 472-281

Tuty Emilia Agustina Chemical Engineering Department, Faculty of Engineering, Universitas Sriwijaya, 30662, Indralaya, South Sumatra, Indonesia
Elda Melwita Chemical Engineering Department, Faculty of Engineering, Universitas Sriwijaya, 30662, Indralaya, South Sumatra, Indonesia
David Bahrin Chemical Engineering Department, Faculty of Engineering, Universitas Sriwijaya, 30662, Indralaya, South Sumatra, Indonesia
Rianyza Gayatri Chemical Engineering Department, Faculty of Engineering, Universitas Sriwijaya, 30662, Indralaya, South Sumatra, Indonesia
Indah Fitriany Purwaningtyas Chemical Engineering Department, Faculty of Engineering, Universitas Sriwijaya, 30662, Indralaya, South Sumatra, Indonesia
Email to Corresponding Author


The development of textile factories has had a significant impact on the environment because dye wastewater is difficult to degrade. The handling of textile wastewater usually involves the adsorption method, in which pollutants only transfer to another phase. As an alternative solution, a photodegradation method was developed using photocatalyst material assisted by ultraviolet irradiation. In this photodegradation method, dye substances are broken down into components that are simpler and safer for the environment. The possibility of using sunlight as a radiation source makes this a particularly promising method for countries such as Indonesia. Procion red, one of the most commonly utilized synthetic dyes in the home textile or Batik industry, was used as a model pollutant in this study. The objectives of the present research were to synthesize and characterize a nano-photocatalyst of ZnO-natural zeolite with the capacity to degrade Procion red. This nano-photocatalyst was synthesized using the sol-gel method, by which Zn(CH3COO)2 2H2O was used as a precursor and combined with natural zeolite to increase its photocatalytic ability. The nano-photocatalyst was characterized using X-ray diffraction (XRD), scanning electron microscope/energy dispersive X-ray spectroscopy (SEM/EDX), and Brunauer-Emmett-Teller (BET). The activity of nano-photocatalyst ZnO-natural zeolite was compared to ZnO alone and natural zeolite alone in terms of its ability to degrade Procion red. An average photocatalyst crystallite diameter of 82 nm was achieved, proving that a nano-sized photocatalyst of ZnO-natural zeolite was successfully synthesized. BET characterization showed that nano-photocatalyst ZnO-natural zeolite had a specific surface area of 14.84 m2/g, a pore size of 32.71 nm, and a pore volume of 0.12 cm2/g. A peak Procion red degradation percentage of 96.23% was obtained using nano-photocatalyst ZnO-natural zeolite after 120 minutes of irradiation under sunlight applied to a Procion red concentration of 50 ppm.

Nano-photocatalyst; Natural zeolite; Photodegradation; Procion red; ZnO


The development of the textile industry has certainly had an impact on the environment, as the dye wastewater produced by this industry is difficult to degrade. Dye-containing wastewater usually consists of non-biodegradable organic compounds that can contribute to pollution, especially in aquatic environments. However, the wastewater produced by the textile industry also contains synthetic dyes that are harmful to the environment. Procion red is one of the most commonly used synthetic dyes in the home textile or Batik industry. This synthetic dye is difficult to degrade due to the strong covalent bonds between the carbon atoms of the dye stuff  and the O,  N,  or  S  atoms of the hydroxy, amino, or thiol groups of the polymer (Hunger, 2003).

 Degradation methods, such as coagulation-flocculation (Rusydi et al., 2016) and a combination of electrocoagulation and photocatalysis (Sharfan et al., 2018), have been developed for dyes in the textile industry. However, these chemical processing methods apply large quantities of chemicals and produce sludge, which must be separated at the end of process. Membrane applications are quite effective but require significant operational costs and have the disadvantage of introducing new problems, such as the production of compounds with more concentrated pollutant levels. A photodegradation method using photocatalyst materials and ultraviolet light irradiation has been developed as an alternative method (Agustina et al., 2015; Zhao et al., 2015). Among modern methods of dealing with wastewater, photodegradation is relatively inexpensive and easy to implement. Widely studied photocatalysts include metal oxide semiconductors, such as ZnO and TiO2. The ZnO semiconductor has an advantage over TiO2 because it is able to absorb the UV spectrum of the sun and quantum of light more readily than TiO2. In addition, ZnO is an efficient photocatalyst material for the detoxification of wastewater because it produces H2O2 more efficiently than other photocatalysts (Hidayanto et al., 2013; Mydeen et al., 2019). ZnO is widely used due to its cost-effectiveness, high oxidation ability, and wide availability. However, electron-hole recombination can block the photocatalytic activity of pure ZnO.

        Research has been carried out to investigate the pure photocatalytic activity of semiconductors, such as ZnO, in degrading organic compounds, such as synthetic dyes. Photocatalyst activity can be increased through the development of supporting materials, such as natural zeolites. Natural zeolite, a cheap and locally available absorbent, has been used in the energy field and for many applications such as additives, catalysts, ion exchangers, and absorbents (Millar et al., 2016; Papa et al., 2017; Wulandari et al., 2019). Zeolite is used as a carrier molecular because its crystal structure is porous and has a large surface area, it is composed of a silica-alumina skeleton, it has a high thermal stability, and its presence is quite abundant (Wang and Peng, 2010). The pore structure of zeolite also allows it to be used as a host material (Rahman et al., 2018). Moreover, zeolite is recommended for the degradation of dye through adsorption due to its large surface area (Viswanathan, 2018). The surface area and acidity of natural zeolite could be modified easily (Suhartana et al., 2018; Wulandari et al., 2019). The present study utilized natural zeolite from West Java.

        Many efforts have been made to enhance the photocatalytic performance, especially in dye degradation. Such efforts have involved making ZnO-zeolite composites by impregnation methods (Salam et al., 2018), doping ZnO nanoparticles with natural zeolite (Rahman et al., 2018), and adding noble metals, such as Ag nanoparticles (Kusdianto et al., 2019) and Fe3O4 (Winatapura et al., 2016). ZnO has a low capacity for adsorption as a photocatalyst, but ZnO photocatalysts can be combined with adsorbents, such as zeolite, to face this problem (Wismayanti, 2015). Therefore, the present study aimed to synthesize photocatalysts of nano-sized ZnO-natural zeolites in order to utilize the adsorbent properties of natural zeolites as well as the photocatalytic properties of ZnO. The obtained photocatalyst material was tested for photocatalyst activity in the degradation of synthetic dyes. Then, this activity was compared with the degradation of Procion red by standard ZnO and natural zeolites alone.


Nano-photocatalyst ZnO-natural zeolite was synthesized using Zn(CH3COO)2 2H2O precursors and activated natural zeolite. Characterization of this photocatalyst showed that it was formed with an average crystallite size of 82 nm, a specific surface area of 14.84 m2/g, a pore size of 32.71 nm, and a pore volume of 0.12 cm2/g. The use of nano-photocatalyst ZnO-natural zeolite produced the highest synthetic dye degradation percentage (96.23%) in the degradation of 50 ppm Procion red under 120 minutes of sunlight irradiation.


The authors would like to thank LPPM Universitas Sriwijaya for funding this research through Hibah Unggulan Kompetitif of 2018. The authors also wish to acknowledge the Waste Management Technology Laboratory of the Chemical Engineering Department for providing laboratory assistance.


Agustina, T.E., Komala, R., Faizal, M., 2015. Application of TiO2 Nano Particles Photocatalyst to Degrade Synthetic Dye Wastewater under Solar Irradiation. Contemporary Engineering Sciences, Volume 8(34), pp. 1625–1636

Balcha, A., Yadav, O.P., Dey, T., 2016. Photocatalytic Degradation of Methylene Blue Dye by Zinc Oxide Nanoparticles Obtained from Precipitation and Sol-Gel Methods. Environmental Science and Pollution Research, Volume 23(24), pp. 25485–25493

Charanpahari, A., Umare, S., Gokhale, S.P., Sudarsan, V., Sreedhar, B., Sasikala, R., 2012. Enhanced Photocatalytic Activity of Multi-Doped TiO2 for the Degradation of Methyl Orange. Applied Catalysis A: General, Volume 443-444, pp. 96102

Chatti, R., Rayalu, S., Dubey, N., Labhsetwar, N., dan Devotta, S., 2007. Solar-based Photoreduction of Methyl Orange using Zeolite Supported Photocatalytic Materials. Solar Energy Materials 7 Solar Cells, Volume 91, pp. 180190

Fraditasari, R., Wardhani, S., Khunur, M.M., 2015. Degradasi Methyl Orange Menggunakan Fotokatalis TiO2-N: Kajian Pengaruh Sinar dan Konsentrasi TiO2-N (Methyl Orange Degradation using TiO2-N Photocatalyst: The Study of Effect of Irradiation and TiO2-N Concentration). Jurnal Ilmu Kimia, Volume 1(1), pp. 606612

Hidayanto, E., Sutanto, H., Sofian, K., Arifin, Z., 2013. Pembuatan Lapisan Fotokatalis Zinc Oxide (ZnO) dengan Teknik Spray Coating dan Aplikasinya pada Pengering Jagung (Preparation of Zinc Oxide  (ZnO) Photocatalyst Layer by Spray Coating Technique and Its Application in Corn Dryer). Jurnal Berkala Fisika, Volume 16, pp. 119124

Hunger, K., 2003. Industrial Dyes: Chemistry, Properties, Applications. Weinheim: Wiley-vch Verlan GmbH & Co. KGaA

Kusdianto, K., Widiyastuti, W., Shimada, M., Nurtono, M.T., Machmudah, S., Winardi, S., 2019. Photocatalytic Activity of ZnO-Ag Nanocomposites Prepared by a One-step Process using Flame Pyrolysis. International Journal of Technology, Volume 10(3), pp. 571581

Millar, G., Couperthwaite, S.J., Alyuz, K., 2016. Behavior of Natural Zeolites Used for the Treatment of Simulated and Actual Coal Seam Gas Water. Journal of Environmental Chemical Engineering, Volume 4(2), pp. 19181928

Mydeen, S., Kottaisamy, M., Vasantha, V.S., Ramachandran, K., 2019. Photocatalytic Performances and Antibacterial Activities of Nano-ZnO Derived by Cetrimide-based Co-precipitation Method by Varying Solvents. International Journal of Innovative Technology and Exploring Engineering (IJITEE), Volume 9, pp. 22783075

Naimah, S., Aviandharie, S.A., Jati, B.N., Aidha, N.N., Cahyaningtyas, A.A., 2011. Degradasi Zat Warna Pada Limbah Cair Industri Tekstil Dengan Metode Fotokatalitik Menggunakan Nano Komposit TiO2-Zeolit (Degradation of Dyes in Textile Industry Wastewater by Photocatalytic Method Using TiO2-Zeolite Nano Composite). Jurnal Kimia Dan Kemasan, Volume 36(2), pp. 225236

Pakpahan, J.K., Karo, P.K., Suroto, B.J., 2017. Studi Luas Permukaan Spesifik Zeolit Akibat Pengaruh Mikrostruktur dan Potensinya sebagai Elektrode Superkapasitor (Study of Zeolite Specific Surface Area Due to the Effects of Microstructure and its Potential as Supercapacitor Electrodes). Jurnal Teori Dan Apikasi Fisika, Volume 5(1), pp. 19–24

Papa, E., Medri, V., Amari, S., Manaud, J., Benito, P., Vaccari, A., Landi, E., 2017. Zeolite Geopolymer Composite Materials: Production and Characterization. Journal of Cleaner Production, Volume 171, pp. 7684?

Rahman, A., Nurjayadi, M., Wartilah, R., Kusrini, E., Prasetyanto E.A., Degermenci, V., 2018. Enhanced Activity of TiO2/Natural Zeolite Composite for Degradation of Methyl Orange under Visible Light Irradiation. International Journal of Technology, Volume 9(6), pp. 11591167

Rakhmawaty, D., Putra, D.A., 2011. Fotodegradasi Methylene Blue Menggunakan  Fotokatalis TiO2/Zeolit Alam. Presiding Seminar Nasional Kimia dan Pendidikan Kimia III (Methylene Blue Photodegradation by using TiO2/Natural Zeolite Photocatalysts. The National Seminar Proceeding of Chemistry and Chemistry Education III). pp. 255264, Program Studi Pendidikan Kimia Jurusan Pendidikan MIPA, FKIP, Universitas Sebelas Maret Surakarta, Surakarta

Razzak, M.T., Las, T., Priyambodo, 2013. The Characterization of Indonesian's Natural Zeolite for Water Filtration System. Jurnal Kimia Valensi, Volume 3(2), pp. 129–137

Rusydi, A.F., Suherman, D., Sumawijaya, N., 2016. Pengolahan air Limbah Tekstil Melalui Proses Koagulasi-Flokulasi Dengan Menggunakan Lempung Sebagai Penyumbang Partikel Tersuspensi. Studi Kasus: Banaran, Sukoharjo dan Lawean, Kerto Suro, Jawa Tengah (Textile Wastewater Treatment through Coagulation-Flocculation Process using Clay as Contributor to Suspended Particles. Case Study: Banaran, Sukoharjo and Lawean, Kerto Suro, Central Java). Arena Tekstil, Volume 31(2), pp. 105–114

Salam, A., Agustina, T.E., Mohadi, R., 2018. Photocatalytic Degradation of Procion Red Synthetic Dye using ZnO-Zeolite Composites. International Journal of Scientific and Technology Research, Volume 7(8), pp. 54–59

Sharfan, N., Shobri, A., Anindria, F.A., Mauricio, R., Tafsili, M.A.B., Slamet, S., 2018. Treatment of Batik Industry Waste with a Combination of Electrocoagulation and Photocatalysis. International Journal of Technology, Volume 9(5), pp. 936943

Suhartana, Sukmasari, E., Azmiyawati, C., 2018. Modification of Natural Zeolite with Fe(III) and its Application as Adsorbent Chloride and Carbonate Ions. In: IOP Conference Series: Materials Science and Engineering, Volume 349, pp. 111

Takeda, N., Torimoto, T., Sampath, S., Kuwabata, S., Yoneyama, H., 1995. Effect of Inert Support for Titanium Dioxide Loading on Enhancement of Photodecomposition Rate of Gaseous Propionaldehyde. The Journal of Physical Chemistry, Volume 99, pp. 99869991

Vaiano, V., Matarangolo, M., Sacco, O., Sannino, D., 2017. Photocatalytic Removal of Eriochrome Black T Dye Over ZnO Nanoparticles Doped with Pr, Ce or Eu. Chemical Engineering Transactions, Volume 57, pp. 625–630

Viswanathan, B., 2018. Photocatalytic Degradation of Dyes: An Overview. Current Catalysis, Volume 7(1), pp. 125

Wang, S., Peng, Y., 2010. Natural Zeolites as Effective Adsorbents in Water and Wastewater Treatment. Chemical Engineering Journal, Volume 156(1), pp. 1124

Widiyastuti, W., Maula, I., Nurtono, T., Taufany, F., Machmudah, S., Winardi, S., Panatarani, C., 2014. Preparation of Zinc Oxide/Silica Nanocomposite Particles via Consecutive Sol-Gel and Flame-Assisted Spray-Drying Methods. Chemical Engineering Journal, Volume 254, pp. 252–258

Winatapura, D.S., Dewi, S.H., Adi, W.A., 2016. Synthesis Characterization, and Photocatalytic Activity of Fe3O4@ZnO Nano Composite. Internasional Journal of Technology, Volume 7(3), pp. 408416

Wismayanti, D.A., Diantariani, N.P., Santi, S.R., 2015. Pembuatan Komposit ZnO-Arang Aktif sebagai Fotokatalis untuk Mendegradasi Zat Warna Metilen Biru (Preparation of ZnO- Active Charcoal Composites as Photocatalysts to Degrade Methylene Blue Dye). Jurnal Kimia, Volume 9(1), pp. 109116

Wulandari, D.A., Nasruddin, Djubaedah, E., 2019. Selectivity of Water Adsorbent Characteristic on Natural Zeolite in Cooling Application. Journal of Advanced Research in Fluid Mechanics and Thermal Sciences, Volume 55(1), pp. 111118

Zhao, L., Liu, Z.C., Liu, Z.F., 2015. Synthetic Zeolite Supported ZnO Nanoparticle Materials for Photocatalytic Applications. Energy Materials: Materials Science and Engineering for Energy Systems, Volume 10(2), pp. 60–64