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CuO-Incorporated onto Eggshell Templating
Available online at www.sciencedirect.com
ScienceDirect Materials Today: Proceedings 19 (2019) 1255–1260
www.materialstoday.com/proceedings
ICCSE 2018
Effective Photocatalytic Removal of Different Dye Stuffs Using ZnO/CuO-Incorporated onto Eggshell Templating Nurul Fahmi Khairol, Norzahir Sapawe, Mohamed Danish Universiti Kuala Lumpur Branch Campus Malaysian Institute of Chemical and Bioengineering Technology, Lot 1988 Vendor City, Taboh Naning, 78000 Alor Gajah, Melaka, Malaysia
Abstract The coupling of ZnO-CuO-supported on eggshell (ZnO-CuO/ES) catalyst was successfully produced through a facile one-pot electrochemical process. The photocatalytic activity of ZnO-CuO/ES catalyst were measured with degradation of various dyes and other organic compound such methylene blue (MB), malachite green (MG), crystal violet (CV), Congo red (CR), and phenol. Above 90% of all dyes and 69% of phenol degraded have been demonstrated. The organic compound in simulated wastewater shows higher degradation by ZnO-CuO/ES catalyst which are 97% (nearly complete). © 2019 Elsevier Ltd. All rights reserved. Selection and peer-review under responsibility of the scientific committee of the International Conference on Chemical Sciences and Engineering: Advance and New Materials, ICCSE 2018. Keywords: ZnO-CuO/ES, Electrochemical, Photocatalytic, Degradation, Dye Stuffs, Simulated Wastewater
1. Introduction Dyes are variety and wide can be classify by several ways. Early, terminology such as azo dyes, anthraquinone dyes, and phthalocyanine dyes was approached to distinguished dyes based on chemical structure [1]. Despite that, the dye classification by application more pleasant and encouraging compared to chemical constitution in detail which has difficulty of dyes nomenclature [2]. The technique of dyes sorting based on application adopted by the Color Index (C.I.) [3]. Several example classes of dyes by application are reactive, disperse, direct, vat, sulphur, basic, acid, solvent, and mordant [3-5]. * Corresponding author. Tel.: +6013-5757795 E-mail address: [email protected]
2214-7853 © 2019 Elsevier Ltd. All rights reserved. Selection and peer-review under responsibility of the scientific committee of the International Conference on Chemical Sciences and Engineering: Advance and New Materials, ICCSE 2018.
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Recently, many issues related to environmental problem especially in water pollution occur due to rapid development of industry. Industries like textile, paper, cosmetic, and plastic consume large amount of dyes [6]. During the dyeing, unwanted dyes generated and discharge into water body by irresponsible industrialist either with or without treatment [7]. Dyes have harmful characteristic like toxic, mutagenic, and carcinogenic toward human and produce color even in small amount such 1 ppm where can prohibited the photosynthesis activity of aquatic plant [8]. Advance oxidation processes (AOPs) is one of potential treatment method for wastewater as can convert organic compound into harmless carbon dioxide (CO2) and water (H2O) molecule [9-16]. The mechanism of AOPs take place when the electrons are trigger and elevate to the conduction band as the light or photon energy adsorb onto the surface of a semiconductor and incident ray must same or higher than the bandgap energy [17-19]. Holes that left in the valence band can oxidize donor molecules and produced hydroxyl by react with water [17-19]. In the meantime, the promoted electron at conduction band encourage the redox reactions and react with dissolved oxygen (O2) species result in formation of superoxide ions [17-19]. This study suggested the preparation of catalysts via electrochemical method as reported on previous study [616,20-25]. The size of metal oxide resulted through electrochemical process are in nanoparticles [6-16,20-25]. On the top of that, the metal oxide size also easily adjustable by current density applied in this process such a higher current density tends to yield smaller size metal oxide nanoparticles or vice versa [20]. Furthermore, this method also gives significant interaction between semiconductor and support material, for example, an isomorphous substitution of Al with Zn occurred in the aluminosilicate framework of support to result in a Si-O-Zn bonds [7]. All this factor contributes in enhancement of catalysts photocatalytic activity. The capability of catalyst to degrade the various organic pollutant by photocatalytic process is very important to meet the requirement of industry wastewater level treatment. Hereby, the ZnO/CuO-ES catalyst proposed to be testing for photodegradation of several dyes and other organic compound in this study such as Congo red (CR), crystal violet (CV), methylene blue (MB), malachite green (MG), phenol as well as simulated wastewater. 2. Experimental procedures 2.1. Materials and method The chicken eggshell (ES) were collected from the nearest farm, stall, and restaurant as solid waste at Melaka. The chemicals that will be used are N,N-dimethylformamide (DMF), naphthalene, and tetraethylammonium bromide solution was purchased from Merck, Fluka, and QReCTM respectively. Zinc (Zn) and copper (Cu) plate cell were acquired from Nilaco Metal, Japan (>99.9% purity). All the reagents were in analytical grade and were used as received. The pH solution by adjustment using 0.1 M HCl and NaOH solution were prepared using deionised water. 2.2. Catalyst preparation The collected chicken egg shell (ES) were immersed in the water overnight to eliminate the impurities and followed with dried in oven at 80 ℃ for 24 hrs. Then, the ES were crushed into pieces and grinded. To produce a powder consistent size of 355-600 μm, the ES were sieved and once again oven-dried at 100 ℃ until the weight was constant. Lastly, the resultant ES were stored in a container. A one-compartment cell was setup with pair of electrodes of Pt plate (2 × 2 cm2) as cathode while Zn and Cu plate (2 × 2 cm2) alternately as anode immersed in a 10 mL of DMF solution mixed with 0.1 M tetraethylammonium perchlorate (TEAP), 6 mmol naphthalene 15 g of ES. Next, the electrolysis was carrying out under normal atmosphere at 273 K and 480 mA cm-2 of constant current density was applied [6-16,20-25]. The produced mixture was impregnated, and oven dried at 378 K overnight.
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Finally, the calcination process take place at 823 K for 3 hrs to yield black powder of ZnO-CuO/ES catalyst. The run time for required to yield 1 wt% ZnO and 5 wt% CuO precursors of ZnO-CuO/ES catalysts approximately 932 s and 4995 s respectively. The required weight percent of the ZnO and CuO supported on ES and the time required for the complete electrolysis was calculated based on Faraday’s law of electrolysis [6-16,20-25]. 𝑡=
𝑧×𝑛
(1)
where t = total time for the constant current applied (s); F = 96,486 C mol−1, which is the Faraday constant; I = the electric current applied; z = the valency number of ions of substances (electrons transferred per ion); and n = the number of moles of Zn (no of moles, liberated n = m/M). 2.3. Photocatalytic testing The photocatalytic activity of the prepared catalyst was tested for the decolorization of methylene blue (MB), malachite green (MG), crystal violet (CV), Congo red (CR), and phenol solution. An amount of 1 g L-1 catalyst was dispersed in 100 mL of 10 mg L-1 dyes and phenol aqueous solution. The experiment was conducted under dark conditions for 1 hr to establish adsorption-desorption equilibrium and then, the mixture was irradiated by visible light from fluorescent lamp at room temperature for 2 h with constant stirring with a cooler. The distance between the light and the reaction vessel about 15 cm. At the specific time intervals, 2.5 mL of the sample solution was withdrawn and centrifuged prior measurement of the dyes and phenol concentration by a UV-vis spectrophotometer (Lambda EZ 210) using the characteristic adsorption band of the MB, MG, CV, CR, and phenol which are 664, 616, 590, 498, and 270 nm respectively. The dyes and phenol degradation percentage were calculated as follow, 𝑃𝑒𝑟𝑐𝑒𝑛𝑡𝑎𝑔𝑒 𝑜𝑓 𝐶𝑅 𝑑𝑒𝑔𝑟𝑎𝑑𝑎𝑡𝑖𝑜𝑛 % =
× 100
(2)
where C0 represents the initial concentration (mg L-1) and Ct denotes a variable concentration (mg L-1). 3. Results and Discussion 3.1. Photocatalytic testing In order to study the proficiency of the ZnO-CuO/ES catalyst, the dye such as methylene blue (MB), malachite green (MG), crystal violet (CV), and phenol were tested and compared to Congo red (CR); the results are shown in Figure 1. The initial concentration of the respective dye was held constant (10 mg L−1) and was prepared using laboratory tab water, stored under dark for 1 h, then irradiated under light for 2 h of contact time. A high degradation percentage (>80%) of various types of dye was obtained, showing the potential of these electrogenerated catalyst. Since that the wastewater contains a lot of color and has a toxic odour, the removal of color from wastewater is more significant than the removal of other organic colorless chemicals [7,11,24]. Therefore, the change in the color of the dye stuffs and simulated dyes over ZnO-CuO/ES catalyst was examined under light irradiation for a different time interval, and shown in insert picture in Figure 1. The color was disappeared steadily with increment in irradiation time, and the degradation efficiency is inversely proportional to the dye concentrations. However, a new dark bluish color was observed from a mixture of MB, MG, CR, CV and phenol; thereby believed to generate a new peak that appears at 289 nm, 410 nm and 600 nm in the system. These peaks were also diminished with the increased in time of irradiation.
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Figure 1. The UV-vis spectra of (a) methylene blue, MB (b) malachite green, MG (c) crystal violet, CV (d) Congo red, CR (e) phenol (f) simulated wastewater.
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4. Conclusion Overall, the 1 g L-1 of ZnO-CuO/ES catalyst give nearly complete degradation towards 10 mg L-1 of methylene blue (MB), malachite green (MG), crystal violet (CV), and Congo red (CR) dyes, while 69% of phenol; within 2 hrs contact time irradiated under fluorescent light. The shorten synthesis time and high photocatalytic activity of ZnOCuO/ES catalyst may make the electrochemical method the best option in preparation of catalyst. Acknowledgements The authors are grateful for the financial support by the Short Term Research Grant (STRG) from Universiti Kuala Lumpur (Grant No. 17004 & 17029) and Majlis Amanah Rakyat (MARA) Malaysia, the awards of Pinjaman Pengajian Tinggi Perak (Nurul Fahmi Khairol), and also the Universiti Kuala Lumpur Branch Campus Malaysian Institute of Chemical and Bioengineering Technology for their support. References [1] [2] [3] [4] [5] [6] [7] [8] [9] [10] [11] [12] [13] [14] [15] [16] [17] [18] [19] [20] [21]
K Hunger. (2003). Industrial Dyes, Chemistry, Properties, Applications. Retrieved from https://books.google.com.my/books?hl=en&lr=&id=uAzS4Hk2TgwC&oi=fnd&pg=PR5&dq=klaus+hunger&ots=e5zpEQR4K&sig=uljoZKsEcR7VeuLOet7JPWACTDM&redir_esc=y#v=onepage&q=klaus%20hunger&f=false MT Yagub, TK Sen, S Afroze, HM Ang. Dye and its removal from aqueous solution by adsorption: A review. Adv Colloid Interfac 2014; 209: 172–184. A Gürses, M Açıkyıldız, K Güneş, MS Gürses. (2016) Classification of Dye and Pigments. In: Dyes and Pigments. SpringerBriefs in Molecular Science. Springer, Cham N.S. Ehishan, N. Sapawe. Performance studies removal of chromium (Cr6+) and lead (Pb2+) by oil palm frond (OPF) adsorbent in aqueous solution. Materials Today: Proceeding 2018; 5(10): 21897-21904 A.H.Z. Fazry, N. Sapawe, A.I.F.A. Aziz, M.Z.H. Zainudin, M.H.H. Hafiz, M.A.F. Idris, M.F. Hanafi, M.F.M. Fozi. Materials Today: Proceeding 2018; 5(10): 22143-22147. S-M Lam, J-C Sin, AZ Abdullah, AR Mohamed. Degradation of wastewaters containing organic dyes photocatalysed by zinc oxide: a review. Desalin Water Treat 2012; 41: 131-169. N. Sapawe. Effective solar-based iron oxide supported HY zeolite catalyst for the decolorization of organic and simulated dyes. New Journal of Chemistry 2015; 39: 6377-6387. N. Sapawe, A.A. Jalil, S. Triwahyono, R.A.R.N. Sah, N.W.C. Jusoh, N.H.H. Hairom, J. Efendi. Electrochemical strategy for grown ZnO nanoparticles deposited onto HY zeolite with enhanced photodecolorization of methylene blue: Effect of the formation of Si–O–Zn bonds. Appl Catal A: Gen 2013; 456: 144–158. N.F. Khairol, N. Sapawe. Electrosynthesis of ZnO nanoparticles deposited onto egg shell for degradation of Congo red Materials Today: Proceeding 2018; 5(10): 21936-21939. N.F. Jaafar, A.A. Jalil, S. Triwahyono, M.N.M. Muhid, N. Sapawe, M.A.H. Satar, H. Asaari. Photodecolorization of methyl orange over αFe2O3-supported HY catalysts: The effects of catalyst preparation and dealumination. Chem. Eng. J. 2012; 191: 112– 122. N. Sapawe, M.F. Hanafi. Facile one-pot electrosynthesis of high photoreactive hexacoordinated Si with Zr and Zn catalyst. RSC Advances 2015; 5: 75141-75144. N. Sapawe. Hybridization of zirconia, zinc and iron supported on HY zeolite as a solar-based catalyst for the rapid decolorization of various dyes. New Journal of Chemistry 2015; 39: 4526-4533. M.S.F.A. Zamri, N. Sapawe. Performance studies of electrobiosynthesis of titanium dioxide nanoparticles (TiO2) for phenol degradation. Materials Today: Proceeding 2018; 5(10): 21797-21801. M.F. Hanafi, N. Sapawe. Remarkable degradation of methyl orange by tetragonal zirconia catalyst. Materials Today: Proceeding 2018; 5(10): 21849-21852. M.F. Hanafi, N. Sapawe, M.Z.A. Rahim, N.N. Rahman, A.H.A. Rahman, A.A. Ahmad. Performance of EGZrO2-EGFe2O3/HY as photocatalyst and its efficacy in decolorization of dye-contaminants. Malaysian Journal of Analytical Sciences 2016; 20: 1052-1058. N. Sapawe, A.A. Jalil, S. Triwahyono. Photodecolorization of methylene blue over EGZrO2/EGZnO/EGFe2O3/HY photocatalyst: Effect of radical scavenger. Malaysian Journal of Fundamental and Applied Sciences 2013; 9: 67-73. N. Sapawe, A.A. Jalil, S. Triwahyono. Photodecomposition of methylene blue over EGZrO2/HY in aqueous alkaline solution. Malaysian Journal of Fundamental and Applied Sciences 2011; 7: 137-139. Gouvêa CAK, Wypych F, Moraes SG, Durán N, Nagata N, Peralta-Zamora P. Semiconductor-assisted photocatalytic degradation of reactive dyes in aqueous solution. Chemosphere 2000; 40: 433-440. Sauer T, Neto GC, José HJ, Moreira RFPM. Kinetics of photocatalytic degradation of reactive dyes in a TiO2 slurry reactor. J Photoch Photobio A 2002; 149: 147–154. Behnajady MA, Modirshahla N, Hamzavi R. Kinetic study on photocatalytic degradation of C.I. Acid Yellow 23 by ZnO photocatalyst. J Hazard Mater 2006; 133: 226–232. Jalil A.A., Satar M.A.H., Triwahyono S., Setiabudi H.D., Kamarudin N.H.N., Jaafar N.F., Sapawe N., Ahamad R. Tailoring the current density to enhance photocatalytic activity of CuO/HY for decolorization of malachite green. Journal of Electroanalytical Chem 2013; 701:50–58.
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[22] Sapawe N., Jalil A.A., Triwahyono S. One-pot electro-synthesis of ZrO2–ZnO/HY nanocomposite for photocatalytic decolorization of various dye-contaminants. Chem. Eng. J. 2013; 225: 254–265. [23] Sapawe N., Jaafar N.F., Hairom N.H.H., Satar M.A.H., Ariffin M.N., Triwahyono S., Jalil A.A. A facile preparation of nanosized ZnO and its use in photocatalytic decolorization of methyl orange. Malaysian Journal of Fundamental and Applied Sciences 2011; 7: 19-23. [24] Sapawe N., Jalil A.A., Triwahyono S. Photodecomposition of methylene blue over EGZrO2/HY in aqueous alkaline solution. Malaysian Journal of Fundamental and Applied Sciences 2011; 7: 137-139. [25] Sapawe N., Jalil A.A., Triwahyono S., Adam S.H., Jaafar N.F., Satar M.A.H. Isomorphous sub substitution of Zr in the framework of aluminosilicate HY by an electrochemical method: Evaluation by methylene blue decolorization. Appl. Catal. B: Environ. 2012; 125: 311323. [26] Jusoh N.W.C., Jalil A.A., Triwahyono S., Setiabudi H.D., Sapawe N., Satar M.A.H., Karim A.H., Kamarudin N.H.N., Jusoh R., Jaafar N.F., Salamun N., Efendi J. Sequential desilication–isomorphous substitution route to prepare mesostructured silica nanoparticles loaded with ZnO and their photocatalytic activity. Appl. Catal. A: Gen. 2013; 468:276–287.
ScienceDirect Materials Today: Proceedings 19 (2019) 1255–1260
www.materialstoday.com/proceedings
ICCSE 2018
Effective Photocatalytic Removal of Different Dye Stuffs Using ZnO/CuO-Incorporated onto Eggshell Templating Nurul Fahmi Khairol, Norzahir Sapawe, Mohamed Danish Universiti Kuala Lumpur Branch Campus Malaysian Institute of Chemical and Bioengineering Technology, Lot 1988 Vendor City, Taboh Naning, 78000 Alor Gajah, Melaka, Malaysia
Abstract The coupling of ZnO-CuO-supported on eggshell (ZnO-CuO/ES) catalyst was successfully produced through a facile one-pot electrochemical process. The photocatalytic activity of ZnO-CuO/ES catalyst were measured with degradation of various dyes and other organic compound such methylene blue (MB), malachite green (MG), crystal violet (CV), Congo red (CR), and phenol. Above 90% of all dyes and 69% of phenol degraded have been demonstrated. The organic compound in simulated wastewater shows higher degradation by ZnO-CuO/ES catalyst which are 97% (nearly complete). © 2019 Elsevier Ltd. All rights reserved. Selection and peer-review under responsibility of the scientific committee of the International Conference on Chemical Sciences and Engineering: Advance and New Materials, ICCSE 2018. Keywords: ZnO-CuO/ES, Electrochemical, Photocatalytic, Degradation, Dye Stuffs, Simulated Wastewater
1. Introduction Dyes are variety and wide can be classify by several ways. Early, terminology such as azo dyes, anthraquinone dyes, and phthalocyanine dyes was approached to distinguished dyes based on chemical structure [1]. Despite that, the dye classification by application more pleasant and encouraging compared to chemical constitution in detail which has difficulty of dyes nomenclature [2]. The technique of dyes sorting based on application adopted by the Color Index (C.I.) [3]. Several example classes of dyes by application are reactive, disperse, direct, vat, sulphur, basic, acid, solvent, and mordant [3-5]. * Corresponding author. Tel.: +6013-5757795 E-mail address: [email protected]
2214-7853 © 2019 Elsevier Ltd. All rights reserved. Selection and peer-review under responsibility of the scientific committee of the International Conference on Chemical Sciences and Engineering: Advance and New Materials, ICCSE 2018.
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Recently, many issues related to environmental problem especially in water pollution occur due to rapid development of industry. Industries like textile, paper, cosmetic, and plastic consume large amount of dyes [6]. During the dyeing, unwanted dyes generated and discharge into water body by irresponsible industrialist either with or without treatment [7]. Dyes have harmful characteristic like toxic, mutagenic, and carcinogenic toward human and produce color even in small amount such 1 ppm where can prohibited the photosynthesis activity of aquatic plant [8]. Advance oxidation processes (AOPs) is one of potential treatment method for wastewater as can convert organic compound into harmless carbon dioxide (CO2) and water (H2O) molecule [9-16]. The mechanism of AOPs take place when the electrons are trigger and elevate to the conduction band as the light or photon energy adsorb onto the surface of a semiconductor and incident ray must same or higher than the bandgap energy [17-19]. Holes that left in the valence band can oxidize donor molecules and produced hydroxyl by react with water [17-19]. In the meantime, the promoted electron at conduction band encourage the redox reactions and react with dissolved oxygen (O2) species result in formation of superoxide ions [17-19]. This study suggested the preparation of catalysts via electrochemical method as reported on previous study [616,20-25]. The size of metal oxide resulted through electrochemical process are in nanoparticles [6-16,20-25]. On the top of that, the metal oxide size also easily adjustable by current density applied in this process such a higher current density tends to yield smaller size metal oxide nanoparticles or vice versa [20]. Furthermore, this method also gives significant interaction between semiconductor and support material, for example, an isomorphous substitution of Al with Zn occurred in the aluminosilicate framework of support to result in a Si-O-Zn bonds [7]. All this factor contributes in enhancement of catalysts photocatalytic activity. The capability of catalyst to degrade the various organic pollutant by photocatalytic process is very important to meet the requirement of industry wastewater level treatment. Hereby, the ZnO/CuO-ES catalyst proposed to be testing for photodegradation of several dyes and other organic compound in this study such as Congo red (CR), crystal violet (CV), methylene blue (MB), malachite green (MG), phenol as well as simulated wastewater. 2. Experimental procedures 2.1. Materials and method The chicken eggshell (ES) were collected from the nearest farm, stall, and restaurant as solid waste at Melaka. The chemicals that will be used are N,N-dimethylformamide (DMF), naphthalene, and tetraethylammonium bromide solution was purchased from Merck, Fluka, and QReCTM respectively. Zinc (Zn) and copper (Cu) plate cell were acquired from Nilaco Metal, Japan (>99.9% purity). All the reagents were in analytical grade and were used as received. The pH solution by adjustment using 0.1 M HCl and NaOH solution were prepared using deionised water. 2.2. Catalyst preparation The collected chicken egg shell (ES) were immersed in the water overnight to eliminate the impurities and followed with dried in oven at 80 ℃ for 24 hrs. Then, the ES were crushed into pieces and grinded. To produce a powder consistent size of 355-600 μm, the ES were sieved and once again oven-dried at 100 ℃ until the weight was constant. Lastly, the resultant ES were stored in a container. A one-compartment cell was setup with pair of electrodes of Pt plate (2 × 2 cm2) as cathode while Zn and Cu plate (2 × 2 cm2) alternately as anode immersed in a 10 mL of DMF solution mixed with 0.1 M tetraethylammonium perchlorate (TEAP), 6 mmol naphthalene 15 g of ES. Next, the electrolysis was carrying out under normal atmosphere at 273 K and 480 mA cm-2 of constant current density was applied [6-16,20-25]. The produced mixture was impregnated, and oven dried at 378 K overnight.
N.F. Khairol et al. / Materials Today: Proceedings 19 (2019) 1255–1260
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Finally, the calcination process take place at 823 K for 3 hrs to yield black powder of ZnO-CuO/ES catalyst. The run time for required to yield 1 wt% ZnO and 5 wt% CuO precursors of ZnO-CuO/ES catalysts approximately 932 s and 4995 s respectively. The required weight percent of the ZnO and CuO supported on ES and the time required for the complete electrolysis was calculated based on Faraday’s law of electrolysis [6-16,20-25]. 𝑡=
𝑧×𝑛
(1)
where t = total time for the constant current applied (s); F = 96,486 C mol−1, which is the Faraday constant; I = the electric current applied; z = the valency number of ions of substances (electrons transferred per ion); and n = the number of moles of Zn (no of moles, liberated n = m/M). 2.3. Photocatalytic testing The photocatalytic activity of the prepared catalyst was tested for the decolorization of methylene blue (MB), malachite green (MG), crystal violet (CV), Congo red (CR), and phenol solution. An amount of 1 g L-1 catalyst was dispersed in 100 mL of 10 mg L-1 dyes and phenol aqueous solution. The experiment was conducted under dark conditions for 1 hr to establish adsorption-desorption equilibrium and then, the mixture was irradiated by visible light from fluorescent lamp at room temperature for 2 h with constant stirring with a cooler. The distance between the light and the reaction vessel about 15 cm. At the specific time intervals, 2.5 mL of the sample solution was withdrawn and centrifuged prior measurement of the dyes and phenol concentration by a UV-vis spectrophotometer (Lambda EZ 210) using the characteristic adsorption band of the MB, MG, CV, CR, and phenol which are 664, 616, 590, 498, and 270 nm respectively. The dyes and phenol degradation percentage were calculated as follow, 𝑃𝑒𝑟𝑐𝑒𝑛𝑡𝑎𝑔𝑒 𝑜𝑓 𝐶𝑅 𝑑𝑒𝑔𝑟𝑎𝑑𝑎𝑡𝑖𝑜𝑛 % =
× 100
(2)
where C0 represents the initial concentration (mg L-1) and Ct denotes a variable concentration (mg L-1). 3. Results and Discussion 3.1. Photocatalytic testing In order to study the proficiency of the ZnO-CuO/ES catalyst, the dye such as methylene blue (MB), malachite green (MG), crystal violet (CV), and phenol were tested and compared to Congo red (CR); the results are shown in Figure 1. The initial concentration of the respective dye was held constant (10 mg L−1) and was prepared using laboratory tab water, stored under dark for 1 h, then irradiated under light for 2 h of contact time. A high degradation percentage (>80%) of various types of dye was obtained, showing the potential of these electrogenerated catalyst. Since that the wastewater contains a lot of color and has a toxic odour, the removal of color from wastewater is more significant than the removal of other organic colorless chemicals [7,11,24]. Therefore, the change in the color of the dye stuffs and simulated dyes over ZnO-CuO/ES catalyst was examined under light irradiation for a different time interval, and shown in insert picture in Figure 1. The color was disappeared steadily with increment in irradiation time, and the degradation efficiency is inversely proportional to the dye concentrations. However, a new dark bluish color was observed from a mixture of MB, MG, CR, CV and phenol; thereby believed to generate a new peak that appears at 289 nm, 410 nm and 600 nm in the system. These peaks were also diminished with the increased in time of irradiation.
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Figure 1. The UV-vis spectra of (a) methylene blue, MB (b) malachite green, MG (c) crystal violet, CV (d) Congo red, CR (e) phenol (f) simulated wastewater.
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4. Conclusion Overall, the 1 g L-1 of ZnO-CuO/ES catalyst give nearly complete degradation towards 10 mg L-1 of methylene blue (MB), malachite green (MG), crystal violet (CV), and Congo red (CR) dyes, while 69% of phenol; within 2 hrs contact time irradiated under fluorescent light. The shorten synthesis time and high photocatalytic activity of ZnOCuO/ES catalyst may make the electrochemical method the best option in preparation of catalyst. Acknowledgements The authors are grateful for the financial support by the Short Term Research Grant (STRG) from Universiti Kuala Lumpur (Grant No. 17004 & 17029) and Majlis Amanah Rakyat (MARA) Malaysia, the awards of Pinjaman Pengajian Tinggi Perak (Nurul Fahmi Khairol), and also the Universiti Kuala Lumpur Branch Campus Malaysian Institute of Chemical and Bioengineering Technology for their support. References [1] [2] [3] [4] [5] [6] [7] [8] [9] [10] [11] [12] [13] [14] [15] [16] [17] [18] [19] [20] [21]
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