Zeolite Catalysis

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Zeolite Catalysis ( zeolite-catalysis )

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rutile is expected to further deteriorate the photocatalytic activity [41–43]. Therefore, the calcination temperature used in this study was 523 K. 3. ExperimentalSection 3.1. Chemicals Ethanol (ě99.5%) and titanium (IV) isopropoxide (TIP) (97%) were purchased from Sigma-Aldrich (St. Louis, MO, USA). The ammonium form of zeolite ZSM-5 (NH4-ZSM-5; nSi/nAl = 55) was supplied by Süd Chemie AG (Munich, Germany). TiO2 was obtained as Hombikat from Sachtleben Chemie (NRW, Duisburg, Germany) and as P25 from Evonik Degussa (Frankfurt, Germany). All chemicals were used as received without further purification. 3.2. Preparation of the TiO2/ZSM-5 Composites 3.2.1. Solid-State Dispersion First, 1.25, 2.50 or 3.75 g of zeolite ZSM-5 was suspended in 20 cm3 of deionized water with continuous stirring for 2 h. Subsequently, 3.75, 2.50 or 1.25 g of Hombikat was added to the ZSM-5 slurry with vigorous stirring for another 2 h. Then, the slurry was dried for 12 h in an air oven at 363 K, grounded and calcined at 523 K in air for 6 h. The composites prepared by this method are referred to as HZSSD. The label HZSSD represents the Hombikat/ZSM-5 composites prepared using solid-state dispersion. The mass fractions of Hombikat to ZSM-5 are 25/75, 50/50 and 75/25, respectively. 3.2.2. Sol-Gel Synthesis A TiO2 sol was prepared by acid-catalyzed hydrolysis of TIP according to [49]. 4.6, 9.2 or 14.4 cm3 of TIP equivalent to 1.25, 2.50 or 3.75 g of TiO2 were dissolved in 25 cm3 of ethanol (ě99.5%, Sigma-Aldrich, St. Louis, MO, USA) and vigorously stirred at room temperature for 2 h. Subsequently, 1 cm3 of 1M HNO3 (65%, VWR International, Radnor, PA, USA) was added to the solution under continuous stirring for 5 min until gelation takes place. Then, 25 cm3 of deionized water was added to the gel. The resulting gel was stirred for another 3 h. To obtain the TiO2/ZSM-5 composites with mass fractions of 25/75, 50/50 or 75/25, the TiO2 sol was added to a suspension of 3.75, 2.50 or 1.25 g of ZSM-5 in 50 cm3 of deionized water over 1 h at room temperature under stirring. The resulting gel was stirred for another 6 h and dried in an air oven at 353 K for 12 h. Finally, the obtained solid was ground to a powder and calcined at 523 K in air for 6 h. These composites were named TZSG indicating the composition of TiO2/ZSM-5 prepared by sol-gel synthesis. For comparison, pure TiO2 and a composite of TiO2/sea sand (Merck) (TSSSG) were also prepared using the same sol-gel route. A TiO2/ZSM-5 composite (50/50) for the purpose of studying the influence of calcination temperature was also prepared by 168

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