22 research outputs found

    Effect of aluminum modification on catalytic performance of Pt supported on MCM-41 for thiophene hydrodesulfurization

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    The catalytic activities and properties of platinum supported on siliceous MCM-41 and Al-modified MCM-41, such as Al-incorporated MCM-41 (AlMCM-41) and alumina-modified MCM-41 (Al_2O_3-MCM-41), for the hydrodesulfurization (HDS) of thiophene were investigated. Al_2O_3-MCM-41 was prepared by an impregnation method using aluminum nitrate (Al(NO_3)_3·9H_2O) aqueous solution. Pt/Al_2O_3-MCM-41 catalyst showed high and stable activity for HDS of thiophene and this activity was remarkably higher than that of a commercial CoMo/Al_2O_3 HDS catalyst. The catalysts were characterized by XRD, hydrogen adsorption, ammonia-TPD, 2-propanol dehydration, cumene cracking and FT-IR. Dispersion of platinum on Al_2O_3-MCM-41 was remarkably higher than on MCM-41 or on AlMCM-41. It was revealed that the acidity of Al_2O_3-MCM-41 was higher than that of MCM-41 or of AlMCM-41. Furthermore, it was observed that there exist Brønsted acid sites on Al-modified MCM-41. FT-IR spectra of thiophene adsorbed on Al-modified MCM-41 support indicates that thiophene molecules interact with Brønsted acid sites on Al-modified MCM-41. It was found that the HDS activity of Pt/quartz mixed mechanically with Al-modified MCM-41 catalyst was higher than that calculated. This suggests that there exists spillover hydrogen on supportedPt catalysts in the HDS of thiophene. Results revealed that the high activity of Pt/Al_2O_3-MCM-41 catalyst for HDS reaction is due to good harmony of high dispersion of Pt particles and Brønsted acidity of the support

    Preparation of highly active AlSBA-15-supported platinum catalyst for thiophene hydrodesulfurization

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    The catalytic activities of various noble metals (Pt, Pd, Rh, and Ru) supported on siliceous SBA-15 and Al-containing SBA-15 (AlSBA-15) for hydrodesulfurization (HDS) of thiophene at 350 C were investigated. AlSBA-15 was prepared by a grafting method using aluminum isopropoxide (Al(OC3H7)3) hexane solution. The HDS activity of Pt/AlSBA-15 catalyst was the highest among those of various supported noble metal catalysts, and this activity was higher than that of commercial CoMo/Al2O3 HDS catalyst. The catalysts were characterized by XRD analysis, hydrogen adsorption, 2-propanol dehydration, cumene cracking, and FT-IR. Dispersion of Pt on SBA-15 was remarkably enhanced by Al grafting. It was revealed that the acidity of AlSBA-15 was higher than that of SBA-15. Furthermore, Brønsted acid sites were observed on AlSBA-15. FT-IR spectra of thiophene adsorbed on AlSBA-15 indicate that thiophene molecules interact with Brønsted acid sites on the surface of AlSBA-15 and that the strength of this interaction was stronger than that of SBA-15. Based on these results, thiophene molecules activated on Brønsted acid site of AlSBA-15 and hydrogen molecules activate to form spillover hydrogen on Pt particles in Pt/AlSBA-15 catalyst in the HDS of thiophene

    Effects of Dealumination and Desilication of Beta Zeolite on Catalytic Performance in n-Hexane Cracking

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    Catalytic cracking of n-hexane to selectively produce propylene on Beta zeolite was carried out. The H-Beta (HB) (Si/Al = 77) zeolite showed higher catalytic stability and propylene selectivity than the Al-rich HB (Si/Al = 12), due to its smaller number of acid sites, especially Lewis acid sites (LAS). However, catalytic stability and propylene selectivity in high n-hexane conversions were still not satisfactory. After dealumination with HNO3 treatment, catalytic stability was improved and propylene selectivity during high n-hexane conversions was increased. On the other hand, catalytic stability was not improved after desilication with NaOH treatment, although mesopores were formed. This may be related to the partially destroyed structure. However, propylene selectivity in high n-hexane conversions was increased after alkali treatment. We successfully found that the catalytic stability was improved and the propylene selectivity in high n-hexane conversions was further increased after the NaOH treatment followed by HNO3 treatment. This is due to the decrease in the number of acid sites and the increase in mesopores which are beneficial to the diffusion of coke precursor

    Control of the Al Distribution in the Framework of ZSM‑5 Zeolite and Its Evaluation by Solid-State NMR Technique and Catalytic Properties

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    The effects of the organic structure-directing agents (OSDAs) and Na cations for the synthesis of ZSM-5 on the location of Al atom in the framework as well as the acidic and catalytic properties were investigated. To achieve these purposes, ZSM-5 zeolites were synthesized by using four kinds of OSDAs including tetrapropylammonium hydroxide cations, dipropylamine, cyclohexylamine, and hexamethylenimine with or without Na cations. In situ FT-IR spectroscopy using CO as probe molecule was applied to the evaluation of the acid property of the ZSM-5 zeolites. The location of Al atoms was examined by high resolution <sup>27</sup>Al MAS and MQMAS NMR techniques. The constraint index (CI) has also been used to estimate the distribution of acid sites in the micropores. The location of acid sites was investigated based on the difference in the transition-state shape-selectivity through the cracking of <i>n</i>-hexane and 3-methylpentane. Furthermore, the cracking of various types of paraffins and the conversion of aromatic compounds were conducted to clarify the acid site distributions
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