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Preparation and characterization of SO 4 2−/TiO 2 and S 2O 8 2−/TiO 2 catalysts
Frontiers of Chemical Science and Engineering ( IF 4.5 ) Pub Date : 2007-02-01 , DOI: 10.1007/s11705-007-0009-5
Xuedan Ma , Daishi Guo , Qizhong Jiang , Zifeng Ma , Zhengfei Ma , Weidong Ye , Chunbo Li

Nanosized solid superacids SO42−/TiO2 and S2O82−/TiO2, as well as MCM-41-supported SO42−/ZrO2, were prepared. Their structures, acidities, and catalytic activities were investigated and compared using XRD, N2 adsorption-desorption, and in situ FTIR-pyridine adsorption, as well as an evaluation reaction with pseudoionone cyclization. The results showed that SO42−/TiO2 and S2O82−/TiO2 possess not only nanosized particles with diameters < 7.0 nm, a BET surface greater than 140 cm2/g and relatively regular mesostructures with pores around 4.0 nm, but also a pure anatase phase and strong acidity. Different from the Lewis acid nature of SO42−/ZrO2/MCM-41, SO42−/TiO2 and S2O82−/TiO2 exhibit mainly Bronsted acidities. The strongest Bronsted acid sites were produced on SO42−/TiO2 promoted with H2SO4, while Lewis acid sites on S2O82−/TiO2 even stronger than those on SO42−/ZrO2/MCM-41 were generated when persulfate solution was used as sulfating agent. Because of their distinct acid natures, SO42−/TiO2 and S2O82−/TiO2 exhibited catalytic activities for the cyclization of pseudoionone that were much higher than that of SO42−/ZrO2/MCM-41. It can be concluded that the existence of more Brønsted acid sites was favorable for proton participation in the cyclization reaction.

中文翻译:

SO 4 2- / TiO 2和S 2 O 8 2- / TiO 2催化剂的制备与表征

制备了纳米级固体超强酸SO 4 2- / TiO 2和S 2 O 8 2- / TiO 2,以及MCM-41负载的SO 4 2- / ZrO 2。利用XRD,N 2吸附-解吸, 原位 FTIR-吡啶吸附以及假紫酮环化反应进行了研究,比较了它们的结构,酸度和催化活性。结果表明,SO 4 2- / TiO 2和S 2 O 8 2- / TiO 2不仅具有直径小于7.0 nm的纳米级颗粒,大于140 cm 2 / g的BET表面和相对规则的介孔结构以及约4.0 nm的孔隙,还具有纯的锐钛矿相和强酸性。与SO 4 2- / ZrO 2 / MCM-41的路易斯酸性质不同,SO 4 2- / TiO 2和S 2 O 8 2- / TiO 2主要表现出布朗斯台德酸度。H 2 SO 4促进的SO 4 2- / TiO 2上产生最强的布朗斯台德酸位,而S 2 O上的路易斯酸位在当使用过硫酸盐溶液作为硫酸化剂时,生成了比SO 4 2- / ZrO 2 / MCM-41上更强的8 2- / TiO 2。由于SO 4 2- / TiO 2和S 2 O 8 2- / TiO 2具有独特的酸性质,因此它们对假紫罗酮的环化反应具有比SO 4 2- / ZrO 2 / MCM-41更高的催化活性。。可以得出结论,存在更多的布朗斯台德酸位点有利于质子参与环化反应。
更新日期:2007-02-01
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