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Effect of calcination temperature on structure, composition and properties of S2O82-/ZrO2 and its catalytic performance for removal of trace olefins from aromatics

机译:煅烧温度对S2O82- / ZrO2结构,组成和性能的影响及其催化从芳烃中去除痕量烯烃的性能

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摘要

A solid superacid catalyst, S2O82-/ZrO2 (S(2)Z), was synthesized by the immersion-precipitation method to remove olefins from aromatics; the effect of calcination temperature on the structure, chemical and phase composition and properties of persulfated zirconia were studied. A series of synthesized catalyst samples were characterized by TG-DTG, XRD, SEM, FTIR, FTIR pyridine adsorption (py-IR) and N-2 adsorption analysis. The characterization results revealed that the outstanding activity for removal trace olefins from aromatics is attributed to the interaction between sulfur species and ZrO2, particularly the more covalent persulfate with tetragonal zirconia (t-ZrO2), and the calcination temperature was shown to be the key factor in governing the phase composition of S(2)Z. Py-IR analysis indicated that the high catalytic activity was well correlated with excellent acidity, primarily with the Lewis acidity of S(2)Z. Different calcination temperatures influenced the amount of catalytically active t-ZrO2, which was favorable to increasing the number of acid sites, improving surface properties and thus enhancing the catalytic activity. Moreover, the regeneration procedure did not change the structure and crystal form of the catalyst. The catalytic activity test revealed that S(2)Z calcined at 650 degrees C was superiorly active and efficiently reusable to remove trace olefins and exhibits promising application prospects in industry.
机译:固体超强酸催化剂S2O82- / ZrO2(S(2)Z)是通过沉沉沉淀法从芳烃中去除烯烃而合成的。研究了煅烧温度对过氧化锆结构,化学和相组成及性能的影响。通过TG-DTG,XRD,SEM,FTIR,FTIR吡啶吸附(py-IR)和N-2吸附分析对一系列合成的催化剂样品进行了表征。表征结果表明,从芳烃中去除痕量烯烃的出色活性归因于硫物种与ZrO2之间的相互作用,尤其是过硫酸盐与四方氧化锆(t-ZrO2)之间的相互作用,并且煅烧温度是关键因素在控制S(2)Z的相组成方面。 Py-IR分析表明,高催化活性与优异的酸度密切相关,主要与S(2)Z的路易斯酸度相关。不同的煅烧温度影响催化活性的t-ZrO2的量,这有利于增加酸位的数量,改善表面性能并因此增强催化活性。而且,再生程序没有改变催化剂的结构和晶体形式。催化活性测试表明,在650摄氏度下煅烧的S(2)Z具有优异的活性,可有效地重复使用以去除痕量烯烃,在工业上具有广阔的应用前景。

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