Brønsted-type relationship for surface active sites on solid acid catalysts: 1-butene isomerization on TiO2SiO2, ZrO2SiO2, and Al2O3SiO2 mixed oxide catalysts

Cristian Contescu , Vlad T. Popa , James B. Miller , Edmond I. Ko , James A. Schwarz
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引用次数: 3

Abstract

Acidic properties (acid sites' strength and concentration) of three series of mixed oxide catalysts (titania-silica, zirconia-silica and alumina-silica) were analyzed by proton affinity distributions. Catalytic properties under mild dehydration conditions (1-butene isomerization at 423 K) of these materials were also evaluated. A Brønsted-type correlation was found between first-order apparent isomerization rate constants and acid strengths of certain components of the pK spectra of the catalysts. This was explained in terms of proton transfer processes that take place at both wet and dry interfaces, i.e. at the surface hydroxyl layer. The results were discussed in terms of Fourier transform infrared data which indicate the presence of large surface hydroxyl populations on all catalysts under the reaction conditions.

固体酸催化剂表面活性位点的br ønsted型关系:TiO2SiO2、ZrO2SiO2和Al2O3SiO2混合氧化物催化剂上的1-丁烯异构化
通过质子亲和分布分析了钛-二氧化硅、氧化锆-二氧化硅和氧化铝-二氧化硅三系混合氧化物催化剂的酸性性质(酸位强度和浓度)。在轻度脱水条件下(423 K时1-丁烯异构化),评价了这些材料的催化性能。一阶表观异构化速率常数与催化剂pK谱中某些组分的酸强度呈br ønsted型相关。这可以用质子转移过程来解释,质子转移过程发生在湿界面和干界面,即在表面羟基层。用傅里叶变换红外数据对结果进行了讨论,结果表明在反应条件下,所有催化剂表面都存在大量的羟基基团。
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