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首页> 外文期刊>Applied Surface Science >Effect of modification methods on the surface properties and n-butane isomerization performance of La/Ni-promoted SO42-/ZrO2-Al2O3
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Effect of modification methods on the surface properties and n-butane isomerization performance of La/Ni-promoted SO42-/ZrO2-Al2O3

机译:改性方法对La / Ni促进的SO42- / ZrO2-Al2O3表面性能和正丁烷异构化性能的影响

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摘要

The La and/or Ni was introduced into alumina-promoted sulfated zirconia by impregnation and co-precipitation to improve the catalytic property of n-butane isomerization. Catalysts characterization shows that the addition of La/Ni has a remarkable influence on the surface and textual properties depending on the modification method. The impregnation of La/Ni facilitates the transformation of a small amount of tetragonal zirconia into monoclinic phase, while the co-precipitation improves the stability of tetragonal ZrO2. H-2-TPR indicates that the addition of La/Ni changes the interaction between SO42- and supports, which affects the acidity on the surface. Specifically, the Lewis acidity is significantly enhanced by either modification method. The co-precipitation reserves almost all of the Bronsted acid sites, while the impregnation causes a remarkable decrease of Bronsted acid sites. Reaction results demonstrate that the co-precipitation exhibits a significant advantage over impregnation that the higher conversion of n-butane and selectivity to isobutane are obtained on the catalyst prepared by co-precipitation. The increase of catalytic activity is ascribed to the accelerated activation rate of n-butane molecules by hydride subtraction on the Lewis acid sites at higher reaction temperature. Furthermore, the addition of La/Ni improves the selectivity to isobutane by inhibiting the bimolecular reaction. (C) 2016 Elsevier B.V. All rights reserved.
机译:通过浸渍和共沉淀将La和/或Ni引入氧化铝促进的硫酸化氧化锆中,以提高正丁烷异构化的催化性能。催化剂表征表明,La / Ni的添加对表面和文本性质有显着影响,具体取决于改性方法。 La / Ni的浸渍有助于少量的四方氧化锆转变为单斜晶相,而共沉淀可提高四方ZrO2的稳定性。 H-2-TPR表明,La / Ni的添加改变了SO42-与载体之间的相互作用,从而影响了表面的酸性。具体地,通过任一种改性方法都显着提高了路易斯酸度。共沉淀保留了几乎所有的布朗斯台德酸性位,而浸渍导致布朗斯台德酸性位的显着减少。反应结果表明,与共浸渍相比,共沉淀具有显着的优势,因为在通过共沉淀制备的催化剂上,正丁烷的转化率更高,对异丁烷的选择性更高。催化活性的增加归因于在较高的反应温度下,通过在路易斯酸位点上进行氢化物减法,正丁烷分子的活化速率加快。此外,La / Ni的添加通过抑制双分子反应而提高了对异丁烷的选择性。 (C)2016 Elsevier B.V.保留所有权利。

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