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Core/shell-structured Al-MWW@B-MWW zeolites for shape-selective toluene disproportionation to para-xylene

机译:核/壳结构Al-MWW @ B-MWW沸石,用于形状选择甲苯歧化为对二甲苯

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摘要

A shape-selective core/shell-structured Al-MWW@B-MWW composite catalyst has been hydrothermally synthesized through isomorphically overgrowing borosilicate on premade MCM-22 aluminosilicate. The secondary growth of borosilicate enlarged obviously the thickness of the platelet crystallites of MCM-22 and increased the surface Si/Al ratio from 16 to 222. The Fourier transform infrared (FTIR) spectra of adsorbed 2,6-di-tert-butylpyridine indicated that the Br?nsted acid sites located on the external surface were virtually covered completely by the generated B-MWW layer, whereas those acid sites within channels were still accessible and detectable by using pyridine or ammonia as probing molecules. When applied to the disproportionation of toluene on a fixed-bed reactor, the Al-MWW@B-MWW composite catalysts exhibited significantly enhanced para-xylene selectivity in comparison with normal MCM-22 and its physical mixture with B-MWW. Al-MWW@B-MWW's unique catalytic behaviors were ascribed to an effective suppression of para-xylene isomerization as a result of removal of non-shape-selective acid sites on the external surface.
机译:通过在预制的MCM-22铝硅酸盐上同晶过量生长的硼硅酸盐水热合成了形状选择性的核/壳结构Al-MWW @ B-MWW复合催化剂。硼硅酸盐的二次生长明显增加了MCM-22的血小板微晶厚度,并使表面Si / Al比从16增加到222。吸附的2,6-二叔丁基吡啶的傅里叶变换红外光谱(FTIR)表明认为位于外表面的布朗斯台德酸位点实际上被生成的B-MWW层完全覆盖,而通道中的那些酸位点仍可通过使用吡啶或氨作为探测分子来访问和检测到。当应用于固定床反应器中甲苯的歧化反应时,与常规MCM-22及其与B-MWW的物理混合物相比,Al-MWW @ B-MWW复合催化剂表现出显着增强的对二甲苯选择性。 Al-MWW @ B-MWW的独特催化行为归因于有效抑制对二甲苯异构化的结果,这是由于去除了外表面的非形状选择性酸位。

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