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首页> 外文期刊>The journal of physical chemistry, C. Nanomaterials and interfaces >Formation of Subnanometer Zr-WOx Clusters within Mesoporous W-Zr Mixed Oxides as Strong Solid Acid Catalysts for Friedel-Crafts Alkylation
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Formation of Subnanometer Zr-WOx Clusters within Mesoporous W-Zr Mixed Oxides as Strong Solid Acid Catalysts for Friedel-Crafts Alkylation

机译：在中孔W-Zr混合氧化物中形成亚纳米Zr-WOx团簇，作为强固体酸催化剂用于Friedel-Crafts烷基化反应

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摘要

WO3—ZrO2 mixed metal oxides is an important class of acid solid. Here, we successfully synthesized a variety of mesoporous WO3—ZrO2 mixed metal oxides by a well-controlled sol—gel process (AcHE) using Zr(OBu)4 and WC16 as the inorganic precursors in the presence of poly block copolymer F127. Their structures and acid properties have been well characterized by XRD, Raman, N2 adsorption measurement, and HRTEM analyses. In addition, new insights from TG-DSC and ~(31)P NMR characterization also provide useful information on the formation of strong acidity of this important solid acid. Moreover, their structure-to-properties relationship has been studied in the Friedel—Crafts (F—C) reaction of anisole and benzyl alcohol. We identified that the subnanometer WOx clusters act as the most active sites for the F—C reaction. Most importantly, we show that the formation of these subnanometer WOx clusters can be rationally controlled. It is shown that a minimum W concentration (0.07 at the calcination temperature of 800 °C) and a minimum calcination temperature (650 °C at a given W concentration of 0.1) are required during the preparation of these acid catalysts for the development of highly active subnano WOx clusters.
机译：WO3-ZrO2混合金属氧化物是一类重要的酸性固体。在这里，我们在聚嵌段共聚物F127的存在下，使用Zr（OBu）4和WC16作为无机前体，通过良好控制的溶胶-凝胶工艺（AcHE）成功合成了各种介孔WO3-ZrO2混合金属氧化物。通过XRD，拉曼，N2吸附测量和HRTEM分析已经很好地表征了它们的结构和酸性质。此外，从TG-DSC和〜（31）P NMR表征获得的新见解也提供了有关此重要固体酸强酸性形成的有用信息。此外，在苯甲醚和苯甲醇的Friedel-Crafts（FC）反应中已经研究了它们的结构与性质的关系。我们发现亚纳米WOx簇是FC反应最活跃的位点。最重要的是，我们表明可以合理地控制这些亚纳米WOx簇的形成。结果表明，在这些酸催化剂的制备过程中，需要最低的W浓度（在800°C的煅烧温度下为0.07）和最低的煅烧温度（在给定的W浓度为0.1的情况下为650°C）来开发高度酸性的催化剂。活跃的亚纳米WOx簇。

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