Supported Ru catalysts have been often employed for hydrogen charge into liquid organic hydrogen carrier molecules (monobenzyltoluene in this work), and their catalytic performance largely depends upon physicochemical properties of the support materials. We prepared supported Ru catalysts on SiO2-ZrO2 with different Si/(Si+Zr) ratios ranging from 0 to 30mol% by loading Ru3(CO)12 onto Si,Zr-mixed metal hydroxide and subsequent thermolysis. The textural properties, Ru particle size, and hydrogenation activity of Ru/SiO2-ZrO2 catalysts show a volcano-shaped dependence on the content of Si added, where the maximum is achieved at the Si/(Si+Zr) ratio of 5 mol%. Up to this Si content the incorporation of Si into ZrO2 improves thermal stability and decreases the particle size of tetragonal ZrO2, resulting in a positive contribution to hydrogen storage efficiency. However, the further addition of Si increases surface heterogeneity and charge imbalance, and hence induces a decrease in the density of surface OH group reacting with Ru3(CO)12, which explains the lowered activity. Therefore, the addition of up to 5 mol% Si into ZrO2 is effective in enhancing the hydrogenation performance of Ru/ZrO2 owing to the improved textural properties and smaller Ru particles.

中文翻译：

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在不同 Si/Zr 比的 SiO2-ZrO2 混合氧化物负载的 Ru 催化剂上将氢储存到单苄基甲苯中

负载的 Ru 催化剂经常用于将氢充入液态有机氢载体分子（本工作中的单苄基甲苯），其催化性能在很大程度上取决于载体材料的物理化学性质。我们通过将 Ru3(CO)12 负载到 Si、Zr 混合金属氢氧化物上并随后进行热分解，在 SiO2-ZrO2 上制备了负载 Ru 催化剂，其 Si/(Si+Zr) 比范围为 0 到 30mol%。Ru/SiO2-ZrO2 催化剂的结构特性、Ru 粒径和加氢活性对添加的 Si 含量呈火山形依赖性，其中在 Si/(Si+Zr) 比为 5 mol% 时达到最大值. 达到此 Si 含量，将 Si 掺入 ZrO2 可提高热稳定性并降低四方 ZrO2 的粒径，从而对储氢效率做出积极贡献。然而，进一步添加 Si 会增加表面异质性和电荷不平衡，从而导致与 Ru3(CO)12 反应的表面 OH 基团的密度降低，这解释了活性降低。因此，在 ZrO2 中加入高达 5 mol% 的 Si 可以有效地提高 Ru/ZrO2 的氢化性能，因为它改善了结构特性和更小的 Ru 颗粒。