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Ruthenium-oxo species with high oxidation performance supported on nano-scale particles prepared by the solvothermal reaction

溶剂热反应制备的纳米级颗粒负载具有高氧化性能的钌氧物种

基本信息

批准号：
18560739
负责人：
IMAMURA Seiichiro
金额：
$ 2.46万
依托单位：
Kyoto University
依托单位国家：
日本
项目类别：
Grant-in-Aid for Scientific Research (C)
财政年份：
2006
资助国家：
日本
起止时间：
2006 至 2007
项目状态：
已结题

项目摘要

In this work, we aimed at designing Ru species with Ru=O group which is highly dispersed on metal oxide supports prepared by the solvothermal reaction. This Ru species is expected to have peculiar and high activity for oxidation reactions. First, CeO_2 was employed as a support. The solvothermal reaction of Ce metal in 2-methoxy ethanol produced ultra fine CeO_2 colloidal particles whose average diameter was 2nm. The obtained CeO_2 colloidal solution was coagulated by various coagulants to produce CeO_2 powders. Their pore structures varied with the kinds of coagulants (NaOH, NH_4OH, Na_2CO_3, (NH_4)_2CO_3, NaHCO_3). The CeO_2 powders produced by using (NH_4)_2CO_3 and NaHCO_3 had macro and meso pores while those obtained with NaOH and NH_4OH had much micro pores. Ruthenium could be supported on the former CeO_2 in a well dispersed state but could not be supported in the micro-pore of the latter; thus, the former catalysts had higher activity in the oxidation of benzyl alcohol than the … More latter.The natures of the CeO_2 sample prepared by an ordinary precipitation method starting from aq. Ce(NO_3)_3 and the one prepared by starting from CeO_2 colloidal solution synthesized by the solvothermal method were compared. The solvothermal sample could be easily reduced and re-oxidized; it had larger amount of surface mobile oxygen than the precipitation sample. Consequently, the activity of the Ru supported on the solvothermal CeO_2 was much larger than that on the CeO_2 prepared by the precipitation method; indicating the excellence of the solvothermal method to prepare high performance ultra fine metal oxide particles.Various other supports were examined to obtain Ru species with Ru=O bond. The target supports to obtain the Ru species were ZrO_2, TbO_2, and Pr_6O_<11>. However, none of them were successful to produce this kind of Ru species. Conclusion of the present research is that the combination of Ru with CeO_2 is the sole and unique system to produce the finely dispersed Ru species with the Ru=O bond. The author expects the high potential of this catalyst to be used in various organic reactions. Less

在这项工作中，我们的目的是设计Ru物种与Ru=O基团，这是高度分散在金属氧化物载体制备的溶剂热反应。该Ru物种被预期具有独特的和高的氧化反应活性。首先，以CeO_2为载体。金属Ce在2-甲氧基乙醇中的溶剂热反应生成了平均粒径为2nm的超细CeO_2胶体颗粒。将所得CeO_2胶体溶液用不同的凝聚剂进行凝聚，得到CeO_2粉体。不同的混凝剂（NaOH、NH_4OH、Na_2CO_3、（NH_4）_2CO_3、NaHCO_3），其孔结构不同。用（NH_4）_2CO_3和NaHCO_3制备的CeO_2粉体具有大孔和中孔结构，而用NaOH和NH_4OH制备的CeO_2粉体具有较多的微孔结构。Ru以分散状态负载在CeO_2上，但不能负载在CeO_2的微孔中，因此前者催化剂对苯甲醇氧化的活性高于后者。 ...更多信息用普通沉淀法制备的CeO_2样品的性质与实验结果基本一致。比较了Ce（NO_3）_3和溶剂热法合成CeO_2胶体溶液制备的CeO_3/CeO_2纳米复合粉体。溶剂热样品易于还原和再氧化，表面移动的氧含量高于沉淀样品。结果表明，在溶剂热法制备的CeO_2上负载Ru的活性远高于沉淀法制备的CeO_2，表明溶剂热法是制备高性能超细金属氧化物颗粒的一种优越方法。以ZrO_2、TbO_2和Pr_6O_2为载体制备Ru物种<11>。然而，他们都没有成功地产生这种Ru物种。本研究的结论是，Ru与CeO_2的结合是产生具有Ru=O键的细分散Ru物种的唯一和独特的体系。作者期望该催化剂在各种有机反应中具有很高的应用潜力。少