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首页> 外文期刊>Catalysis science & technology >Hydrocarboxylation of methanol to methyl acetate using rhodium and ruthenium nanoparticles supported on titanate nanotubes as catalysts: infrared spectroscopy study
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Hydrocarboxylation of methanol to methyl acetate using rhodium and ruthenium nanoparticles supported on titanate nanotubes as catalysts: infrared spectroscopy study

机译:Hydrocarboxylation of methanol to methyl acetate using rhodium and ruthenium nanoparticles supported on titanate nanotubes as catalysts: infrared spectroscopy study

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Titanate nanotubes (TiNT) were synthesized by the hydrothermal method and used as a support for Rh (Rh/TiNT) and Ru nanoparticles (Ru/TiNT). Both catalysts were found active in the gas-phase hydrocarboxylation of methanol with CO2 and H2 as reactants and methyl iodide as a promoter at 1 bar and 150 °C to produce methyl acetate (MA), the Rh/TiNT catalyst being more active in the reaction with a reaction rate of 0.698 molMA molRh−1 h−1 compared with 0.272 molMA molRu−1 h−1 for the Ru/TiNT catalyst. The structural, textural, and compositional properties of the supported metal catalysts were evaluated by N2 physisorption, X-ray diffraction (XRD), Raman spectroscopy, and transmission electron microscopy (TEM). Results of XRD and Raman spectroscopy demonstrated that TiNT consisted of a unique crystalline structure of trititanate (Na2Ti3O7), while the results of TEM confirmed the multilayer nanotubular morphology with an internal diameter of ∼3 nm. Also, the TEM analysis of Rh/TiNT and Ru/TiNT samples revealed small (∼1 nm) and highly dispersed metal particles. Infrared spectroscopy studies performed under reaction conditions allowed the identification of important surface species; in particular, Rh-acetyl species were proposed as key reaction intermediates. This work shows an interesting and promising heterogeneous route for the valorization of CO2 to produce a value-added compound under moderate conditions.
机译:合成的钛酸纳米管(色彩)水热法和用作对Rh的支持(Rh /色彩)和俄文纳米颗粒(俄文/色调)。催化剂被发现活跃在气相hydrocarboxylation CO2和H2的甲醇反应物和碘甲烷作为启动子在1酒吧和150°C生产乙酸甲酯(MA),Rh /色彩更活跃的催化剂0.698 molMA反应的反应速率molRh−1 h−1比0.272 molMA molRu−1 h−1俄文/色彩催化剂。结构和成分的属性支持金属催化剂被N2评估物理吸附、x射线衍射(XRD),拉曼光谱和透射电子显微镜(TEM)。光谱分析表明,色彩由trititanate独特的晶体结构(Na2Ti3O7),而透射电镜证实的结果一个多层nanotubular形态内部直径∼3海里。分析Rh /色彩和俄文/色彩显示样品小(∼1海里)和高分散的金属粒子。在反应条件下允许执行识别重要的表面物种;特别Rh-acetyl物种被提出关键中间体的反应。有趣和有前途的异构途径二氧化碳的稳定物价产生增值在温和的条件下复合。

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