Ru/WO3纳米催化剂的制备、表征及催化氨硼烷水解性能研究

Preparation, Characterization and Catalytic Performance of Ru/WO3 Nanocatalysts for Ammonia Borane Hydrolysis

  • 摘要: 通过直接焙烧钨酸铵制得WO3纳米粉体, 继而以其为载体, 采用吸附-化学还原工艺制备了一系列负载型Ru纳米催化剂。使用X-射线衍射、X-射线光电子能谱、拉曼光谱、扫描电镜、透射电镜等技术对所制催化剂进行了表征分析, 考察了它们对氨硼烷(AB)水解释氢反应的催化性能, 并进行了相应的动力学研究。结果表明, Ru最佳负载质量分数为2.0%。得益于多孔结构、WO3的氧缺陷及Ru纳米粒子的高分散, 所制最佳催化剂Ru/WO3呈现出优于诸多文献所报道的催化性能。在Ru/WO3催化作用下, 该水解反应对于Ru和反应底物浓度的反应级数分别为0.67和0.87级, 表观活化能为34.93 kJ/mol。在碱性溶液中, 相应的转化频率达到445.1 min-1

     

    Abstract: WO3 nano-powders are prepared via the direct calcination of ammonium tungstate and used as the supports to make a series of Ru nanoparticles (NPs) with an adsorption-chemical reduction strategy. The resulting catalysts are characterized by various techniques, such as X-ray diffraction, X-ray photoelectron spectroscopy, Raman spectroscopy, scanning electron microscopy and transmission electron microscopy. The catalytic performance of the obtained Ru NPs is assessed for the hydrolysis of ammonia borane (AB), and the corresponding reaction kinetics is explored. The results show that the optimal mass fraction of Ru loading is 2.0%. The excellent catalytic performance of Ru/WO3 catalysts is ascribed to the porous structure, oxygen deficiency of WO3 and high dispersion of Ru NPs. The reaction order of AB hydrolysis which catalyzed Ru/WO3 is 0.67 and 0.87 with respect to the concentration of Ru and AB, respectively, with apparent activation energy of 34.93 kJ/mol. Upon the addition of appropriate NaOH basic solution, the turnover frequency reaches to 445.1 min-1.

     

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