不同形貌MnO2及其负载Au催化剂的制备与CO和甲苯催化氧化性能研究

Preparation of different morphologies of Au/α-MnO2 catalyst for oxidation of carbon monoxide and toluene

  • 摘要: 以高锰酸钾和(或)硫酸锰为锰源,分别采用水热法和PVA保护的硼氢化钠还原法,制备了一维纳米棒状、线状和管状xAu/MnO2(x为2%、4%、8%和10%)催化剂。一维棒状、线状和管状xAu/MnO2中的MnO2均为四方晶相α-MnO2,其α-MnO2样品的比表面积为48.4~114.0 m 2/g。棒状4%Au/α-MnO2的催化活性最好:在空速为20 000 mL/(g·h)的条件下,CO转化率达到50%和90%时的反应温度(T50%T90%)分别为11.4和16.3 ℃;氧化甲苯的T50%T90%分别为210和225 ℃。基于大量的表征结果和多组催化活性数据分析发现,棒状4%Au/α-MnO2催化剂催化活性最好的主要原因是其低温还原性能最好、吸附氧物种浓度较高、催化剂上的Au纳米粒子高度分散、Au纳米粒子与α-MnO2纳米棒之间有较强相互作用。

     

    Abstract: 1-D nanosized rod-like, wire-like, and tubular α-MnO2 (xAu/α-MnO2,x=2%,4%,8%,10%) were prepared using the hydrothermal and PVA-protected NaBH4 reduction methods at different temperatures with KMnO4 and/or MnSO4 as Mn source, respectively. It is shown that the α-MnO2 in xAu/α-MnO2 was tetragonal in crystal structure, surface area of α-MnO2 nanorods, nanowires, and nanotubes was in the range of 48.4-114.0 m 2/g. The 4%Au/α-MnO2 sample possessed the highest adsorbed oxygen species concentration and the best low-temperature reducibility, thus showing the highest catalytic activity: the T50% and T90% (temperatures required for achieving reactant conversions of 50% and 90%) were 11.4 and 16.3 ℃ for CO oxidation, and 210 and 225 ℃ for toluene oxidation at a space velocity of 20 000 mL/(g ·h), respectively. Based on the characterization results and activity data, it is concluded that the better low-temperature reducibility, higher oxygen adspecies concentration, highly dispersed Au NPs, and stronger interaction between Au NPs and MnO2 nanorods were the main factors influencing the catalytic performance of 4%Au/α-MnO2.

     

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