Well-dispersed palladium supported on ordered mesoporous Co3O4 for catalytic oxidation of o-xylene

Well-dispersed palladium supported on ordered mesoporous Co3O4 for catalytic oxidation of o-xylene
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有序介孔Co3O4负载分散良好的钯用于邻二甲苯的催化氧化

DOI:
10.1016/j.apcatb.2013.05.003
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发表时间:
2013-10-01
影响因子:
22.1
通讯作者:
He, Hong
He, Hong
中科院分区:
化学1区
文献类型:
--
作者:
Wang, Yafei;Zhang, Changbin;He, Hong

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以介孔SiO2(KIT-6)为硬模板,采用纳米浇铸法制备了有序介孔Co 3 O 4(3D)和Pd/Co 3 O 4(3D)。此外,通过在Co 3 O 4(3D)中后浸渍Pd来制备Pd/Co 3 O 4(3DL)作为参比。在150-300 ℃的温度范围内测试所有催化剂的邻二甲苯的总氧化。介孔Co_3O_4(3D)对邻二甲苯的催化氧化活性优于本体Co_3O_4(B)。对于Pd负载的样品,Pd/Co 3 O 4(3D)比Pd/Co 3 O 4(3DL)具有更高的活性。用BET、XRD、TEM、XPS、H2-TPR和XAFS等方法对催化剂进行了表征。表征结果表明,与后浸渍法制备的Pd/Co 3 O 4(3DL)相比,原位纳米浇铸法制备的Pd/Co 3 O 4(3D)具有更加有序的介观结构和更加均匀的PdO物种,从而具有优异的邻二甲苯氧化活性。此外,还证明了氧化态的Pd是邻二甲苯氧化的活性中心。(c)2013爱思唯尔有限公司版权所有。
Ordered mesoporous Co3O4(3D) and Pd/Co3O4(3D) were prepared by a nanocasting route using mesoporous silica (KIT-6) as a hard template. In addition, Pd/Co3O4(3DL) was prepared as a reference by post-impregnation of Pd in Co3O4(3D). All catalysts were tested for the total oxidation of o-xylene in the temperature range of 150-300 degrees C. The mesoporous Co3O4(3D) showed better activity than bulk Co3O4 (B) for o-xylene oxidation. As for Pd-loaded samples, Pd/Co3O4(3D) had much higher activity than Pd/Co3O4(3DL). These catalysts were characterized by BET, XRD, TEM, XPS, H-2-TPR and XAFS methods. The characterization results show that the Pd/Co3O4(3D) synthesized by in situ nanocasting presented a more ordered mesostructure and more well-dispersed PdO species than the Pd/Co3O4(3DL) prepared with the post-impregnation method, which account for its excellent activity for o-xylene oxidation. In addition, it was demonstrated that Pd in the oxidized state is the active site for o-xylene oxidation. (c) 2013 Elsevier B.V. All rights reserved.