自组装低负载量Pd/γ-Al2O3催化剂催化氧化甲苯
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O643;X13;X51

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浙江省科技计划项目(2016C31104); 国家重点研发计划(2017YFC0210900)


A Self-assembled Pd/γ-Al2O3 Catalyst with Low Loading for Catalytic Oxidation of Toluene
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The Plan Projects of Science & Technology?in Zhejiang Province, China (2016C31104); The National Key Research and Development Program of China (2017YFC0210900).

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    摘要:

    以PdCl2和Pd2(dba)3为前驱体,通过浸渍法、沉积沉淀法和自组装法分别制备了负载量为0.03%(质量分数 )的Pd/γ-Al2O3-IM、Pd/γ-Al2O3-DP和Pd/γ-Al2O3-SA催化剂用于催化氧化甲苯。在甲苯体积分数为0.1%、空速(SV)为18000 mL/(g•h)条件下,Pd/γ-Al2O3-SA催化剂上甲苯实现98%转化率的温度(T98)为220 ℃,比Pd/γ-Al2O3-DP和Pd/γ-Al2O3-IM分别降低了40和75 ℃。通过N2吸附-脱附、XRD、TEM、XPS和H2-TPR对催化剂进行了表征。结果表明:自组装法制备的Pd/γ-Al2O3-SA催化剂的比表面积(345 m2/g)和孔体积(0.52 cm3/g)最大,Pd纳米粒子(Pd NPs)平均粒径(5.0 nm)最小,活性物种主要以PdO的形式高度分散于载体γ-Al2O3表面。此外,PdO与载体γ-Al2O3之间的强相互作用(SMSI)促进了其催化氧化甲苯的活性。

    Abstract:

    Pd/γ-Al2O3-IM, Pd/γ-Al2O3-DP and Pd/γ-Al2O3-SA catalysts with 0.03 wt% Pd loading for catalytic oxidation of toluene were respectively prepared by the impregnation, deposition-precipition, and self-assembly methods using PdCl2 and Pd2(dba)3 as precursors. The temperature for conversion of 98% toluene (T98) over Pd/γ-Al2O3-SA catalyst was 220 ℃ under the conditions of toluene volume fraction at 0.1% and space velocity (SV) at 18000 mL/(g•h), which was 40 and 75 ℃ lower than those of Pd/γ-Al2O3-DP and Pd/γ-Al2O3-IM. The catalysts were characterized by N2 adsorption-desorption, XRD, TEM, XPS, H2-TPR. The results indicated that Pd/γ-Al2O3-SA catalyst possessed the largest specific surface area (345 m2/g) and pore volume (0.52 cm3/g), the smallest average diameter (5.0 nm) of Pd nanopaticles (NPs), and the main active PdO species were well-dispersed on the surface of the γ-Al2O3 support. Besides, the strong metal-support interaction (SMSI) between PdO and γ-Al2O3 promoted its performance in catalytic oxidation of toluene.

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李奔,周贝,李思汉,严新焕.自组装低负载量Pd/γ-Al2O3催化剂催化氧化甲苯[J].精细化工,2018,35(9):

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  • 收稿日期:2017-10-07
  • 最后修改日期:2018-01-19
  • 录用日期:2018-02-01
  • 在线发布日期: 2018-08-08
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