Significant enhancement in water resistance of Pd/Al2O3 catalyst for benzene oxidation by Na addition
Significant enhancement in water resistance of Pd/Al2O3 catalyst for benzene oxidation by Na addition
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Na 添加显着增强 Pd/Al2O3 苯氧化催化剂的耐水性
DOI：
10.1016/j.cclet.2019.03.023
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发表时间：
2019-07
影响因子：
9.1
通讯作者：
邓华
中科院分区：
文献类型：
--
作者：
邓华
采用湿法浸渍法制备了一系列不同钠负载量的Na掺杂1 质量分数Pd/Al_2O_3催化剂，并考察了它们对苯的催化氧化性能。适量的Na对Pd/Al_2O_3催化剂的耐水性和低温活性的提高有显著的促进作用。最佳的Na/Pd摩尔比为1：1。用X-射线衍射仪、BET、透射电子显微镜、X-射线光电子能谱、O2-程序升温脱附、DIFTS等手段对催化剂进行了表征。结果表明，Na的加入不仅降低了催化剂上吸附的水物种的含量，而且增加了表面易吸氧物种的数量，这可能是催化剂具有良好的耐水性的关键因素。Na的加入也提高了晶格氧物种的迁移率，有利于催化活性。此外，Na1Pd1/Al_2O_3催化剂中分散良好的负电荷Pd粒子和合适的氧化还原性能也有助于提高催化剂的性能和耐水性。在此情况下，DRIFTS结果表明，苯通过中间体邻苯二酚物种被氧化为顺丁烯二酸酯和乙酸酯，最终生成无害的CO2和H2O。
A series of Na-doped 1 wt% Pd/Al2O3catalysts with different Na loadings were prepared by wet impregnation and tested for the catalytic oxidation of benzene. Suitable addition of Na had a remarkable promotion effect on water resistance and enhancement of low temperature activity of Pd/Al2O3catalysts. The optimal mole ratio between Na and Pd was 1:1. The properties of the prepared catalysts were characterized by X-ray diffraction (XRD), Brunauer Emmett Teller (BET), transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS), O2-temperature-programmed desorption (O2-TPD), andin situDRIFTS. Results indicated that the addition of Na not only decreased the content of adsorbed water species but also increased the amount of liable surface oxygen species, which are likely the key factors for the excellent water resistance of the catalyst. Na addition also improved the mobility of the lattice oxygen species, which was favorable for catalytic activity. Moreover, the well-dispersed negatively charged Pd particles and suitable redox properties derived from Na addition also contributed to the improved performance and water resistance of the Na1Pd1/Al2O3catalyst.In situDRIFTS results revealed that benzene was oxidized to maleate and acetate speciesviaintermediate o-benzoquinone species, which finally turned into harmless CO2and H2O.
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