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Templated Synthesis of Copper Modified Tin-Doped Ceria for Catalytic CO Oxidation
Topics in Catalysis ( IF 3.6 ) Pub Date : 2020-02-22 , DOI: 10.1007/s11244-020-01251-w
Igor Yu. Kaplin , Ekaterina S. Lokteva , Artem V. Tikhonov , Kirill A. Zhilyaev , Elena V. Golubina , Konstantin I. Maslakov , Alexey O. Kamaev , Oksana Ya. Isaikina

Ceria-tin (CS) oxide catalytic systems were synthesized using cetyltrimethylammonium bromide (CTAB) and Pluronic 123 (P123) templates and modified with CuOx using two techniques: the “one-pot” method (Cu addition during CS synthesis) and the post-impregnation (IM). The catalysts were tested in CO oxidation in the stoichiometric CO/O2 mixture balanced with He. XRD, TPR, Raman spectroscopy, XPS, N2 physisorption, H2-TPR, HR TEM and SEM–EDS were used for catalysts characterization. CS P123 showed better CO conversion than CS CTAB at 100–200 °C and lower at higher temperatures, due to higher defectiveness and oxygen mobility in CS CTAB. Modification with copper improves catalytic action of all catalysts at low temperatures, but to a different degree depending on modification technique and template type. Cu–CS CTAB prepared by the “one-pot” technique was much more efficient than its IM counterpart and both P123-templated catalysts. The best efficiency of Cu–CS CTAB results from the strongest interaction of Cu with CS to form CuCeSnOx which provides accessibility of Cu+ adsorption sites, and low stability of surface carbonate groups improving low-temperature efficiency. Cu–CS P123 IM efficiency decreases in the oxygen-enriched reaction mixture, the reasons are discussed in terms of the ratio between oxidation and reduction stage rates in MvK mechanism.



中文翻译:

铜修饰锡掺杂二氧化铈用于CO氧化的模板化合成

使用十六烷基三甲基溴化铵(CTAB)和Pluronic 123(P123)模板合成二氧化铈(CS)氧化物催化体系,并使用以下两种技术用CuO x进行修饰:“一锅法”(在CS合成过程中添加Cu)和后-浸渍(IM)。在与He平衡的化学计量CO / O 2混合物中的CO氧化中测试了催化剂。XRD,TPR,拉曼光谱,XPS,N 2物理吸附,H 2-TPR,HR TEM和SEM-EDS用于催化剂表征。CS P123在100–200°C时表现出比CS CTAB更好的CO转化率,在更高的温度下表现出更低的CO转化率,这是因为CS CTAB中的缺陷和氧气迁移率更高。用铜进行改性可改善所有催化剂在低温下的催化作用,但在不同程度上取决于改性技术和模板类型。通过“一锅法”技术制备的Cu-CS CTAB比其IM对应物和两种P123模板催化剂的效率要高得多。Cu-CS CTAB的最佳效率是由于Cu与CS最强的相互作用形成了CuCeSnO x,从而提供了Cu +吸附位和表面碳酸酯基团的低稳定性提高了低温效率。在富氧反应混合物中,Cu–CS P123 IM效率降低,原因是根据MvK机理中氧化速率与还原级速率之比来讨论的。

更新日期:2020-02-22
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