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Ceria-zirconia modified MnOx catalysts for gaseous elemental mercury oxidation and adsorption

机译：Ceria-zirconia修改MnOx气态的催化剂汞元素氧化和吸附

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摘要

A series of MnOx/CeO2 (Mn/Ce), MnOx/ZrO2 (Mn/Zr), and MnOx/Ce0.75Zr0.25O2 (Mn/CZ) catalysts prepared by an impregnation method were tested for their ability to catalyse the oxidation of Hg-0 at relatively low temperature (423 K). Various characterization techniques, namely, Brunauer-Emmett-Teller (BET) surface area analysis, X-ray diffraction (XRD), Raman spectroscopy (RS), X-ray photoelectron spectroscopy (XPS), and H-2-temperature programmed reduction (H-2-TPR) were employed to understand the structural, surface, and redox properties of the prepared catalysts. Specific aspects of the catalysis of Hg-0 oxidation that were investigated included the influence of MnOx loading (5, 15, and 25%) and the influence of HCl and O-2. Among the catalysts tested, the 15Mn/CZ catalyst achieved the best Hg-0 oxidation performance (similar to 83% conversion of Hg-0 to Hg2+) in the presence of HCl and O-2. The higher activity of the 15Mn/CZ catalyst was most likely due to the presence of more oxygen vacancies, enhanced Mn4+/Mn4+ + Mn3+ + Mn2+ ratio and more surface adsorbed oxygen, which were proved by XRD, BET, Raman, and XPS. H-2-TPR results also show that the strong interaction between the Ce0.75Zr0.25O2 support and MnOx improved the redox properties significantly as compared to pure CeO2 and ZrO2 supported MnOx catalysts.
机译：和MnOx / Ce0.75Zr0.25O2 (Mn / CZ)催化剂由一个浸渍方法进行测试催化氧化的能力Hg-0在相对较低温度(423 K)。各种表征技术,即Brunauer-Emmett-Teller(打赌)表面积分析、x射线衍射(XRD)、拉曼光谱学(RS), x射线光电子能谱(XPS)和H-2-temperature减少程序(H-2-TPR)了理解的结构,表面,氧化还原制备催化剂的性质。方面的Hg-0氧化的催化作用研究了包括MnOx的影响加载(5、15和25%)和盐酸的影响和0 2。达到最好的Hg-0氧化催化剂性能(类似于Hg-0转换成83%Hg2 +)在盐酸和0 2。活动的15 mn / CZ催化剂是最有可能的由于更多的氧空位的存在,增强Mn4 + - Mn4 + Mn3 +、Mn2 + ratio和更多表面吸附氧,证明XRD、打赌、拉曼和XPS。表明之间的强相互作用Ce0.75Zr0.25O2支持和MnOx改善了氧化还原性能明显比纯CeO2和锆支持MnOx催化剂。

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