Size-Dependent Oxidation State and CO Oxidation Activity of Tin Oxide Clusters,ACS Catalysis

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Size-Dependent Oxidation State and CO Oxidation Activity of Tin Oxide Clusters
ACS Catalysis ( IF 11.3 ) Pub Date : 2017-12-12 00:00:00 , DOI: 10.1021/acscatal.7b02981
Yusuke Inomata ₁ , Ken Albrecht _{1,

2} , Kimihisa Yamamoto _{1,

2}

Affiliation

The CO oxidation reaction is an industrially important reaction; however, the practical catalysts are limited to noble metals. In this paper, we report a systematic study of the CO oxidation ability on cheap and less noble tin oxide clusters with the aim of quantitatively understanding the active sites. We synthesized size-controlled tin oxide clusters in mesoporous silica using the dendrimer templating method, employing dendritic phenylazomethine with a tetraphenylmethane core (TPMG4) as the template molecule. The clusters had different sizes depending on the added amount of SnCl₂ as a precursor to TPMG4. The synthesized tin oxide clusters contained not only stable tetravalent Sn(IV) but also metastable divalent Sn(II) due to the structural stability and had a size-dependent composition. The CO oxidation activity of the tin oxide clusters increased with decreasing cluster size depending on the Sn(II)/Sn(IV) ratio. We also found the correlation between the Sn(II) fraction and the CO oxidation activity, clearly indicating that the partially reduced Sn(II) acted as the active site for the CO oxidation in the tin oxide clusters. This knowledge give a clue on how to design a highly active CO oxidation catalyst with base metal oxides.

中文翻译：

氧化锡团簇的尺寸依赖性氧化态和CO氧化活性

CO氧化反应是工业上重要的反应。然而，实际的催化剂仅限于贵金属。在本文中，我们报告了对廉价和较不贵的氧化锡簇上的CO氧化能力的系统研究，目的是定量了解活性位点。我们使用树枝状聚合物模板法，以具有四苯基甲烷核（TPMG4）的树枝状苯基偶氮甲胺为模板分子，在中孔二氧化硅中合成了尺寸可控的氧化锡簇。簇的大小取决于SnCl ₂的添加量作为TPMG4的前身。合成的氧化锡簇由于结构稳定性而不仅包含稳定的四价Sn（IV），而且包含亚稳态的二价Sn（II），并且具有取决于尺寸的组成。氧化锡团簇的CO氧化活性随团簇尺寸的减小而增加，具体取决于Sn（II）/ Sn（IV）的比例。我们还发现了Sn（II）馏分与CO氧化活性之间的相关性，明确表明部分还原的Sn（II）充当了氧化锡簇中CO氧化的活性位点。该知识为如何设计具有贱金属氧化物的高活性CO氧化催化剂提供了线索。

更新日期：2017-12-12

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