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支撑表面层对金纳米颗粒催化一氧化碳氧化活性的影响。

Effect of supporting surface layers on catalytic activities of gold nanoparticles in CO oxidation.

作者信息

Yan Wenfu, Mahurin Shannon M, Chen Bei, Overbury Steven H, Dai Sheng

机构信息

Chemical Sciences Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, USA.

出版信息

J Phys Chem B. 2005 Aug 18;109(32):15489-96. doi: 10.1021/jp052006m.

Abstract

The surfaces of fumed silica materials were modified with a surface sol-gel process for catalysis applications. This surface-modification approach allows not only a monolayer growth of TiO(2) or Al(2)O(3) but also a stepwise double-layer growth of TiO(2)/TiO(2), Al(2)O(3)/Al(2)O(3), TiO(2)/Al(2)O(3), or Al(2)O(3)/TiO(2) on the surfaces of the silica materials with a monolayer precision. XRD analyses revealed that the coated monolayers and double layers of TiO(2) and Al(2)O(3) were amorphous. Gold nanoparticles were successfully deposited on the above six surface-modified silica materials via a deposition-precipitation method. The catalytic activities of these six gold catalysts for CO oxidation are highly dependent on the structures of their surface monolayers or double layers. The gold catalyst supported on the silica material functionalized with a TiO(2) monolayer (Au/TiO(2)) is the most active in both as-synthesized and oxidized forms, while the gold catalyst supported on the silica material functionalized with an Al(2)O(3)/TiO(2) double layer (Au/Al(2)O(3)/TiO(2)/SiO(2)) is the most active in the reduced form among the six catalysts. Surprisingly, the gold catalyst supported on the silica material functionalized with a TiO(2)/Al(2)O(3) double layer (Au/TiO(2)/Al(2)O(3)/SiO(2)) has much less activity than Au/Al(2)O(3)/TiO(2)/SiO(2) under all various treatments, underscoring the sensitivity of the catalytic activity to the structure of the supporting surfaces.

摘要

采用表面溶胶 - 凝胶法对气相二氧化硅材料的表面进行改性,用于催化应用。这种表面改性方法不仅能使TiO(2)或Al(2)O(3)单层生长,还能在二氧化硅材料表面以单层精度逐步实现TiO(2)/TiO(2)、Al(2)O(3)/Al(2)O(3)、TiO(2)/Al(2)O(3)或Al(2)O(3)/TiO(2)的双层生长。X射线衍射分析表明,包覆的TiO(2)和Al(2)O(3)单层和双层均为非晶态。通过沉积沉淀法成功地在上述六种表面改性的二氧化硅材料上沉积了金纳米颗粒。这六种金催化剂对CO氧化的催化活性高度依赖于其表面单层或双层的结构。负载在TiO(2)单层功能化二氧化硅材料上的金催化剂(Au/TiO(2))在合成态和氧化态下均最具活性,而负载在Al(2)O(3)/TiO(2)双层功能化二氧化硅材料上的金催化剂(Au/Al(2)O(3)/TiO(2)/SiO(2))在六种催化剂中还原态下最具活性。令人惊讶的是,负载在TiO(2)/Al(2)O(3)双层功能化二氧化硅材料上的金催化剂(Au/TiO(2)/Al(2)O(3)/SiO(2))在所有不同处理条件下的活性都远低于Au/Al(2)O(3)/TiO(2)/SiO(2),这突出了催化活性对载体表面结构的敏感性。

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