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用常压 X 射线光电子能谱研究介孔氧化铈中金属纳米团簇上的水汽变换反应。

Water-gas shift reaction on metal nanoclusters encapsulated in mesoporous ceria studied with ambient-pressure X-ray photoelectron spectroscopy.

机构信息

Department of Chemistry and Biochemistry, University of Notre Dame, Notre Dame, Indiana 46556, USA.

出版信息

ACS Nano. 2012 Oct 23;6(10):9305-13. doi: 10.1021/nn303901q. Epub 2012 Sep 21.

Abstract

Metal nanoclusters (Au, Pt, Pd, Cu) encapsulated in channels of mesoporous ceria (mp-CeO(2)) were synthesized. The activation energies of water-gas shift (WGS) reaction performed at oxide-metal interfaces of metal nanoclusters encapsulated in mp-CeO(2) (M@mp-CeO(2)) are lower than those of metal nanoclusters impregnated on ceria nanorods (M/rod-CeO(2)). In situ studies using ambient-pressure XPS (AP-XPS) suggested that the surface chemistry of the internal concave surface of CeO(2) pores of M@mp-CeO(2) is different from that of external surfaces of CeO(2) of M/rod-CeO(2) under reaction conditions. AP-XPS identified the metallic state of the metal nanoclusters of these WGS catalysts (M@mp-CeO(2) and M/rod-CeO(2)) under a WGS reaction condition. The lower activation energy of M@mp-CeO(2) in contrast to M/rod-CeO(2) is related to the different surface chemistry of the two types of CeO(2) under the same reaction condition.

摘要

介孔氧化铈(mp-CeO(2))中孔道内包裹的金属纳米团簇(Au、Pt、Pd、Cu)被成功合成。在介孔氧化铈(mp-CeO(2))中包裹的金属纳米团簇(M@mp-CeO(2))的氧化物-金属界面上进行水煤气变换(WGS)反应的活化能低于浸渍在氧化铈纳米棒上的金属纳米团簇(M/rod-CeO(2))。原位使用常压 XPS(AP-XPS)研究表明,在反应条件下,M@mp-CeO(2)的 CeO(2) 孔内凹表面的表面化学性质与 M/rod-CeO(2) 的 CeO(2) 外表面不同。AP-XPS 确定了这些 WGS 催化剂(M@mp-CeO(2) 和 M/rod-CeO(2))在 WGS 反应条件下金属纳米团簇的金属态。与 M/rod-CeO(2) 相比,M@mp-CeO(2) 的较低活化能与相同反应条件下两种 CeO(2) 的不同表面化学性质有关。

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