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甲醇在 Pt/CeO2(111)/Cu(111)薄膜模型催化剂上的吸附与分解。

Methanol adsorption and decomposition on Pt/CeO2(111)/Cu(111) thin film model catalyst.

机构信息

Department of Surface and Plasma Science, Faculty of Mathematics and Physics, Charles University, 18000 Prague 8, Czech Republic.

出版信息

Langmuir. 2010 Aug 17;26(16):13333-41. doi: 10.1021/la101936b.

Abstract

Adsorption and desorption of methanol on Pt particles on a CeO(2)(111)/Cu(111) thin film surface and on an ion-eroded Pt(111) single crystal were investigated by X-ray photoelectron spectroscopy and soft X-ray synchrotron radiation photoelectron spectroscopy (PES). Resonant PES was used to determine the occupancy of the Ce 4f states with high sensitivity. Multilayers of methanol were adsorbed at low temperature and subsequently desorbed by heating to 600 K. Methanol desorption is accompanied by the formation of chemisorbed methoxy -OCH(3). Cerium oxide surface is strongly reduced by methanol, which was detected via the transition Ce(4+) --> Ce(3+) and an increase of the Ce 4f electronic state occupancy. Partial C-O bond scission and formation of atomic carbon was observed on the Pt particles as well as on the rough Pt(111) surface. On Pt/CeO(2)(111), all traces of surface carbon and residual hydrocarbons disappear at 500 K.

摘要

采用 X 射线光电子能谱和软 X 射线同步辐射光电子能谱(PES)研究了甲醇在 CeO(2)(111)/Cu(111)薄膜表面上的 Pt 颗粒和离子侵蚀的 Pt(111)单晶上的吸附和脱附。共振 PES 用于以高灵敏度确定 Ce 4f 态的占有率。在低温下吸附甲醇多层,然后通过加热至 600 K 脱附。甲醇脱附伴随着化学吸附甲氧基-OCH(3)的形成。CeO 表面被甲醇强烈还原,这通过 Ce(4+) → Ce(3+)的转变和 Ce 4f 电子态占有率的增加来检测。在 Pt 颗粒以及粗糙的 Pt(111)表面上观察到部分 C-O 键断裂和原子碳的形成。在 Pt/CeO(2)(111)上,所有表面碳和残余烃的痕迹在 500 K 时消失。

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