CeO2(111)和CeO2(100)的界面调控合成及在Pt(111)上的结构转变

doi:10.1016/S1872-2067(18)63171-7

催化学报 ›› 2019, Vol. 40 ›› Issue (2): 204-213.DOI: 10.1016/S1872-2067(18)63171-7

CeO₂(111)和CeO₂(100)的界面调控合成及在Pt(111)上的结构转变

张毅^a,c, 冯卫^b, 杨帆^a, 包信和^a

a 中国科学院大连化学物理研究所催化基础国家重点实验室, 辽宁大连 116023;
b 表面物理与化学重点实验室, 四川江油 621908;
c 中国科学院大学, 北京 100049

收稿日期:2018-08-12 修回日期:2018-09-18 出版日期:2019-02-28 发布日期:2019-01-11
通讯作者: 杨帆, 包信和
基金资助:
国家重点研发计划（2017YFB0602205，2016YFA0202803，2017YFA0303104）；中国科学院战略性先导科技专项（XDB17020200）；国家自然科学基金（21473191，91545204）.

Interface-controlled synthesis of CeO₂(111) and CeO₂(100) and their structural transition on Pt(111)

Yi Zhang^a,c, Wei Feng^b, Fan Yang^a, Xinhe Bao^a

a State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, Liaoning, China;
b Science and Technology on Surface Physics and Chemistry Laboratory, Jiangyou 621908, Sichuan, China;
c University of Chinese Academy of Sciences, Beijing 100049, China

Received:2018-08-12 Revised:2018-09-18 Online:2019-02-28 Published:2019-01-11
Contact: 10.1016/S1872-2067(18)63171-7
Supported by:
This work was supported by the National Key R&D Program of China (2017YFB0602205, 2016YFA0202803, 2017YFA0303104), the Strategic Priority Research Program of the Chinese Academy of Sciences (XDB17020200), and the National Natural Science Foundation of China (21473191, 91545204).

摘要/Abstract

摘要：

氧化铈基催化材料在催化反应中存在显著的晶面效应，为了在分子尺度上理解其催化化学，需要可控合成具有明确表面结构的氧化铈.因此，我们研究了Pt（111）上氧化铈纳米结构和薄膜的生长.人们通常使用金属-氧化物之间的强相互作用来解释Pt/CeO_x催化剂上的催化过程，然而对于Pt与CeO_x之间的强相互作用仍旧缺乏原子尺度上的了解.我们的结果表明，Pt与氧化铈之间的相互作用可以影响氧化铈的表界面结构，这可能会进而影响Pt/CeO_x催化剂的性质.
在Pt（111）上生长的氧化铈薄膜通常暴露CeO₂（111）表面.我们发现Pt（111）表面厚度在三层以内的氧化铈薄膜，其结构是高度动态且随着退火温度升高而变化的，这种动态结构变化可归因于Pt和氧化铈间的界面电子作用.当氧化铈薄膜的厚度增大到三层以上，其负载的氧化铈团簇开始表现出迥异于三层以下氧化铈纳米岛的优异的热稳定性，表明Pt与CeO_x之间的界面电子作用主要影响厚度在三层以内的氧化铈纳米结构.采用常规的反应沉积方法难以获得完全覆盖Pt（111）衬底的规整氧化铈薄膜，而我们通过采取一种两步的动力学限制生长方法，制备出了完全覆盖Pt（111）衬底的氧化铈薄膜.对于Pt（111）上厚度约为3-4层的氧化铈薄膜，在超高真空中于1000K退火会导致氧化铈薄膜表面形成CeO₂（100）结构.这是因为高温还原促进了c-Ce₂O₃（100）缓冲层的形成，该缓冲层被Pt的界面电子转移以及相匹配的超晶格所稳定，并进一步成为顶层CeO₂（100）结构生长的模板.进一步在900 K的氧气中处理则可将薄膜CeO₂（100）表面完全转变为CeO₂（111）表面.
因此，Pt（111）上氧化铈纳米岛和薄膜所展现的结构动态变化是由Pt-CeO_x界面作用与氧化铈层间作用相互竞争所决定.本研究提供了对氧化铈负载Pt催化剂的原子级理解，虽然Pt/CeO₂催化剂活性增强的原因常被简单归结于界面强相互作用，我们的研究在原子尺度上进一步表明Pt/CeO₂在还原条件下易形成界面Ce₂O₃层.此外，本研究提供了不同晶面二氧化铈模型催化剂的构筑方法，可将对氧化铈晶面效应和Pt/CeO_x催化剂的研究推进到分子尺度.

关键词: 界面作用, Pt/CeO_x催化剂, CeO₂(111), CeO₂(100), c-Ce₂O₃(100)

Abstract:

Ceria-based catalytic materials are known for their crystal-face-dependent catalytic properties. To obtain a molecular-level understanding of their surface chemistry, controlled synthesis of ceria with well-defined surface structures is required. We have thus studied the growth of CeO_x nanostructures (NSs) and thin films on Pt(111). The strong metal-oxide interaction has often been invoked to explain catalytic processes over the Pt/CeO_x catalysts. However, the Pt-CeO_x interaction has not been understood at the atomic level. We show here that the interfacial interaction between Pt and ceria could indeed affect the surface structures of ceria, which could subsequently determine their catalytic chemistry. While ceria on Pt(111) typically exposes the CeO₂(111) surface, we found that the structures of ceria layers with a thickness of three layers or less are highly dynamic and dependent on the annealing temperatures, owing to the electronic interaction between Pt and CeO_x. A two-step kinetically limited growth procedure was used to prepare the ceria film that fully covers the Pt(111) substrate. For a ceria film of~3-4 monolayer (ML) thickness on Pt(111), annealing in ultrahigh vacuum (UHV) at 1000 K results in a surface of CeO₂ (100), stabilized by a c-Ce₂O₃(100) buffer layer. Further oxidation at 900 K transforms the surface of the CeO₂(100) thin film into a hexagonal CeO₂(111) surface.

Key words: Interfacial interaction, Pt/CeO_x catalyst, CeO₂(111), CeO₂(100), c-Ce₂O₃(100)

张毅, 冯卫, 杨帆, 包信和. CeO₂(111)和CeO₂(100)的界面调控合成及在Pt(111)上的结构转变[J]. 催化学报, 2019, 40(2): 204-213.

Yi Zhang, Wei Feng, Fan Yang, Xinhe Bao. Interface-controlled synthesis of CeO₂(111) and CeO₂(100) and their structural transition on Pt(111)[J]. Chinese Journal of Catalysis, 2019, 40(2): 204-213.

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CeO₂(111)和CeO₂(100)的界面调控合成及在Pt(111)上的结构转变

Interface-controlled synthesis of CeO₂(111) and CeO₂(100) and their structural transition on Pt(111)

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