Ni在ZrO<sub>2</sub>(111)薄膜表面的生长、电子结构及热稳定性

引用本文: 韩永, 徐倩, 鞠焕鑫, 朱俊发. Ni在ZrO₂(111)薄膜表面的生长、电子结构及热稳定性[J]. 物理化学学报, 2015, 31(11): 2151-2157. doi: 10.3866/PKU.WHXB201510083 shu

Citation: HAN Yong, XU Qian, JU Huan-Xin, ZHU Jun-Fa. Growth, Electronic Structure and Thermal Stability of Ni on ZrO₂(111) Thin Film Surfaces[J]. Acta Physico-Chimica Sinica, 2015, 31(11): 2151-2157. doi: 10.3866/PKU.WHXB201510083 shu

Ni在ZrO₂(111)薄膜表面的生长、电子结构及热稳定性

1.
中国科学技术大学, 国家同步辐射实验室和苏州纳米科技协同创新中心, 合肥 230029

通讯作者: 朱俊发

基金项目:
国家自然科学基金(U1232102, 21403205) (U1232102, 21403205)

国家重点基础研究发展规划项目(973) (2013CB834605)资助 (973) (2013CB834605)

摘要: 利用X射线光电子能谱、紫外光电子能谱和低能电子衍射研究了Ni纳米颗粒在ZrO₂(111)薄膜表面的生长模式、电子结构及热稳定性. ZrO₂(111)薄膜外延生长于Pt(111)单晶表面, 厚度约为3 nm. 结果表明, 当Ni气相沉积到ZrO₂(111)薄膜表面上时, 遵循Stranski-Krastanov生长模式, 即先二维生长至0.5 ML(monolayer),然后呈三维岛状生长. 随着覆盖度的减小, Ni 2p_3/2峰逐渐向高结合能位移. 利用俄歇参数法分析发现, 引起该峰向高结合能位移的主要原因来源于终态效应的贡献, 但在低的Ni覆盖度时, 也有部分初态效应的贡献, 说明Ni在ZrO₂表面初始生长时, 两者存在较强的界面相互作用, Ni向ZrO₂衬底传递电荷, 形成带部分正电荷的Ni_δ+.两种不同覆盖度(0.05和0.5 ML)的Ni/ZrO₂(111)模型催化剂热稳定性研究表明, 当温度升高时, Ni逐渐被氧化成Ni₂₊, 并伴随着向ZrO₂衬底的扩散. 本文从原子水平上认识了Ni与ZrO₂表面的相互作用和界面结构, 为理解实际ZrO₂担载的Ni催化剂结构提供了重要的依据.

关键词:

English

Growth, Electronic Structure and Thermal Stability of Ni on ZrO₂(111) Thin Film Surfaces

1.
National Synchrotron Radiation Laboratory and Collaborative Innovation Center of Suzhou Nano Science and Technology, University of Science and Technology of China, Hefei 230029, P. R. China

Corresponding author: 朱俊发

Received Date: 06 August 2015
Fund Project:
国家自然科学基金(U1232102, 21403205)

国家重点基础研究发展规划项目(973) (2013CB834605)资助

Abstract: The growth mode, electronic structure, and thermal stability of Ni nanoparticles on thin ZrO₂(111) film surfaces were investigated using X-ray photoelectron spectroscopy, ultraviolet photoelectron spectroscopy, and low-energy electron diffraction. Stoichiometric ZrO₂(111) thin films with thickness of 3 nm were epitaxially grown on a Pt(111) single-crystal surface. The results indicate that the growth of Ni vapor deposited on thin ZrO₂(111) films follows two-dimensional growth up to 0.5 ML (monolayer), followed by threedimensional growth (i.e., the Stranski-Krastanov growth mode). The Ni 2p_3/2 binding energy (BE) increases with decreasing Ni coverage. We used the Auger parameter method to differentiate the contributions to this BE shift from the initial-state and final-state effects. The main contribution to the Ni 2p core level BE shift is made by the final-state effect. However, at low Ni coverages, the initial-state effect also contributes. This suggests that at the initial stage of Ni growth on the ZrO₂(111) surface, Ni and ZrO₂ interact strongly, leading to charge transfer from Ni to the ZrO₂ substrate, with the appearance of partially positively charged Ni_δ+. Thermal stability studies of Ni/ZrO₂(111) model catalysts with two different coverages (0.05 and 0.5 ML) indicate further oxidation of Ni to Ni₂₊ and concurrent diffusion of Ni into the ZrO₂ substrate at elevated temperatures. These findings provide an atomic-level fundamental understanding of the interactions between Ni with ZrO₂, which is essential for identifying the structures of real ZrO₂-supported Ni catalysts.

Key words:

Nickel
/ Zirconia
/ Model catalyst
/ X-ray photoelectron spectroscopy
/ Ultraviolet photoelectron spectroscopy

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沈阳化工大学材料科学与工程学院沈阳 110142

Ni在ZrO₂(111)薄膜表面的生长、电子结构及热稳定性

通讯作者: 朱俊发

English

Growth, Electronic Structure and Thermal Stability of Ni on ZrO₂(111) Thin Film Surfaces

Corresponding author: 朱俊发

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通讯作者: 陈斌, bchen63@163.com

中国化学会秘书处

Ni在ZrO2(111)薄膜表面的生长、电子结构及热稳定性

通讯作者: 朱俊发

English

Growth, Electronic Structure and Thermal Stability of Ni on ZrO2(111) Thin Film Surfaces

Corresponding author: 朱俊发

CCS Chemistry：嵌段共聚物自组装成 “三明治”二维有机材料，实现纳米级压力传感功能

CCS Chemistry：颜徐州、鲍哲南： 你的皮肤可能是一片SPMs

CCS Chemistry：工作高效不疲劳，只须让催化剂动起来

CCS Chemistry：静电组装导向聚合- 聚电解质纳米凝胶量化制备新策略

CCS Chemistry：金黄色葡萄球菌醛基脱氢酶是如何识别特异性底物的？

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通讯作者: 陈斌, bchen63@163.com

中国化学会秘书处

Ni在ZrO₂(111)薄膜表面的生长、电子结构及热稳定性

Growth, Electronic Structure and Thermal Stability of Ni on ZrO₂(111) Thin Film Surfaces

CCS Chemistry：颜徐州、鲍哲南：你的皮肤可能是一片SPMs