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被羰基镍污染的CO气体在Cu(111)表面的近常压吸附研究
崔义
中国科学院苏州纳米技术和纳米仿生研究所
摘要:
在含一氧化碳(CO)的催化反应中,挥发性羰基镍的形成是催化剂失活的原因之一。CO是模型催化中研究表面性质最常用的探针分子之一。在超高真空(UHV)实验条件下,直接使用高纯度CO几乎不存在羰基镍杂质的问题。但在近常压实验环境下(NAP),CO气体通过含镍的气路后,催化剂表面很容易出现羰基镍。本论文利用近常压技术手段如近常压X射线光电子能谱(NAP-XPS)和近常压扫描隧道显微镜(NAP-STM)研究了在超高真空(UHV)和近常压条件下,被羰基镍污染的CO气体在Cu(111)表面的吸附过程。通过控制被污染CO的气体压力,可以在Cu(111)表面上形成Ni-Cu双金属催化剂。此外,我们探索了CO在所形成的Ni-Cu双金属表面上的吸附和解离过程,并报道了几种CO的高压吸附相结构。这项工作有助于理解室温下羰基镍与 Cu(111) 的相互作用机制,并提醒科研工作者在进行近常压实验时要考虑到CO分子被羰基镍污染的问题。
关键词:  羰基镍  一氧化碳  Cu(111)  近常压X射线光电子能谱  近常压扫描隧道显微镜
DOI:
分类号:
基金项目:
Near Ambient Pressure Adsorption of Nickel Carbonyl Contaminated CO on Cu(111) Surface
Yi Cui
Suzhou Institute of Nano-Tech and Nano-Bionics, Chinese Academy of Sciences
Abstract:
Formation of volatile nickel carbonyls with CO in catalytic reaction is one of the mechanisms of catalyst deactivation. CO is one of the most popular probe molecules to study the surface properties in model catalysis. In ultra-high vacuum (UHV) conditions, the problem of nickel carbonyl impurity almost does not exist in case a high purity of CO is used directly. While in the near ambient pressure (NAP) range, nickel carbonyl is easily found on the surface by passing through the Ni containing tubes. Here, the NAP techniques such as NAP-X-ray photoelectron spectroscopy (XPS) and NAP-scanning tunneling microscopy (STM) are used to study the adsorption of nickel carbonyl contaminated CO gas on Cu(111) surface in UHV and NAP conditions. By controlling the pressure of contaminated CO, the Ni-Cu bimetallic catalyst can form on Cu(111) surface. Furthermore, we investigated the process of CO adsorption and dissociation on the formed Ni-Cu bi-metal surface, and several high-pressure phase of CO structures were reported. This work contributes to understanding the interaction of nickel carbonyl with Cu(111) at room temperature, and reminds the consideration of CO molecules contaminated by nickel carbonyl especially in the NAP range study.
Key words:  nickel carbonyl  carbon monoxide  Cu(111)  NAP-XPS  NAP-STM