Pt(110)表面催化CO氧化反应原位研究

李昌; 蔡军; 杨甜; 韩永; 董乔; 李毅敏; 刘志

doi:10.11889/j.0253-3219.2018.hjs.41.120501

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Pt(110)表面催化CO氧化反应原位研究

核物理、交叉学科研究 | 更新时间：2021-05-19

- Pt(110)表面催化CO氧化反应原位研究
- In-situ studies of CO oxidation on Pt(110)
- 核技术 2018年41卷第12期文章编号：120501
- 作者机构：
  
  1.中国科学院上海微系统与信息技术研究所信息功能材料国家重点实验室上海 200050
  2.上海科技大学物质科学与技术学院上海 201210
  3.中国科学院大学北京 100049
- 作者简介：
  
  [ "李昌, 男, 1991年出生, 2014年毕业于西安电子科技大学, 现为硕士研究生, 研究领域为近常压光电子能谱", "LI Chang, male, born in 1991, graduated from Xidian University in 2014, master student, focusing on ambient pressure X-ray photoelectron spectroscopy" ]
  李毅敏, E-mail:liym1@shanghaitech.edu.cn
  刘志, E-mail:zliu2@mail.sim.ac.cn
- 基金信息：
  
  国家自然科学基金(11227902);上海市科学技术委员会(14520722100)
- DOI：10.11889/j.0253-3219.2018.hjs.41.120501
  中图分类号： O647
- 收稿日期：2018-09-04，
  
  修回日期：2018-10-11，
  
  纸质出版日期：2018-12-10
- 稿件说明：
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李昌, 蔡军, 杨甜, 等. Pt(110)表面催化CO氧化反应原位研究[J]. 核技术, 2018,41(12):120501

Chang LI, Jun CAI, Tian YANG, et al. In-situ studies of CO oxidation on Pt(110)[J]. Nuclear techniques, 2018, 41(12): 120501
李昌, 蔡军, 杨甜, 等. Pt(110)表面催化CO氧化反应原位研究[J]. 核技术, 2018,41(12):120501 DOI： 10.11889/j.0253-3219.2018.hjs.41.120501.

Chang LI, Jun CAI, Tian YANG, et al. In-situ studies of CO oxidation on Pt(110)[J]. Nuclear techniques, 2018, 41(12): 120501 DOI： 10.11889/j.0253-3219.2018.hjs.41.120501.

摘要

摘要CO氧化作为最重要的原型反应之一始终受到广泛关注，而Pt系金属表面催化CO氧化反应的机理目前仍存争议。为了研究Pt表面催化CO氧化反应的机理，借助近常压光电子能谱（Ambient Pressure X-ray Photoelectron Spectroscopy，APXPS）结合在线质谱（Mass Spectra，MS），原位分析了Pt（110）表面催化CO氧化反应过程中表面物种以及反应产物的变化。实验结果表明：Pt（110）表面催化CO氧化反应过程可以分为三个状态：1）低反应活性状态，Pt（110）表面CO中毒，CO

的产生速率很低；2）高反应活性状态，Pt（110）表面发生点火反应并伴随大量反应热的释放；3）传质速率限制的反应状态，Pt（110）表面O过量，反应速率受到CO扩散速率的限制。保持反应气体总压强为100 Pa，通过改变不同的CO和O

比例，发现Pt（110）表面催化CO氧化反应的点火温度随着CO含量的增加而升高。本工作对于理解Pt（110）表面催化CO氧化反应机理具有重要帮助，同时为进一步弄清催化反应的活性物种提供了基础。

Abstract

Background

CO oxidation is a very important prototypical reaction in heterogeneous process. The reaction mechanism of Pt-group metals under ultrahigh vacuum (UHV) conditions was studied in detail

and unambiguous evidence of Langmuir-Hinshelwood kinetics was found. However

the reaction mechanism of the Pt(110) surface under high pressure conditions was still controversial.

Purpose

This study aims to clarify the reaction mechanism and active sites of CO oxidation on Pt(110).

Methods

The oxidation of CO on Pt(110) surface was studied under total pressures up to 100 Pa in different CO:O

reaction mixtures. Surface species and composition of products were analyzed in situ by ambient pressure X-ray photoelectron spectroscopy (APXPS) and online gas analysis by mass spectra (MS).

Results

The process of CO oxidation on Pt(110) fell into three regimes:1) low active regime with CO poisoned Pt(110) surface and low CO

formation rate; 2) highly active regime with ignition reaction on Pt(110) surface companied by a large amount of heat release; 3) mass transfer rate limited regime

excessive O-rich Pt(110) surface

the CO

formation rate controlled by CO diffusion rate.

Conclusion

The active sites of CO oxidation reaction on Pt(110) surface are metallic Pt.

关键词

Keywords

references

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