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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
Received:04 September 2018,
Revised:11 October 2018,
Published:10 December 2018
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Chang LI, Jun CAI, Tian YANG, et al. In-situ studies of CO oxidation on Pt(110)[J]. Nuclear techniques, 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 DOI: 10.11889/j.0253-3219.2018.hjs.41.120501.
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
2
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
2
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。
Background
2
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
2
This study aims to clarify the reaction mechanism and active sites of CO oxidation on Pt(110).
Methods
2
The oxidation of CO on Pt(110) surface was studied under total pressures up to 100 Pa in different CO:O
2
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
2
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
2
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
2
formation rate controlled by CO diffusion rate.
Conclusion
2
The active sites of CO oxidation reaction on Pt(110) surface are metallic Pt.
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