Structure Effects on Pyridine Hydrogenation over Pt(111) and Pt(100) Studied with Sum Frequency Generation Vibrational Spectroscopy

Structure Effects on Pyridine Hydrogenation over Pt(111) and Pt(100) Studied with Sum Frequency Generation Vibrational Spectroscopy
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DOI:
10.1007/s10562-010-0353-9
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发表时间:
2010-04
期刊:
影响因子:
2.8
通讯作者:
C. Kliewer;G. Somorjai
C. Kliewer;G. Somorjai
中科院分区:
化学4区
文献类型:
--
作者:
C. Kliewer;G. Somorjai

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摘要对铂(100)和铂(111)两种定义明确的铂单晶铂(100)加氢过程(10 Torr吡啶和100 Torr氢)进行了原位和频产生振动光谱研究。澄清了表面反应中间体。吡啶垂直吸附在两种晶体上,具有完整的芳环。在Pt(100)上观察到通过氮结合的1,4-二氢吡啶作为反应中间体,而在Pt(111)上没有检测到这一点。当晶体从300 K加热到350 K时,吡啶环平躺在催化剂表面。在铂(111)上,一个倾斜的哌啶产物与表面结合。在任何一个表面上都没有观察到环裂产物。图形抽象
AbstractSum frequency generation vibrational spectroscopy was applied in-situ during pyridine hydrogenation (10 Torr pyridine and 100 Torr hydrogen) over two well-defined platinum single crystals, Pt(100) and Pt(111). The surface reaction intermediates were clarified. Pyridine adsorbs to both crystals vertically, with in-tact aromatic ring. Over Pt(100) 1,4-dihydropyridine bound through the nitrogen was observed as a reaction intermediate, while over Pt(111) this was not detected. Upon heating the crystals from 300 to 350 K, the pyridine ring lies down flat on the catalyst surfaces. Over Pt(111) a tilted piperidine product is bound to the surface. Ring-cracking products were not observed over either surface.Graphical Abstract