Observation of a hydrogen-induced shape resonance on Pt/LTL catalysts and its relation with support acidity/alkalinity

被引:27
作者
Mojet, BL
Ramaker, DE
Miller, JT
Koningsberger, DC
机构
[1] Univ Utrecht, Debye Inst, Dept Inorgan Chem & Catalysis, NL-3508 TB Utrecht, Netherlands
[2] George Washington Univ, Dept Chem, Washington, DC 20052 USA
[3] George Washington Univ, Inst Mat Sci, Washington, DC USA
[4] Amoco Res Ctr, Naperville, IL 60656 USA
关键词
shape resonance; metal-support interaction; XAFS spectroscopy; Pt/LTL; Pt-H bonding; support acidity/alkalinity;
D O I
10.1023/A:1019018215806
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
A novel analysis method of the platinum L-3 and L-2 X-ray absorption edges of Pt/LTL catalysts indicates that chemisorbed hydrogen induces an antibonding resonance state just above the Fermi level at the Pt L-3 edge. The difference in energy of this antibonding state (E-res) with respect to the Fermi level is strongly influenced by the acidity/alkalinity of the LTL support: E-res decreases with increasing alkalinity. The decrease in E-res can also be correlated with the decrease of the neopentane hydrogenolysis turnover frequency of Pt/LTL with increasing support alkalinity. These results provide the most direct experimental evidence that the support acidity/alkalinity alters the actual chemical bond between the surface platinum atoms and the reacting molecule.
引用
收藏
页码:15 / 20
页数:6
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