Adsorption and dissociation of molecular hydrogen on Pt/CeO2 catalyst in the hydrogen spillover process: A quantum chemical molecular dynamics study

被引：21

作者：

Ahmed, Farouq ^{[1
]}

Alam, Md. Khorshed ^{[3
]}

Muira, Ryuji ^{[3
]}

Suzuki, Ai ^{[2
]}

Tsuboi, Hideyuki ^{[1
]}

Hatakeyama, Nozomu ^{[1
]}

Endou, Akira ^{[1
]}

Takaba, Hiromitsu ^{[3
]}

Kubo, Momoji ^{[4
]}

Miyamoto, Akira ^{[1
,2
,3
]}

机构：

[1] Tohoku Univ, Grad Sch Engn, Dept Appl Chem, Sendai, Miyagi 9808579, Japan

[2] Tohoku Univ, New Ind Creat Hatchery Ctr, Sendai, Miyagi 9808579, Japan

[3] Tohoku Univ, Grad Sch Engn, Dept Chem Engn, Sendai, Miyagi 9808579, Japan

[4] Tohoku Univ, Grad Sch Engn, Fracture & Reliabil Res Inst, Sendai, Miyagi 9808579, Japan

来源：

APPLIED SURFACE SCIENCE | 2010年 / 256卷 / 24期

关键词：

Hydrogen spillover; Quantum chemical molecular dynamics; Catalyst surface; TOPOCHEMICAL HETEROGENEOUS CATALYSIS; SUPPORTED METAL-CATALYSTS; DENSITY-FUNCTIONAL THEORY; GAS-PHASE TRANSPORT; COMPUTATIONAL CHEMISTRY; OXYGEN SPILLOVER; PLATINUM; SURFACE; ALUMINA; ACCURATE;

D O I：

10.1016/j.apsusc.2010.06.021

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：

Ultra accelerated quantum chemical molecular dynamics method (UA-QCMD) was used to study the dynamics of the hydrogen spillover process on Pt/CeO2 catalyst surface for the first time. The direct observation of dissociative adsorption of hydrogen on Pt/CeO2 catalyst surface as well as the diffusion of dissociative hydrogen from the Pt/CeO2 catalyst surface was simulated. The diffusion of the hydrogen atom in the gas phase explains the high reactivity observed in the hydrogen spillover process. Chemical changes, change of adsorption states and structural changes were investigated. It was observed that parallel adsorption of hydrogen facilitates the dissociative adsorption leading to hydrogen desorption. Impact with perpendicular adsorption of hydrogen causes the molecular adsorption on the surface, which decelerates the hydrogen spillover. The present study also indicates that the CeO2 support has strong interaction with Pt catalyst, which may cause an increase in Pt activity as well as enhancement of the metal catalyst dispersions and hence increasing the rate of hydrogen spillover reaction. (C) 2010 Elsevier B.V. All rights reserved.

引用

页码：7643 / 7652

页数：10

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