Dynamics of Hydrogen Spillover on Pt/γ-Al2O3 Catalyst Surface: A Quantum Chemical Molecular Dynamics Study

被引：65

作者：

Ahmed, Farouq ^{[1
]}

Alam, Md Khorshed ^{[1
]}

Suzuki, Ai ^{[2
]}

Koyama, Michihisa ^{[3
]}

Tsuboi, Hideyuki ^{[1
]}

Hatakeyama, Nozomu ^{[1
]}

Endou, Akira ^{[1
]}

Takaba, Hiromitsu ^{[3
]}

Del Carpio, Carlos A. ^{[1
]}

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：

JOURNAL OF PHYSICAL CHEMISTRY C | 2009年 / 113卷 / 35期

关键词：

TOPOCHEMICAL HETEROGENEOUS CATALYSIS; DENSITY-FUNCTIONAL THEORY; GAS-PHASE TRANSPORT; SUPPORTED PLATINUM; OXYGEN SPILLOVER; ADSORPTION; ACCURATE; ENERGY; ATOMS; CHEMISORPTION;

D O I：

10.1021/jp903606e

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：

The hydrogen spillover mechanism has earned intensive interest in the past decades because it plays a vital role in emerging technologies for the reduction of NOx in automobile exhausts. Hydrogen spillover arises in hydrogen-catalyzed reactions on a supported metal catalyst. In the present study, we applied quantum chemical molecular dynamics (QCMD) to investigate the mechanism of the hydrogen spillover process on a Pt/gamma-Al2O3 catalyst surface for the first time. The direct observation of dissociative adsorption of hydrogen and diffusion of hydrogen on a Pt/gamma-Al2O3 catalyst surface were successfully investigated. The diffusion of the hydrogen atom in the gas phase explains the high reactivity observed in the hydrogen spillover mechanism.

引用

页码：15676 / 15683

页数：8

共 61 条

[51]

SERMON PA, 1973, CATAL REV, V8, P211

[52] Dynamics of Hydrogen Spillover on Carbon-Based Materials [J].

Sha, Xianwei ;

Knippenberg, M. Todd ;

Cooper, Alan C. ;

Pez, Guido P. ;

Cheng, Hansong .

JOURNAL OF PHYSICAL CHEMISTRY C, 2008, 112 (44) :17465-17470

[53] HYDROGEN SPILLOVER THROUGH GAS-PHASE TRANSPORT OF HYDROGEN-ATOMS - COMMENT [J].

SPENCER, MS ;

BURCH, R ;

GOLUNSKI, SE .

JOURNAL OF CATALYSIS, 1990, 126 (01) :311-313

[54] DIRECT OBSERVATION OF HYDROGEN SPILLOVER ON CARBON-SUPPORTED PLATINUM AND ITS INFLUENCE ON THE HYDROGENATION OF BENZENE [J].

SRINIVAS, ST ;

RAO, PK .

JOURNAL OF CATALYSIS, 1994, 148 (02) :470-477

[55]

TEICHNER SJ, 1993, STUD SURF SCI CATAL, V77, P27

[56] RECENT STUDIES IN HYDROGEN AND OXYGEN SPILLOVER AND THEIR IMPACT ON CATALYSIS [J].

TEICHNER, SJ .

APPLIED CATALYSIS, 1990, 62 (01) :1-10

[57] On the activation of Pt/Al2O3 catalysts in HC-SCR by sintering:: determination of redox-active sites using Multitrack [J].

Vaccaro, AR ;

Mul, G ;

Pérez-Ramírez, J ;

Moulijn, JA .

APPLIED CATALYSIS B-ENVIRONMENTAL, 2003, 46 (04) :687-702

[58] COMPUTER EXPERIMENTS ON CLASSICAL FLUIDS .I. THERMODYNAMICAL PROPERTIES OF LENNARD-JONES MOLECULES [J].

VERLET, L .

PHYSICAL REVIEW, 1967, 159 (01) :98-+

[59] ACCURATE SPIN-DEPENDENT ELECTRON LIQUID CORRELATION ENERGIES FOR LOCAL SPIN-DENSITY CALCULATIONS - A CRITICAL ANALYSIS [J].

VOSKO, SH ;

WILK, L ;

NUSAIR, M .

CANADIAN JOURNAL OF PHYSICS, 1980, 58 (08) :1200-1211

[60] CRYSTAL-FIELD SURFACE ORBITAL - BOND-ENERGY BOND-ORDER (CFSO-BEBO) MODEL FOR CHEMISORPTION - APPLICATION TO HYDROGEN ADSORPTION ON A PLATINUM (111) SURFACE [J].

WEINBERG, WH ;

MERRILL, RP .

SURFACE SCIENCE, 1972, 33 (03) :493-&

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