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

[1] Study of Carbon Monoxide Oxidation on CeO2(111) Using Ultra Accelerated Quantum Chemical Molecular Dynamics [J].

Alam, Md. Khorshed ;

Ahmed, Farouq ;

Nakamura, Katsuyoshi ;

Suzuki, Ai ;

Sahnoun, Riadh ;

Tsuboi, Hideyuki ;

Koyama, Michihisa ;

Hatakeyama, Nozomu ;

Endou, Akira ;

Takaba, Hiromitsu ;

Del Carpio, Carlos A. ;

Kubo, Momoji ;

Miyamoto, Akira .

JOURNAL OF PHYSICAL CHEMISTRY C, 2009, 113 (18) :7723-7727

[2] Potential energy of H2 dissociation and adsorption on Pt(111) surface:: First-principles calculation [J].

Arboleda, Nelson B., Jr. ;

Kasai, Hideaki ;

Dino, Wilson A. ;

Nakanishi, Hiroshi .

JAPANESE JOURNAL OF APPLIED PHYSICS PART 1-REGULAR PAPERS BRIEF COMMUNICATIONS & REVIEW PAPERS, 2007, 46 (7A) :4233-4237

[3] STUDIES OF TOPOCHEMICAL HETEROGENEOUS CATALYSIS .3. CATALYSIS OF REDUCTION OF METAL-OXIDES BY HYDROGEN [J].

BATLEY, GE ;

EKSTROM, A ;

JOHNSON, DA .

JOURNAL OF CATALYSIS, 1974, 34 (03) :368-375

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

BAUMGARTEN, E ;

LENTESWAGNER, C ;

WAGNER, R .

JOURNAL OF CATALYSIS, 1989, 117 (02) :533-541

[5] REACTIVITY OF SPILLOVER HYDROGEN - REACTIVITY OF UNSATURATED-COMPOUNDS [J].

BAUMGARTEN, E ;

WAGNER, R ;

LENTESWAGNER, C .

JOURNAL OF CATALYSIS, 1987, 104 (02) :307-311

[6] HYDROGEN SPILLOVER THROUGH GAS-PHASE TRANSPORT OF HYDROGEN-ATOMS - REPLY [J].

BAUMGARTEN, E ;

LENTENSWAGNER, C ;

WAGNER, R .

JOURNAL OF CATALYSIS, 1990, 126 (01) :314-315

[7] FTIR INVESTIGATIONS ON THE INFLUENCE OF OXYGEN SPILLOVER ON THE OXIDATION RATE OF ADSORBED BENZOIC-ACID [J].

BAUMGARTEN, E ;

DEDEK, B .

JOURNAL OF MOLECULAR CATALYSIS, 1990, 62 (01) :37-44

[8] H-D EXCHANGE AND HYDROGEN SPILLOVER IN THE PD/SIO2 SYSTEM - KINETICS AND DETECTION OF HYDROGEN-ATOMS [J].

BAUMGARTEN, E ;

LENTESWAGNER, C ;

WAGNER, R .

JOURNAL OF MOLECULAR CATALYSIS, 1989, 50 (02) :153-165

[9] A MULTICENTER NUMERICAL-INTEGRATION SCHEME FOR POLYATOMIC-MOLECULES [J].

BECKE, AD .

JOURNAL OF CHEMICAL PHYSICS, 1988, 88 (04) :2547-2553

[10] DENSITY FUNCTIONAL CALCULATIONS OF MOLECULAR-BOND ENERGIES [J].

BECKE, AD .

JOURNAL OF CHEMICAL PHYSICS, 1986, 84 (08) :4524-4529

← 1 2 3 4 5 6 7 →