Experimental and Theoretical Study of CO Oxidation on PdAu Catalysts with NO Pulse Effects

被引：14

作者：

Hao, Xianghong ^{[3
]}

Shan, Bin ^{[3
]}

Hyun, Jangsuk ^{[3
]}

Kapur, Neeti ^{[3
]}

Fujdala, Kyle ^{[3
]}

Truex, Timothy ^{[3
]}

Cho, Kyeongjae ^{[1
,2
,3
]}

机构：

[1] Univ Texas Dallas, Dept Mat Sci & Engn, Richardson, TX 75080 USA

[2] Univ Texas Dallas, Dept Phys, Richardson, TX 75080 USA

[3] Nanostellar Inc, Redwood City, CA 94063 USA

来源：

TOPICS IN CATALYSIS | 2009年 / 52卷 / 13-20期

关键词：

PdAu; CO oxidation; NO; DFT; CLOSE-PACKED TRANSITION; VINYL-ACETATE SYNTHESIS; METAL SURFACES; AU; TEMPERATURE; ADSORPTION; GOLD; ACETYLENE; KINETICS; PT(111);

D O I：

10.1007/s11244-009-9378-y

中图分类号：

O69 [应用化学];

学科分类号：

081704 ;

摘要：

The effect of NO on CO oxidation was studied for Pt, Pd and PdAu catalysts. It was found that NO inhibits significantly the CO oxidation reactivity on both Pt and Pd catalysts. On PdAu catalyst, however, the presence of NO resulted in an enhancement of CO oxidation activity. In order to gain an atomistic understanding of this effect, density-function theory (DFT) calculations were performed on the adsorption and reaction properties of NO and CO on these metal surfaces. We have identified that the inhibition effects on Pt and Pd catalysts are due to stronger NO binding, and that the enhanced reactivity on PdAu is due to the reduced NO oxidation barrier on PdAu leading to NO2 formation.

引用

页码：1946 / 1950

页数：5

共 25 条

[1] SURFACE-STRUCTURE AND REACTIVITY IN THE CYCLIZATION OF ACETYLENE TO BENZENE WITH PD OVERLAYERS AND PD/AU SURFACE ALLOYS ON AU(111) [J].

BADDELEY, CJ ;

ORMEROD, RM ;

STEPHENSON, AW ;

LAMBERT, RM .

JOURNAL OF PHYSICAL CHEMISTRY, 1995, 99 (14) :5146-5151

[2] SIZE EFFECT ON MELTING TEMPERATURE OF GOLD PARTICLES [J].

BUFFAT, P ;

BOREL, JP .

PHYSICAL REVIEW A, 1976, 13 (06) :2287-2298

[3] The nature of the active site for vinyl acetate synthesis over Pd-Au [J].

Chen, M. S. ;

Luo, K. ;

Wei, T. ;

Yan, Z. ;

Kumar, D. ;

Yi, C. -W. ;

Goodman, D. W. .

CATALYSIS TODAY, 2006, 117 (1-3) :37-45

[4] The promotional effect of gold in catalysis by palladium-gold [J].

Chen, MS ;

Kumar, D ;

Yi, CW ;

Goodman, DW .

SCIENCE, 2005, 310 (5746) :291-293

[5] A first principles analysis of CO oxidation over Pt and Pt66.7%Ru33.3% (111) surfaces [J].

Desai, S ;

Neurock, M .

ELECTROCHIMICA ACTA, 2003, 48 (25-26) :3759-3773

[6] Au, Pd (mono and bimetallic) catalysts supported on graphite using the immobilisation method - Synthesis and catalytic testing for liquid phase oxidation of glycerol [J].

Dimitratos, N ;

Porta, F ;

Prati, L .

APPLIED CATALYSIS A-GENERAL, 2005, 291 (1-2) :210-214

[7] Atomic and molecular adsorption on Pt(111) [J].

Ford, DC ;

Xu, Y ;

Mavrikakis, M .

SURFACE SCIENCE, 2005, 587 (03) :159-174

[8] CO adsorption on close-packed transition and noble metal surfaces:: trends from ab initio calculations [J].

Gajdos, M ;

Eichler, A ;

Hafner, J .

JOURNAL OF PHYSICS-CONDENSED MATTER, 2004, 16 (08) :1141-1164

[9] Improved adsorption energetics within density-functional theory using revised Perdew-Burke-Ernzerhof functionals [J].

Hammer, B ;

Hansen, LB ;

Norskov, JK .

PHYSICAL REVIEW B, 1999, 59 (11) :7413-7421

[10] A kinetic study of vinyl acetate synthesis over Pd-based catalysts:: kinetics of vinyl acetate synthesis over Pd-Au/SiO2 and Pd/SiO2 catalysts [J].

Han, YF ;

Wang, JH ;

Kumar, D ;

Yan, Z ;

Goodman, DW .

JOURNAL OF CATALYSIS, 2005, 232 (02) :467-475

← 1 2 3 →