Finite Size Effects in Chemical Bonding: From Small Clusters to Solids

被引：236

作者：

Kleis, J. ^{[1
]}

Greeley, J. ^{[2
]}

Romero, N. A. ^{[3
]}

Morozov, V. A. ^{[3
]}

Falsig, H. ^{[1
]}

Larsen, A. H. ^{[1
]}

Lu, J. ^{[1
]}

Mortensen, J. J. ^{[1
]}

Dulak, M. ^{[1
]}

Thygesen, K. S. ^{[1
]}

Norskov, J. K. ^{[1
,4
,5
]}

Jacobsen, K. W. ^{[1
]}

机构：

[1] Tech Univ Denmark, Dept Phys, Ctr Atom Scale Mat Design, DK-2800 Lyngby, Denmark

[2] Argonne Natl Lab, Ctr Nanoscale Mat, Argonne, IL 60439 USA

[3] Argonne Natl Lab, Leadership Comp Facil, Argonne, IL 60439 USA

[4] SUNCAT Ctr Interface Sci & Catalysis, SLAC Natl Accelerator Lab, Menlo Pk, CA 94025 USA

[5] Stanford Univ, Dept Chem Engn, Stanford, CA 94305 USA

来源：

CATALYSIS LETTERS | 2011年 / 141卷 / 08期

关键词：

Nano-particle; Size effects; DFT; METAL NANOPARTICLES; GOLD CLUSTERS; CHEMISTRY;

D O I：

10.1007/s10562-011-0632-0

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：

We address the fundamental question of which size a metallic nano-particle needs to have before its surface chemical properties can be considered to be those of a solid, rather than those of a large molecule. Calculations of adsorption energies for carbon monoxide and oxygen on a series of gold nanoparticles ranging from 13 to 1,415 atoms, or 0.8-3.7 nm, have been made possible by exploiting massively parallel computing on up to 32,768 cores on the Blue Gene/P computer at Argonne National Laboratory. We show that bulk surface properties are obtained for clusters larger than ca. 560 atoms (2.7 nm). Below that critical size, finite-size effects can be observed, and we show those to be related to variations in the local atomic structure augmented by quantum size effects for the smallest clusters.

引用

页码：1067 / 1071

页数：5

共 27 条

[1]

Bader R. F. W., 1994, ATOMS MOL QUANTUM TH

[2] PROJECTOR AUGMENTED-WAVE METHOD [J].

BLOCHL, PE .

PHYSICAL REVIEW B, 1994, 50 (24) :17953-17979

[3]

Bond GC, 1994, CATAL REV SCI ENG, V41, P319

[4] Oxidation-resistant gold-55 clusters [J].

Boyen, HG ;

Kästle, G ;

Weigl, F ;

Koslowski, B ;

Dietrich, C ;

Ziemann, P ;

Spatz, JP ;

Riethmüller, S ;

Hartmann, C ;

Möller, M ;

Schmid, G ;

Garnier, MG ;

Oelhafen, P .

SCIENCE, 2002, 297 (5586) :1533-1536

[5] Binding of propene on small gold clusters and on Au(111):: Simple rules for binding sites and relative binding energies [J].

Chrétien, S ;

Gordon, MS ;

Metiu, H .

JOURNAL OF CHEMICAL PHYSICS, 2004, 121 (08) :3756-3766

[6] Electronic structure calculations with GPAW: a real-space implementation of the projector augmented-wave method [J].

Enkovaara, J. ;

Rostgaard, C. ;

Mortensen, J. J. ;

Chen, J. ;

Dulak, M. ;

Ferrighi, L. ;

Gavnholt, J. ;

Glinsvad, C. ;

Haikola, V. ;

Hansen, H. A. ;

Kristoffersen, H. H. ;

Kuisma, M. ;

Larsen, A. H. ;

Lehtovaara, L. ;

Ljungberg, M. ;

Lopez-Acevedo, O. ;

Moses, P. G. ;

Ojanen, J. ;

Olsen, T. ;

Petzold, V. ;

Romero, N. A. ;

Stausholm-Moller, J. ;

Strange, M. ;

Tritsaris, G. A. ;

Vanin, M. ;

Walter, M. ;

Hammer, B. ;

Hakkinen, H. ;

Madsen, G. K. H. ;

Nieminen, R. M. ;

Norskov, J. K. ;

Puska, M. ;

Rantala, T. T. ;

Schiotz, J. ;

Thygesen, K. S. ;

Jacobsen, K. W. .

JOURNAL OF PHYSICS-CONDENSED MATTER, 2010, 22 (25)

[7] Reactions at surfaces: From atoms to complexity (Nobel lecture) [J].

Ertl, Gerhard .

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2008, 47 (19) :3524-3535

[8] 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

[9] NOVEL GOLD CATALYSTS FOR THE OXIDATION OF CARBON-MONOXIDE AT A TEMPERATURE FAR BELOW 0-DEGREES-C [J].

HARUTA, M ;

KOBAYASHI, T ;

SANO, H ;

YAMADA, N .

CHEMISTRY LETTERS, 1987, (02) :405-408

[10] Ammonia synthesis from first-principles calculations [J].

Honkala, K ;

Hellman, A ;

Remediakis, IN ;

Logadottir, A ;

Carlsson, A ;

Dahl, S ;

Christensen, CH ;

Norskov, JK .

SCIENCE, 2005, 307 (5709) :555-558

← 1 2 3 →