Ab initio calculations of adsorbate hydrogen-bond strength: Ammonia on Pt(111)

被引：32

作者：

Jennison, DR ^{[1
]}

Schultz, PA ^{[1
]}

Sears, MP ^{[1
]}

机构：

[1] SANDIA NATL LABS,DEPT PARALLEL COMPUTAT SCI 9225,ALBUQUERQUE,NM 87185

来源：

SURFACE SCIENCE | 1996年 / 368卷

关键词：

ammonia; chemisorption; density functional calculations; low index single crystal surfaces; platinum; surface structure; morphology; roughness; and topography;

D O I：

10.1016/S0039-6028(96)01058-8

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：

Seven-layer slab results for 1/4 monolayer of NH3 on Pt(111) (so called alpha-NH3) are compared with NH3 on a 91-atom Pt cluster; we find that the latter closely mimics the extended surface. The calculations predict atop site occupancy for alpha-NH3 with N-down. The H-bond between alpha-NH3 and an additional N-down molecule (beta-NH3) approaching from the gas-phase is then compared with that of two molecules in the gas phase; we discover the H-bond on the surface is almost three times stronger and the bond length appreciably shorter. Geometry relaxation then results in a 65+/-5 degree tilt of the beta-NH3 axis. Finally, slab calculations with 1/4 ML each of alpha- and beta-NH3 support this geometry over symmetrically coordinated beta-NH3 and predict an adsorption energy in good agreement with experiment.

引用

页码：253 / 257

页数：5

共 23 条

[11] INHOMOGENEOUS ELECTRON-GAS
RAJAGOPAL, AK
CALLAWAY, J
[J]. PHYSICAL REVIEW B, 1973, 7 (05) : 1912 - 1919
[12] CHEMISORBED-MOLECULE POTENTIAL-ENERGY SURFACES AND DIET PROCESSES
JENNISON, DR
STECHEL, EB
BURNS, AR
LI, YS
[J]. NUCLEAR INSTRUMENTS & METHODS IN PHYSICS RESEARCH SECTION B-BEAM INTERACTIONS WITH MATERIALS AND ATOMS, 1995, 101 (1-2) : 22 - 30
[13] MODIFIED BROYDEN METHOD FOR ACCELERATING CONVERGENCE IN SELF-CONSISTENT CALCULATIONS
JOHNSON, DD
[J]. PHYSICAL REVIEW B, 1988, 38 (18) : 12807 - 12813
[14] SELF-CONSISTENT EQUATIONS INCLUDING EXCHANGE AND CORRELATION EFFECTS
KOHN, W
SHAM, LJ
[J]. PHYSICAL REVIEW, 1965, 140 (4A): : 1133 - &
[15] EFFECTS OF BASIS SET AND ELECTRON CORRELATION ON THE CALCULATED PROPERTIES OF THE AMMONIA DIMER
LATAJKA, Z
SCHEINER, S
[J]. JOURNAL OF CHEMICAL PHYSICS, 1984, 81 (01) : 407 - 409
[16] LATAJKA Z, 1985, J CHEM PHYS, V84, P341
[17] THE ELECTRIC-DIPOLE MOMENT OF (NH3)2 FOR G - VERTICAL-BAR-K-VERTICAL-BAR=1
LINNARTZ, H
KIPS, A
MEERTS, WL
HAVENITH, M
[J]. JOURNAL OF CHEMICAL PHYSICS, 1993, 99 (04) : 2449 - 2452
[18] Lundqvist S., 1983, THEORY INHOMOGENEOUS
[19] ATOMS, MOLECULES, SOLIDS, AND SURFACES - APPLICATIONS OF THE GENERALIZED GRADIENT APPROXIMATION FOR EXCHANGE AND CORRELATION
PERDEW, JP
CHEVARY, JA
VOSKO, SH
JACKSON, KA
PEDERSON, MR
SINGH, DJ
FIOLHAIS, C
[J]. PHYSICAL REVIEW B, 1992, 46 (11): : 6671 - 6687
[20] SELF-INTERACTION CORRECTION TO DENSITY-FUNCTIONAL APPROXIMATIONS FOR MANY-ELECTRON SYSTEMS
PERDEW, JP
ZUNGER, A
[J]. PHYSICAL REVIEW B, 1981, 23 (10): : 5048 - 5079

← 1 2 3 →