Dynamic ion pairs in the adsorption of isolated water molecules on alkaline-earth oxide (001) surfaces

被引：69

作者：

Carrasco, Javier ^{[2
,3
,4
]}

Illas, Francesc ^{[2
,3
,4
]}

Lopez, Nuria ^{[1
]}

机构：

[1] Inst Chem Res Catalonia ICIQ, Tarragona 43007, Spain

[2] Univ Barcelona, Dept Quim Fis, E-08028 Barcelona, Spain

[3] Univ Barcelona, IRQTC, E-08028 Barcelona, Spain

[4] PCB, Barcelona 08028, Spain

来源：

PHYSICAL REVIEW LETTERS | 2008年 / 100卷 / 01期

关键词：

D O I：

10.1103/PhysRevLett.100.016101

中图分类号：

O4 [物理学];

学科分类号：

0702 ;

摘要：

Low coverage water adsorption on alkaline-earth oxides is studied by first principles methods and ab initio molecular dynamic simulations. On CaO and BaO(001), water dissociation is thermodynamically favored in contrast with the molecular adsorption found for MgO(001). On CaO(001), the barrier for water splitting is very small leading to a tight ion pair H-OH that exhibits a dynamic character with the hydroxyl group able to visit four equivalent adsorption sites while remaining attached to the proton. In contrast, ion pair separation is endothermic by 0.8 eV. These results are common to other basic surfaces such as BaO(001) and have important implications in the chemistry of partially hydroxylated oxide surfaces.

引用

页数：4

共 31 条

[1] Atomic resolution imaging of the (001) surface of UHV cleaved MgO by dynamic scanning force microscopy [J].

Barth, C ;

Henry, CR .

PHYSICAL REVIEW LETTERS, 2003, 91 (19) :196102/1-196102/4

[2] Metal oxide surfaces and their interactions with aqueous solutions and microbial organisms [J].

Brown, GE ;

Henrich, VE ;

Casey, WH ;

Clark, DL ;

Eggleston, C ;

Felmy, A ;

Goodman, DW ;

Grätzel, M ;

Maciel, G ;

McCarthy, MI ;

Nealson, KH ;

Sverjensky, DA ;

Toney, MF ;

Zachara, JM .

CHEMICAL REVIEWS, 1999, 99 (01) :77-174

[3] Novel water overlayer growth on Pd(111) characterized with scanning tunneling microscopy and density functional theory -: art. no. 116101 [J].

Cerdá, J ;

Michaelides, A ;

Bocquet, ML ;

Feibelman, PJ ;

Mitsui, T ;

Rose, M ;

Fomin, E ;

Salmeron, M .

PHYSICAL REVIEW LETTERS, 2004, 93 (11) :116101-1

[4]

Chizallet C, 2006, J PHYS CHEM B, V110, P15878, DOI 10.1021/jp0608401

[5] Density functional theory calculations of adsorption of water at calcium oxide and calcium fluoride surfaces [J].

de Leeuw, NH ;

Purton, JA ;

Parker, SC ;

Watson, GW ;

Kresse, G .

SURFACE SCIENCE, 2000, 452 (1-3) :9-19

[6] Observation of the dynamical change in a water monolayer adsorbed on a ZnO surface [J].

Dulub, O ;

Meyer, B ;

Diebold, U .

PHYSICAL REVIEW LETTERS, 2005, 95 (13)

[7] Water monolayers on MgO(100): structural investigations by LEED experiments, tensor LEED dynamical analysis and potential calculations [J].

Ferry, D ;

Picaud, S ;

Hoang, PNM ;

Girardet, C ;

Giordano, L ;

Demirdjian, B ;

Suzanne, J .

SURFACE SCIENCE, 1998, 409 (01) :101-116

[8] Interaction of a water molecule with the oxygen vacancy on the MgO(100) surface [J].

Finocchi, F ;

Goniakowski, J .

PHYSICAL REVIEW B, 2001, 64 (12)

[9] Partial dissociation of water molecules in the (3 x 2) water monolayer deposited on the MgO (100) surface [J].

Giordano, L ;

Goniakowski, J ;

Suzanne, J .

PHYSICAL REVIEW LETTERS, 1998, 81 (06) :1271-1273

[10] A helium atom scattering study of the structure and phonon dynamics of the ice surface [J].

Glebov, A ;

Graham, AP ;

Menzel, A ;

Toennies, JP ;

Senet, P .

JOURNAL OF CHEMICAL PHYSICS, 2000, 112 (24) :11011-11022

← 1 2 3 4 →