Car-Parrinello simulation of H2O dissociation on rutile

被引:100
作者
Langel, W [1 ]
机构
[1] Ernst Moritz Arndt Univ Greifswald, Inst Chem & Biochem, D-17489 Greifswald, Germany
关键词
chemisorption; computer simulations; models of surface kinetics; molecular dynamics; physical adsorption; titanium oxide; water;
D O I
10.1016/S0039-6028(01)01606-5
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
Chemisorption and physical adsorption of H2O at the (10 0) and (I 10) surfaces of the rutile modification of TiO2 have been studied using the Car-Parrinello method. Spontaneous dissociation was observed in the simulation when a water molecule was inserted into a vacancy on the partially reduced (10 0) surface. On the partially reduced (110) surface no spontaneous dissociation took place but hydroxylated configurations were stable. The perfect rutile surfaces adsorbed undissociated water forming a stable Ti-O bond and one hydrogen bond. When starting from two hydroxyl groups fast recombination was observed. The relaxation of the non-hydroxylated (11 0)-surface was studied by molecular dynamics and a soft surface phonon at 380 cm(-1) was found. (C) 2001 Elsevier Science B.V. All rights reserved.
引用
收藏
页码:141 / 150
页数:10
相关论文
共 45 条
[1]   Hartree-Fock periodic study of the chemisorption of small molecules on TiO2 and MgO surfaces [J].
Ahdjoudj, J ;
Markovits, A ;
Minot, C .
CATALYSIS TODAY, 1999, 50 (3-4) :541-551
[2]   First principles simulations of titanium oxide clusters and surfaces [J].
Albaret, T ;
Finocchi, F ;
Noguera, C .
FARADAY DISCUSSIONS, 1999, 114 :285-304
[3]   ELECTROCHEMICAL SYNTHESIS AND INSITU RAMAN-SPECTROSCOPY OF THIN-FILMS OF TITANIUM-DIOXIDE [J].
ARSOV, LD ;
KORMANN, C ;
PLIETH, W .
JOURNAL OF RAMAN SPECTROSCOPY, 1991, 22 (10) :573-575
[4]   The adsorption and dissociation of ROH molecules on TiO2(110) [J].
Bates, SP ;
Kresse, G ;
Gillan, MJ .
SURFACE SCIENCE, 1998, 409 (02) :336-349
[5]   A systematic study of the surface energetics and structure of TiO2(110) by first-principles calculations [J].
Bates, SP ;
Kresse, G ;
Gillan, MJ .
SURFACE SCIENCE, 1997, 385 (2-3) :386-394
[6]   DENSITY-FUNCTIONAL EXCHANGE-ENERGY APPROXIMATION WITH CORRECT ASYMPTOTIC-BEHAVIOR [J].
BECKE, AD .
PHYSICAL REVIEW A, 1988, 38 (06) :3098-3100
[7]   Relaxation of TiO2(110)-(1x1) using surface X-ray diffraction [J].
Charlton, G ;
Howes, PB ;
Nicklin, CL ;
Steadman, P ;
Taylor, JSG ;
Muryn, CA ;
Harte, SP ;
Mercer, J ;
McGrath, R ;
Norman, D ;
Turner, TS ;
Thornton, G .
PHYSICAL REVIEW LETTERS, 1997, 78 (03) :495-498
[8]   Evidence for oxygen adatoms on TiO2(110) resulting from O2 dissociation at vacancy sites [J].
Epling, WS ;
Peden, CHF ;
Henderson, MA ;
Diebold, U .
SURFACE SCIENCE, 1998, 412-13 :333-343
[9]   Potential energy surface for a seven-atom reaction.: Thermal rate constants and kinetic isotope effects for CH4+OH [J].
Espinosa-García, J ;
Corchado, JC .
JOURNAL OF CHEMICAL PHYSICS, 2000, 112 (13) :5731-5739
[10]  
Evarestov RA, 1997, PHYS STATUS SOLIDI B, V203, pR3, DOI 10.1002/1521-3951(199709)203:1<R3::AID-PSSB99993>3.0.CO