Ab initio study of HCl and HF interaction with crystalline ice.: I.: Physical adsorption

被引:70
作者
Bussolin, G [1 ]
Casassa, S [1 ]
Pisani, C [1 ]
Ugliengo, P [1 ]
机构
[1] Univ Turin, Dept Inorgan Phys & Mat Chem, I-10125 Turin, Italy
关键词
D O I
10.1063/1.475340
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
A quantum-mechanical ab initio study is presented concerning the physisorption of HCl and HF on ice surfaces, modeled with periodic, proton-ordered thin films. Three methods are adopted: (1) Periodic two-dimensional calculations concerning ice surfaces, both clean and covered with ordered overlayers; (2) embedded cluster calculations, concerning two-dimensional ordered structures interacting with a single molecule; (3) molecular:cluster calculations, simulating a portion of the surface. The combined and interactive use of these techniques has permitted us to recognize some deficiencies of molecular cluster models of ice and to correct for them. The energy of physisorption of HCl on a perfect basal surface of ice is estimated to be about 8 kcal/mol, on prismatic faces about 11 kcal/mol. Adsorption energies of HF are larger by 4 to 5 kcal/mol. (C) 1998 American Institute of Physics.
引用
收藏
页码:9516 / 9528
页数:13
相关论文
共 60 条
[1]   CALCULATION OF SMALL MOLECULAR INTERACTIONS BY DIFFERENCES OF SEPARATE TOTAL ENERGIES - SOME PROCEDURES WITH REDUCED ERRORS [J].
BOYS, SF ;
BERNARDI, F .
MOLECULAR PHYSICS, 1970, 19 (04) :553-&
[2]  
BUSSOLIN G, 1997, TESI LAUREA
[3]   Proton-ordered models of ordinary ice for quantum-mechanical studies [J].
Casassa, S ;
Ugliengo, P ;
Pisani, C .
JOURNAL OF CHEMICAL PHYSICS, 1997, 106 (19) :8030-8040
[4]   CORRELATION CORRECTION TO THE HARTREE-FOCK TOTAL ENERGY OF SOLIDS [J].
CAUSA, M ;
DOVESI, R ;
PISANI, C ;
COLLE, R ;
FORTUNELLI, A .
PHYSICAL REVIEW B, 1987, 36 (02) :891-897
[5]   Uptake and interaction of HI on ice films [J].
Chu, LT ;
Chu, L .
JOURNAL OF PHYSICAL CHEMISTRY B, 1997, 101 (32) :6271-6275
[6]   UPTAKE OF HCL IN WATER ICE AND NITRIC-ACID ICE FILMS [J].
CHU, LT ;
LEU, MT ;
KEYSER, LF .
JOURNAL OF PHYSICAL CHEMISTRY, 1993, 97 (29) :7779-7785
[7]   Density functional study of hydrogen-bonded systems: Energetic and vibrational features of some gas-phase adducts of hydrogen fluoride [J].
Civalleri, B ;
Garrone, E ;
Ugliengo, P .
JOURNAL OF MOLECULAR STRUCTURE-THEOCHEM, 1997, 419 :227-238
[8]   Influence of surface defects on the adsorption of HCl on ice [J].
Clary, DC ;
Wang, LC .
JOURNAL OF THE CHEMICAL SOCIETY-FARADAY TRANSACTIONS, 1997, 93 (16) :2763-2767
[9]   Molecules on ice [J].
Clary, DC .
SCIENCE, 1996, 271 (5255) :1509-1509
[10]   TEMPERATURE-DEPENDENCE OF THE EQUILIBRIUM FORM OF ICE [J].
COLBECK, SC .
JOURNAL OF CRYSTAL GROWTH, 1985, 72 (03) :726-732