Ice-catalyzed ionization of hydrochloric acid

被引:56
作者
Bolton, K
Pettersson, JBC
机构
[1] Univ Coll Boras, Sch Engn, SE-50190 Boras, Sweden
[2] Univ Gothenburg, Dept Chem, SE-41296 Gothenburg, Sweden
关键词
D O I
10.1021/ja010096c
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Ionization of hydrochloric acid (HCl) on stratospheric ice particles is believed to be a key step in the depletion of stratospheric ozone. Ab initio calculations based on a model HCl-water cluster show that HCl ionization on ice surfaces is a barrierless process. Since this mechanism is rapid and produces chloride anions that are exposed to ambient stratospheric chlorine reservoir molecules, it is likely to be important for stratospheric chemistry. It complements a previously suggested mechanism where HCl forms part of the ice lattice before ionizing. The mechanism proposed here is also consistent with experimentally observed ionization of HCl on ice at low temperatures and under vacuum, where the HCl is not expected to be encapsulated in the ice lattice.
引用
收藏
页码:7360 / 7363
页数:4
相关论文
共 38 条
[1]   Molecular beam studies of HCl interactions with pure and HCl-covered ice surfaces [J].
Andersson, PU ;
Någård, MB ;
Pettersson, JBC .
JOURNAL OF PHYSICAL CHEMISTRY B, 2000, 104 (07) :1596-1601
[2]   Ab initio Monte Carlo simulated annealing study of HCl(H2O)n (n=3, 4) clusters [J].
Bacelo, DE ;
Binning, RC ;
Ishikawa, Y .
JOURNAL OF PHYSICAL CHEMISTRY A, 1999, 103 (24) :4631-4640
[3]   Surface sensitive studies of the reactive uptake of chlorine nitrate on ice [J].
Berland, BS ;
Tolbert, MA ;
George, SM .
JOURNAL OF PHYSICAL CHEMISTRY A, 1997, 101 (51) :9954-9963
[4]   Proton transfer reactions at the surface of ice. Heterogeneous reactions involved in stratospheric ozone depletion [J].
Bianco, R ;
Gertner, BJ ;
Hynes, JT .
BERICHTE DER BUNSEN-GESELLSCHAFT-PHYSICAL CHEMISTRY CHEMICAL PHYSICS, 1998, 102 (03) :518-526
[5]   Trapping-desorption and surface penetration of argon on ice [J].
Bolton, K ;
Pettersson, JBC .
CHEMICAL PHYSICS LETTERS, 1999, 312 (2-4) :71-76
[6]   A molecular dynamics study of the long-time ice Ih surface dynamics [J].
Bolton, K ;
Pettersson, JBC .
JOURNAL OF PHYSICAL CHEMISTRY B, 2000, 104 (07) :1590-1595
[7]   Ab initio study of HCl and HF interaction with crystalline ice.: I.: Physical adsorption [J].
Bussolin, G ;
Casassa, S ;
Pisani, C ;
Ugliengo, P .
JOURNAL OF CHEMICAL PHYSICS, 1998, 108 (22) :9516-9528
[8]  
Frisch M. J., 2016, Gaussian, V16
[9]   Ab initio study of HOCl, HCl, H2O, and Cl2 interacting with four water molecules [J].
Geiger, FM ;
Hicks, JM ;
de Dios, AC .
JOURNAL OF PHYSICAL CHEMISTRY A, 1998, 102 (09) :1514-1522
[10]   Molecular dynamics simulation of hydrochloric acid ionization at the surface of stratospheric ice [J].
Gertner, BJ ;
Hynes, JT .
SCIENCE, 1996, 271 (5255) :1563-1566