Electron-driven acid-base chemistry: Proton transfer from hydrogen chloride to ammonia

被引：72

作者：

Eustis, Soren N. ^{[1
]}

Radisic, Dunja ^{[1
]}

Bowen, Kit H. ^{[1
]}

Bachorz, Rafal A. ^{[2
,3
,4
]}

Haranczyk, Maciej ^{[4
,5
]}

Schenter, Gregory K. ^{[4
]}

Gutowski, Maciej ^{[4
,5
,6
]}

机构：

[1] Johns Hopkins Univ, Dept Chem, Baltimore, MD 21218 USA

[2] Univ Karlsruhe, CFN, D-76128 Karlsruhe, Germany

[3] Univ Karlsruhe, Inst Chem Phys, D-76128 Karlsruhe, Germany

[4] Pacific NW Natl Lab, Div Chem & Mat Sci, Richland, WA 99352 USA

[5] Univ Gdansk, Dept Chem, PL-80952 Gdansk, Poland

[6] Heriot Watt Univ, Dept Chem, Edinburgh EH14 4AS, Midlothian, Scotland

来源：

SCIENCE | 2008年 / 319卷 / 5865期

关键词：

D O I：

10.1126/science.1151614

中图分类号：

O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];

学科分类号：

07 ; 0710 ; 09 ;

摘要：

In contrast to widely familiar acid- base behavior in solution, single molecules of NH3 and HCl do not react to form the ionic salt, NH4+Cl-, in isolation. We applied anion photoelectron spectroscopy and ab initio theory to investigate the interaction of an excess electron with the hydrogen- bonded complex NH3. HCl. Our results show that an excess electron induces this complex to form the ionic salt. We propose a mechanism that proceeds through a dipole- bound state to form the negative ion of ionic ammonium chloride, a species that can also be characterized as a deformed Rydberg radical, NH4, polarized by a chloride anion, Cl-.

引用

页码：936 / 939

页数：4

共 32 条

[1] Hydrogen bond vs proton transfer between neutral molecules in the gas phase [J].

Alkorta, I ;

Rozas, I ;

Mó, O ;

Yáñez, M ;

Elguero, J .

JOURNAL OF PHYSICAL CHEMISTRY A, 2001, 105 (31) :7481-7485

[2] Anion of the formic acid dimer as a model for intermolecular proton transfer induced by a π* excess electron -: art. no. 204304 [J].

Bachorz, RA ;

Haranczyk, M ;

Dabkowska, I ;

Rak, J ;

Gutowski, M .

JOURNAL OF CHEMICAL PHYSICS, 2005, 122 (20)

[3] STRONGLY HYDROGEN-BONDED MOLECULAR-COMPLEXES STUDIED BY MATRIX-ISOLATION VIBRATIONAL SPECTROSCOPY .1. THE AMMONIA HYDROGEN-CHLORIDE COMPLEX [J].

BARNES, AJ ;

BEECH, TR ;

MIELKE, Z .

JOURNAL OF THE CHEMICAL SOCIETY-FARADAY TRANSACTIONS II, 1984, 80 :455-463

[4] Amine-hydrogen halide complexes: Experimental electric dipole moments and a theoretical decomposition of dipole moments and binding energies [J].

Brauer, Carolyn S. ;

Craddock, Matthew B. ;

Kilian, Jacob ;

Grumstrup, Erik M. ;

Orilall, M. Christopher ;

Mo, Yirong ;

Gao, Jiali ;

Leopold, Kenneth R. .

JOURNAL OF PHYSICAL CHEMISTRY A, 2006, 110 (33) :10025-10034

[5] A CANDIDATE FOR AN ION-PAIR IN THE VAPOR-PHASE - PROTON-TRANSFER IN COMPLEXES R3N.HX [J].

BRCIZ, A ;

KARPFEN, A ;

LISCHKA, H ;

SCHUSTER, P .

CHEMICAL PHYSICS, 1984, 89 (03) :337-343

[6] Proton transfer reaction of hydrogen chloride with ammonia: is it possible in the gas phase? [J].

Cazar, R ;

Jamka, A ;

Tao, FM .

CHEMICAL PHYSICS LETTERS, 1998, 287 (5-6) :549-552

[7] Formation of ammonium halide particles from pure ammonia and hydrogen halide gases:: A theoretical study on small molecular clusters (NH3-HX)n (n=1, 2, 4; X = F, Cl, Br) [J].

Cherng, B ;

Tao, FM .

JOURNAL OF CHEMICAL PHYSICS, 2001, 114 (04) :1720-1726

[8] PHOTOELECTRON-SPECTROSCOPY OF THE NEGATIVE CLUSTER IONS NO-(N2O)N=1,2 [J].

COE, JV ;

SNODGRASS, JT ;

FREIDHOFF, CB ;

MCHUGH, KM ;

BOWEN, KH .

JOURNAL OF CHEMICAL PHYSICS, 1987, 87 (08) :4302-4309

[9] A NOVEL DISCRETE VARIABLE REPRESENTATION FOR QUANTUM-MECHANICAL REACTIVE SCATTERING VIA THE S-MATRIX KOHN METHOD [J].

COLBERT, DT ;

MILLER, WH .

JOURNAL OF CHEMICAL PHYSICS, 1992, 96 (03) :1982-1991

[10] On the binding of electrons to nitromethane: Dipole and valence bound anions [J].

Compton, RN ;

Carman, HS ;

Desfrancois, C ;

AbdoulCarmine, H ;

Schermann, JP ;

Hendricks, JH ;

Lyapustina, SA ;

Bowen, KH .

JOURNAL OF CHEMICAL PHYSICS, 1996, 105 (09) :3472-3478

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