Protonation of N2O and NO2 in a solid phase

被引:8
|
作者
Stoyanov, Evgenii S. [1 ,2 ]
Stoyanova, Irina V. [1 ]
机构
[1] Russian Acad Sci, Vorozhtsov Inst Organ Chem, Siberian Branch, Novosibirsk 630090, Russia
[2] Novosibirsk State Univ, Dept Nat Sci, Natl Res Univ, Novosibirsk 630090, Russia
基金
俄罗斯基础研究基金会; 俄罗斯科学基金会;
关键词
NATURAL RESONANCE THEORY; SPECTROSCOPIC DETECTION; ACID PROTONATION; GAS-PHASE; IONS; CHEMISTRY; AFFINITY; CATION; ORDER; BOND;
D O I
10.1039/c7cp04474g
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
Adsorption of gaseous N2O on the acidic surface Bronsted centers of the strongest known solid acid, H(CHB11F11), results in formation of the N N-OH+ cation. Its positive charge is localized mainly to the H-atom, which is H-bonded to the CHB11F11- anion forming an asymmetric proton disolvate of the L-1-H+center dot center dot center dot L-2 type, where L-1 = N2O and L-2 = CHB11F11-. NO2 protonation under the same conditions leads to the formation of the highly reactive cation radical NO2H center dot+, which reacts rapidly with an NO2 molecule according to the equation N2OH+ + NO2 --> [N2O4H+] --> N2OH+ + O-2 resulting in the formation of two types of N2OH+ cations: (i) a typical Bronsted superacid, N N-OH+, with a strongly acidic OH group involved in a rather strong H-bond with the anion, and (ii) a typical strong Lewis acid, N N+-OH, with a positive charge localized to the central N atom and ionic interactions with the surrounding anions via the charged central N atom.
引用
收藏
页码:32733 / 32740
页数:8
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