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The reaction of N 2 O 5 with H 3 O + : A first‐principles direct molecular dynamics study of acid‐catalyzed reactive uptake of N 2 O 5
Author(s) -
Ishikawa Sascha T.,
Nakajima Takahito
Publication year - 2009
Publication title -
international journal of quantum chemistry
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 0.484
H-Index - 105
eISSN - 1097-461X
pISSN - 0020-7608
DOI - 10.1002/qua.22071
Subject(s) - decomposition , chemistry , catalysis , molecular dynamics , quantum chemical , computational chemistry , molecule , organic chemistry
Abstract Direct molecular dynamics simulations of N 2 O 5 + H 3 O + collision were conducted; (1) to assess the importance of acid‐catalyzed N 2 O 5 decomposition paths expected to play a significant role in the chemistry of stratospheric ozone depletion and (2) for their potential to identify unexpected decomposition paths. A single H 3 O + ‐catalyzed N 2 O 5 decomposition path was observed. Products formed are H 2 O, NO 2 + , HNO 3 , and complexes of the decomposition products, (H 2 O)(NO 2 + ), (H 2 O)(HNO 3 ), and (HNO 3 )(NO 2 + ). All decompositions were barrierless, including complex formations of the products. Reaction exothermicities, which were characterized with a QCISD(T)/6‐311++G(d,p)//MP2/6‐311++G(d,p) model, ranged from 5.9 to 32.0 kcal/mol. © 2009 Wiley Periodicals, Inc. Int J Quantum Chem, 2009