The Reaction of N2O5 With H3O+: A First-Principles Direct Molecular Dynamics Study of Acid-Catalyzed Reactive Uptake of N2O5

摘要

Direct molecular dynamics simulations of N2O5 + H3O+ collision were conducted; (1) to assess the importance of acid-catalyzed N2O5 decomposition paths expected to play a significant role in the chemistry of stratospheric ozone depletion and (2) for their potential to identify tmexpected decomposition paths. A single H3O+-catalyzed N2O5 decomposition path was observed. Products formed are H2O, NO2+, HNO3, and complexes of the decomposition products, (H2O)(NO2+), (H2O)(HNO3), and (HNO3)(NO2+). All decompositions were barrierless, including complex formations of the products. Reaction exothermicities, which Nvere 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.