TY - JOUR
T1 - Microscopic Mechanisms of N2O5 Hydrolysis on the Surface of Water Droplets
AU - Rossich Molina, Estefaniá
AU - Gerber, R. Benny
N1 - Publisher Copyright:
Copyright © 2019 American Chemical Society.
PY - 2020/1/9
Y1 - 2020/1/9
N2 - Reactions of N2O5, in particular heterogeneous hydrolysis, play a vital role in determining the chemistry of the atmosphere. The N2O5 heterogeneous hydrolysis reaction has been the subject of extensive research for decades, yet the physicochemical details of the mechanism have not been established. In this study, we show that this reaction can occur on the surface of a pure water droplet. We compute a relevant transition state for a nano-size model system and follow its evolution in time by means of ab initio molecular dynamics. This transition state, where N2O5 has a strong ion-pair character, leads directly to HNO3. Both electrophilic and nucleophilic mechanisms take place. It is suggested that corresponding simulations for hydrolysis in the bulk are desirable.
AB - Reactions of N2O5, in particular heterogeneous hydrolysis, play a vital role in determining the chemistry of the atmosphere. The N2O5 heterogeneous hydrolysis reaction has been the subject of extensive research for decades, yet the physicochemical details of the mechanism have not been established. In this study, we show that this reaction can occur on the surface of a pure water droplet. We compute a relevant transition state for a nano-size model system and follow its evolution in time by means of ab initio molecular dynamics. This transition state, where N2O5 has a strong ion-pair character, leads directly to HNO3. Both electrophilic and nucleophilic mechanisms take place. It is suggested that corresponding simulations for hydrolysis in the bulk are desirable.
UR - http://www.scopus.com/inward/record.url?scp=85077761740&partnerID=8YFLogxK
U2 - 10.1021/acs.jpca.9b08900
DO - 10.1021/acs.jpca.9b08900
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C2 - 31829595
AN - SCOPUS:85077761740
SN - 1089-5639
VL - 124
SP - 224
EP - 228
JO - Journal of Physical Chemistry A
JF - Journal of Physical Chemistry A
IS - 1
ER -