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How the shape of an H-Bonded network controls proton-coupled water activation in HONO formation

Relph, RA and Guaseo, TL and Elliott, BM and Kamrath, MZ and McCoy, AB and Steele, RP and Schofield, DP and Jordan, KD and Viggiano, AA and Ferguson, EE and Johnson, MA (2010) How the shape of an H-Bonded network controls proton-coupled water activation in HONO formation. Science, 327 (5963). 308 - 312. ISSN 0036-8075

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Abstract

Many chemical reactions in atmospheric aerosols and bulk aqueous environments are influenced by the surrounding solvation shell, but the precise molecular interactions underlying such effects have rarely been elucidated. We exploited recent advances in isomer-specific cluster vibrational spectroscopy to explore the fundamental relation between the hydrogen (H)-bonding arrangement of a set of ion-solvating water molecules and the chemical activity of this ensemble. We find that the extent to which the nitrosonium ion (NO+) and water form nitrous acid (HONO) and a hydrated proton cluster in the critical trihydrate depends sensitively on the geometrical arrangement of the water molecules in the network. Theoretical analysis of these data details the role of the water network in promoting charge derealization.

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Details

Item Type: Article
Status: Published
Creators/Authors:
CreatorsEmailPitt UsernameORCID
Relph, RA
Guaseo, TL
Elliott, BM
Kamrath, MZ
McCoy, AB
Steele, RP
Schofield, DP
Jordan, KDjordan@pitt.eduJORDAN
Viggiano, AA
Ferguson, EE
Johnson, MA
Date: 15 January 2010
Date Type: Publication
Journal or Publication Title: Science
Volume: 327
Number: 5963
Page Range: 308 - 312
DOI or Unique Handle: 10.1126/science.1177118
Schools and Programs: Dietrich School of Arts and Sciences > Chemistry
Refereed: Yes
ISSN: 0036-8075
PubMed ID: 20075247
Date Deposited: 12 Nov 2012 15:01
Last Modified: 12 Jun 2021 22:55
URI: http://d-scholarship-dev.library.pitt.edu/id/eprint/16159

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