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Proton mobility and stability of water clusters containing the bisulfate anion, HSO(4)(-)(H(2)O)(n).
MedLine Citation:
PMID:  21701718     Owner:  NLM     Status:  Publisher    
Abstract/OtherAbstract:
Bisulfate water clusters, HSO(4)(-)(H(2)O)(n), have been studied both experimentally by a quadrupole time-of-flight mass spectrometer and by quantum chemical calculations. For the cluster distributions studied, there are some possible "magic number" peaks, although the increase in abundance compared to their neighbours is small. Experiments with size-selected clusters with n = 0-25, reacting with D(2)O at a center-of-mass energy of 0.1 eV, were performed, and it was observed that the rate of hydrogen/deuterium exchange is lower for the smallest clusters (n < 8) than for the larger (n > 11), with a transition taking place in the range n = 8-11. We propose that the protonic defect of the bisulfate ion remains rather stationary unless the degree of hydration reaches a given level. In addition, it was observed that H/D scrambling becomes close to statistically randomized for the larger clusters. Insight into this size dependency was obtained by B3LYP/6-311++G(2d,2p) calculations for HSO(4)(-)(H(2)O)(n) with n = 0-10. In agreement with experimental observations, these calculations suggest pronounced effectiveness of a ''see-saw mechanism'' for pendular proton transfer with increasing HSO(4)(-)(H(2)O)(n) cluster size.
Authors:
Alexey S Zatula; Patrik Urban Andersson; Mauritz Johan Ryding; Einar Uggerud
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Publication Detail:
Type:  JOURNAL ARTICLE     Date:  2011-6-23
Journal Detail:
Title:  Physical chemistry chemical physics : PCCP     Volume:  -     ISSN:  1463-9084     ISO Abbreviation:  -     Publication Date:  2011 Jun 
Date Detail:
Created Date:  2011-6-24     Completed Date:  -     Revised Date:  -    
Medline Journal Info:
Nlm Unique ID:  100888160     Medline TA:  Phys Chem Chem Phys     Country:  -    
Other Details:
Languages:  ENG     Pagination:  -     Citation Subset:  -    
Affiliation:
Mass Spectrometry Laboratory and Centre of Theoretical and Computational Chemistry, Department of Chemistry, University of Oslo, POB 1033 Blindern, N-0315 Oslo, Norway. einar.uggerud@kjemi.uio.no.
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