Capturing the Role of Explicit Solvent in the Dimerization of RuV(bda) Water Oxidation Catalysts
Zhan, Shaoqi ; Mårtensson, Daniel ; Purg, Miha ; Kamerlin, Shina C L LU
and Ahlquist, Mårten S G
(2017)
In Angewandte Chemie (International edition)
56(24).
p.6962-6965
- Abstract
A ground-breaking empirical valence bond study for a soluble transition-metal complex is presented. The full reaction of catalyst monomers approaching and reacting in the RuV oxidation state were studied. Analysis of the solvation shell in the reactant and along the reaction coordinate revealed that the oxo itself is hydrophobic, which adds a significant driving force to form the dimer. The effect of the solvent on the reaction between the prereactive dimer and the product was small. The solvent seems to lower the barrier for the isoquinoline (isoq) complex while it is increased for pyridines. By comparing the reaction in the gas phase and solution, the proposed π-stacking interaction of the isoq ligands is found to be entirely driven... (More)
A ground-breaking empirical valence bond study for a soluble transition-metal complex is presented. The full reaction of catalyst monomers approaching and reacting in the RuV oxidation state were studied. Analysis of the solvation shell in the reactant and along the reaction coordinate revealed that the oxo itself is hydrophobic, which adds a significant driving force to form the dimer. The effect of the solvent on the reaction between the prereactive dimer and the product was small. The solvent seems to lower the barrier for the isoquinoline (isoq) complex while it is increased for pyridines. By comparing the reaction in the gas phase and solution, the proposed π-stacking interaction of the isoq ligands is found to be entirely driven by the water medium.
(Less)
- author
- Zhan, Shaoqi
; Mårtensson, Daniel
; Purg, Miha
; Kamerlin, Shina C L
LU
and Ahlquist, Mårten S G
- publishing date
- 2017-06-06
- type
- Contribution to journal
- publication status
- published
- in
- Angewandte Chemie (International edition)
- volume
- 56
- issue
- 24
- pages
- 4 pages
- publisher
- John Wiley & Sons Inc.
- external identifiers
-
- scopus:85019990678
- pmid:28493633
- ISSN
- 1521-3773
- DOI
- 10.1002/anie.201701488
- language
- English
- LU publication?
- no
- additional info
- © 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.
- id
- b998a7ab-1af5-4642-8141-8d6f0deec900
- date added to LUP
- 2025-01-11 21:25:04
- date last changed
- 2025-01-21 03:19:56
@article{b998a7ab-1af5-4642-8141-8d6f0deec900,
abstract = {{<p>A ground-breaking empirical valence bond study for a soluble transition-metal complex is presented. The full reaction of catalyst monomers approaching and reacting in the RuV oxidation state were studied. Analysis of the solvation shell in the reactant and along the reaction coordinate revealed that the oxo itself is hydrophobic, which adds a significant driving force to form the dimer. The effect of the solvent on the reaction between the prereactive dimer and the product was small. The solvent seems to lower the barrier for the isoquinoline (isoq) complex while it is increased for pyridines. By comparing the reaction in the gas phase and solution, the proposed π-stacking interaction of the isoq ligands is found to be entirely driven by the water medium.</p>}},
author = {{Zhan, Shaoqi and Mårtensson, Daniel and Purg, Miha and Kamerlin, Shina C L and Ahlquist, Mårten S G}},
issn = {{1521-3773}},
language = {{eng}},
month = {{06}},
number = {{24}},
pages = {{6962--6965}},
publisher = {{John Wiley & Sons Inc.}},
series = {{Angewandte Chemie (International edition)}},
title = {{Capturing the Role of Explicit Solvent in the Dimerization of Ru<sup>V</sup>(bda) Water Oxidation Catalysts}},
url = {{http://dx.doi.org/10.1002/anie.201701488}},
doi = {{10.1002/anie.201701488}},
volume = {{56}},
year = {{2017}},
}