Journal
CHEMICAL SCIENCE
Volume 4, Issue 2, Pages 734-738Publisher
ROYAL SOC CHEMISTRY
DOI: 10.1039/c2sc21419a
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Funding
- Canadian Natural Science and Engineering Research Council
- Canada Research Chairs
- Canadian Foundation for Innovation
- Canada School of Energy and Environment
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The proton-coupled electron transfer (PCET) chemistry associated with the [Co-OH](2+)/[Co-OH2](2+) redox couple for [Co(PY5)(OH2)](2+) (1; PY5 = 2,6-(bis(bis-2-pyridyl)-methoxymethane)-pyridine) and [Co-II(pz(4)depy)(OH2)](2+) (2; pz(4)depy 2,6-bis(1,1-di(1H-pyrazol-1-yl) ethyl) pyridine) is reported. It is found that the couple is acutely sensitive to the geometry of the axially ligated group in addition to the electronic-donating/-withdrawing character of the ligand. Interrogation of the electron-transfer kinetics by electrochemical methods also shows for the first time that the interconversion of [Co-III-OH](2+) and [CoII-OH2](2+) proceeds through a concerted pathway in favour of energetically unfavourable stepwise electron-transfer or proton-transfer reaction steps.
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