Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 135, Issue 51, Pages 19075-19078Publisher
AMER CHEMICAL SOC
DOI: 10.1021/ja4104974
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Funding
- California Institute of Technology
- Searle Scholars Program
- NSF CAREER [CHE-1151918]
- Camille & Henry Dreyfus Environmental Chemistry Fellowship
- Resnick Sustainability Institute
- National Science Foundation Center for Chemical Innovation on Solar Fuels (CCI Solar) [CHE-1305124]
- NSF Chemistry Research Instrumentation [CHE-0639094]
- Gordon and Betty Moore Foundation
- Beckman Institute
- Sanofi-Aventis BRP at Caltech
- U.S. DOE
- NIH
- Direct For Mathematical & Physical Scien
- Division Of Chemistry [1151918] Funding Source: National Science Foundation
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A series of tetranuclear oxo/hydroxo clusters comprised of three Fe centers and a redox-inactive metal (M) of various charge is reported. Crystallographic studies show an unprecedented Fe3M(mu(4)-O)(mu(2)-OH) core that remains intact upon changing M or the oxidation state of iron. Electrochemical studies reveal that the reduction potentials (E-1/2) span a window of 500 mV and depend upon the Lewis acidity of M. Using the pK(a) of the M-aqua complex as a measure of Lewis acidity, these compounds display a linear dependence between E-1/2 and acidity, with a slope of similar to 70 mV per pK(a) unit. The current study of [Fe3MO(OH)] and previous ones of [Mn3MOn] (n = 2,4) moieties support the generality of the above relationship between the reduction potentials of heterometallic oxido clusters and the Lewis acidity of incorporated cations, as applied to clusters of different redox-active metals.
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