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Trapping an iron(VI) water-splitting intermediate in nonaqueous media

Hunter, Bryan and Thompson, Niklas and Mueller, Astrid and Rossman, George and Hill, Michael and Winkler, Jay and Gray, Harry (2018) Trapping an iron(VI) water-splitting intermediate in nonaqueous media. In: 256th American Chemical Society National Meeting & Exposition, 19-23 August 2018, Boston, MA.

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Understanding the mechanisms of highly-active, earth-abundant water oxidn. electrocatalysts can guide the development of advanced water-splitting devices that convert renewable electricity to clean fuels. Unfortunately, catalytic intermediates are difficult to isolate and characterize because they tend to be extremely transient and present at low concns. A typical approach to this problem is to slow down turnover by limiting the availability of substrate. However, in cases where substrate and solvent are identical-such as in water oxidn.-the soln. can be more complex. By dramatically limiting the availability of substrate (water and hydroxide) in nickel-iron catalyzed heterogeneous water oxidn., we have obsd. and characterized a high-valent iron intermediate. Orthogonal spectroscopies indicate that the intermediate contains iron in the rare 6+ oxidn. state. This ferrate analog makes dioxygen upon addn. of hydroxide and can be stepwise regenerated by anodic polarization.

Item Type:Conference or Workshop Item (Paper)
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URLURL TypeDescription Website
Hunter, Bryan0000-0001-8559-9304
Thompson, Niklas0000-0003-2745-4945
Mueller, Astrid0000-0002-2785-6808
Rossman, George0000-0002-4571-6884
Winkler, Jay0000-0002-4453-9716
Gray, Harry0000-0002-7937-7876
Additional Information:© 2018 American Chemical Society.
Record Number:CaltechAUTHORS:20181109-141642042
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Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:90803
Deposited By: Tony Diaz
Deposited On:14 Nov 2018 19:10
Last Modified:09 Mar 2020 13:19

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