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The coupling of a single proton to [4Fe-4S]2+/+ oxidation/reduction in a de novo designed iron-sulfur protein maquette is presented. The reduced state pKared is 9.3, and the oxidized state pKaox is &lt;6.5. The reduced state pKared shifts to 8.3 upon incorporation of a [4Fe-4Se]2+/+ cluster, implicating the cluster itself or its primary coordination sphere as the proton-coupling site.

Proton Coupling to [4Fe-4S]2+/+ and [4Fe-4Se]2+/+ Oxidation and Reduction in a Designed Protein

Proton Coupling to [4Fe-4S]^2+/+ and [4Fe-4Se]^2+/+ Oxidation and Reduction in a Designed Protein