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The physicochemical and electrocatalytic behaviors of eight multi-iron Wells−Dawson sandwich-type polyoxometalates were studied with specific emphasis on the Fe III centers. Magnetization measurements were used to identify and quantify the antiferromagnetic interactions between the edge-sharing Fe III units. Electrochemical studies show the stepwise reduction of the Fe III centers, in complete agreement with magnetization conclusions. The location of the potential of each wave depends on the pH of the solution, as well as the concentration and composition of the electrolyte. In addition, ion-pairing studies show there is a positive shift