Coordination tuning electronic structure of host materials is a quite effective strategy for activating and improving the intrinsic properties. Herein, halogen anion (X−)-incorporated β-FeOOH (β-FeOOH(X), X = F−, Cl−, and Br−) was investigated with a spontaneous adsorption process, which realized a great improvement of supercapacitor performances by adjusting the coordination geometry. Experiments coupled with theoretical calculations demonstrated that the change of Fe–O bond length and structural distortion of β-FeOOH, which is rooted in halogen ions embedment, led to the relatively narrow band gap. Because of the strong electronegativity of X−, the Fe element in β-FeOOH(X)s presented the unexpected high valence state (3 + δ), which is facilitating to adsorb SO32− species. Consequently, the designed β-FeOOH(X)s exhibited the good electric conductivity and enhanced the contact between electrode and electrolyte. When used as a negative electrode, the β-FeOOH(F) showed the excellent specific capacity of 391.9 F g−1 at 1 A g−1 current density, almost tenfold improvement compared with initial β-FeOOH, with the superior rate capacity and cyclic stability. This combinational design principle of electronic structure and electrochemical performances provides a promising way to develop advanced electrode materials for supercapacitor.
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