Three new inorganic-organic hybrid compounds, (H3DIBA)2·SiMo12O40·H2O (1), (H3DIBA)2·SiW12O40·H2O (2), and [(H2DIBA)(H3DIBA)]·PMo12O40·2H2O (3) (HDIBA = 3,5-di(1H-imidazol-1-yl)benzoic acid) were synthesized by the hydrothermal method. The structures were characterized by single-crystal X-ray diffraction, elemental analysis, powder X-ray diffraction, infrared spectroscopy, and thermogravimetric analysis. These three compounds are all 3D supramolecular structures formed by Keggin-type polyoxometalate anions and HDIBA through intermolecular weak interactions, which have been studied via Hirshfeld surface analysis. The electrochemistry properties of 1 and 3 have been studied, including cyclic voltammetric behaviors and electrocatalytic properties. The study on the removal of organic dye pollutants in water showed that compounds 1 and 3 had an adsorption effect on cationic dye RhB, and the adsorption process conforms to the Langmuir isotherm model. Compound 2 can photocatalytically degrade cationic organic dyes RhB, MB, and CV, and the photocatalytic mechanism study indicates that h+ plays a major role in the photocatalytic process.
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