Syntheses, crystal structures, topology and dual electronic behaviors of a family of amine-templated three- dimensional zinc-organophosphonate hybrid solids

•Three new crystalline zinc-organophosphonate hybrid compounds have been synthesized.•Templated amines play crucial role for the structural diversity.•High dielectric permittivity values are observed for anionic framework.•Hybrid phosphonate frameworks are applicable as electrode material. Three new inorganic–organic hybrid zinc organodiphosphonate compounds, [H2TEMED][Zn3(hedp)2] (1), [H2TEPA][Zn6(Hhedp)2(hedp)2]·2H2O (2) and [H2DETA]2[Zn12(Hhedp)4(hedp)4]·3H2O (3) (H4hedp = 1-hydroxyethane 1,1-diphosphonic acid, TEMED = N,N,N',N'-tetramethylethylenediamine, TEPA = tetraethylenepentamine and DETA = diethylenetriamine) have been synthesized by employing the variable amine-templated hydrothermal strategy. All the compounds are characterized and analyzed by PXRD, FT-IR, TGA, SEM and EDAX studies. Single crystal x-ray diffraction experiments reveal that the compounds 1–3 have formed interconnected 4-T, 8-T and 12-T open ring three-dimensional framework structure through the alternate connection of zinc ions and diphosphonate ligands. Topological analysis study displays compound 1 adopts (4.5.72.8.9)(4.7.8)(52.72.82)(52.7) net topology whereas compounds 2 and 3 show ILEHUD (4.5.6.83)(4.6.8)(52.6.83)(52.8) net topology, even though the observed asymmetric units are dissimilar in case of 2 and 3. The UV-visible spectroscopic studies recommend the compounds as wide band-gap semiconducting materials. The observed dielectric permittivity of the compounds are considerably high (ε′ ∼ 100) at room temperature. The electrochemical performance tests indicate that compound 3 exhibit a high specific capacitance of 216 F g−1 at 1 A g−1 along with an excellent cycle stability of 79.6 % even after 5000 cycles at 5 A g−1 in the 6 M KOH solution while compound 1 and 2 possess specific capacitance values of 164 and 170 F g−1 with cycling retention of 68.42 % and 57.82 %, respectively. Such high-performance supercapacitance behavior in amine templated framework is noteworthy. [Display omitted]