Crystal structure and electronic structure calculations of a novel organic triphosphate complex: excellent electrochemical properties with ultra-efficient lithium storage capacity

Abstract

A new organic–inorganic hybrid molecule, cyclohexyl ammonium dihydride triphosphate, was synthesized at room temperature with slow evaporation, yielding a new triphosphate with the formula HO₁₀P₃·(C₆H₁₄N)₄·2(H₂O) using a chemical ion exchange process. Detailed crystal structure analysis by single crystal X-ray diffraction has been reported, and different units in the molecular arrangement are held together by N–H⋯O and O–H⋯O hydrogen bonds to form a three-dimensional structure. Spectroscopic analysis including FT-IR, UV-visible, and ATD/ATG were also employed to characterize the complex. Explorations of impedance spectroscopy on HO₁₀P₃·(C₆H₁₄N)₄·2(H₂O) show fascinating electrical behavior, which reveals that the triphosphate component can be used as an electronic chip and under certain conditions; this semiconductor can act as a conductor, which can be considered as a pure element. Electrochemical impedance spectroscopy (EIS) and cyclic voltammetry (CV) measurements were performed. Electronic structure calculations were performed using the ωB97XD/def2tzvp method. In the thermodynamic study, the Gibbs free energy of formation, interaction energy, and enthalpy of formation were calculated. NBO charges and FMO study show the nature of the donor–acceptor part in the complex. Quantum theory of atoms in molecule (QTAIM) is employed to unfold the noncovalent interactions present in the complex. Optical and nonlinear optical (NLO) properties are determined by calculating polarizability and hyperpolarizability. Hirshfeld surface (HS) analysis reveals the strength and nature of elemental interactions in crystal packing. Theoretical findings are compatible with the experimental study.