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Hydrothermal Synthesis of Spinel-Perovskite Li-Mn-Fe-Si Nanocomposites for Electrochemical Hydrogen Storage.

Owing to the extensive requirement for renewable energy sources such as hydrogen, great efforts are being devoted to optimizing the active ingredients for advanced hydrogen storage. In this regard, an ideal spinel-perovskite nanocomposite based on Li-Mn-Fe-Si materials was successfully fabricated via a one-pot hydrothermal route to store hydrogen electrochemically. To optimize both the phase composition and morphological features of nanostructures, the reaction was engineered under different conditions. Li-Mn-Fe-Si spinel-perovskite diphase structures were created with diverse shapes of polyhedral-shaped bulk particles, nanoparticles, nanoplates, and hierarchical structures. The alteration of multiple factors such as hydrothermal reaction time, temperature, polymeric surfactant type, and calcination temperature was surveyed to achieve the optimized size and morphology of the nanoproducts to be obtained. The morphological changes, structural regulations, porosity, and magnetic properties of the nanosized products were studied via field-emission scanning electron microscopy (FE-SEM), high-resolution transmission electron microscopy (HR-TEM), X-ray powder diffraction (XRD), Raman spectroscopy, Brunauer-Emmett-Teller (BET), and vibrating sample magnetometer (VSM) analyses. In addition, the electrochemistry features of the Li0.66Mn1.85Fe0.43O4/Fe2.57Si0.43O4/FeSiO3 (LMFO/FSO) nanocomposites were introduced on the basis of discharge capacity, electrochemical impedance spectroscopy (EIS) and cyclic voltammetry(CV) methods in an alkaline electrolyte. The discharge capacity of the LMFO/FSO nanostructures with a nanoplate-like morphology as an optimal sample was calculated to be 910 mAh/g after 15 cycles at a constant current of 1 mA. The electrochemistry results confirm that the hydrogen storage capability of nanoplate composites is higher than those of other morphologies due to their superior surface area and faster electron transfer. Besides, this proposed strategy could simultaneously manipulate the architectural and compositional complexities to generate a superior electrochemical behavior in energy storage devices.