Homoleptic hydrides of the first row transition metals
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Author : LZH
Update time : 2023-07-25 02:42:22
What is vanadium hydride? Vanadium hydride is particularly true for lightweight, high oxidation state vanadium materials, as shown by the relative performance of V2O5. Lower oxidation state vanadium materials such as VO2 and V2O3 have also shown potential with initial capacities of >150 mAhg -1. Thus, related vanadium hydride materials could have significant potential as lithium battery cathode materials. They would possess several vanadium centers in the V(IV) or V(III) oxidation states, providing the capacity for lithium insertion. Furthermore, the hydride ligand is considerably lighter than the O and P used in traditional vanadium-based battery materials, potentially affording much higher electron per-gram energy storage numbers. Fabricating these materials in a nanocrystalline form would be of added benefit because of the potential for pseudocapacitance, which uses the vast majority of the redox centers situated near the surface to improve the kinetics of the charge transfer reaction due to the shorter diffusion path lengths, leading to a capacitive-like response. A nanocrystalline vanadium hydride may thus be highly desirable as it could potentially possess higher energy densities than observed in vanadium oxides and phosphates but with higher power density due to the faster charge and discharge kinetics afforded by pseudocapacitance.
Homoleptic hydrides of the first row transition metals Homoleptic hydrides of the first-row transition metals represent a new frontier in energy storage because of their low molecular weight, electrochemical flexibility, and potential for coordinative unsaturation. This feature can be exploited in hydrogen or methane storage. The transition metal dihydrides MH2 (M= Cr, 2 Mn, 3 Fe, 4 Co, and Ni5 ) and trihydrides of the form MH3 (M= Ti6 ) have been observed as molecular species using matrix isolation techniques at cryogenic temperatures but have never been isolated pure in bulk form. Because of the low cost of vanadium (ca. 15-20 USD/kg) and its importance in battery materials of this metal as well as the overall low mass of the hydride ligand, a gravimetric advantage in any energy storage application, the development of general and convenient synthetic routes into vanadium hydrides for energy storage applications would represent an important advance. Metallic vanadium reacts with hydrogen at room temperature and atmospheric pressure to give nonstoichiometric monohydrides up to VH0.9. Higher hydrides of vanadium (VH~1.6) were prepared by Maeland et al. using electrolytic techniques. Later, the dihydride VH2 was formed by a reaction of vanadium with 6.9 bar hydrogen at 450 °C, which was found to be unstable at room temperature.8 From the standpoint of electrochemical energy storage, the synthesis of vanadium hydrides in higher oxidation states than II is important because of the greater electron per mole capacities relative to lower oxidation state species, however to the best of our knowledge, a pure phase has higher hydride such as VH3 or VH4 has never been isolated or characterized in bulk form.
In previous work we explored the potential of vanadium hydride transition metal alkyl hydrides In previous work, we explored the potential of homoleptic transition metal alkyl hydrides9 for applications in hydrogen storage using the Kubas interaction, 10,11 a type of H2 binding intermediate in energy between physisorption and dissociative hydride-forming pathways. The first example we reported was an amorphous Ti(III) alkyl hydride with a reversible gravimetric hydrogen storage capacity of 3.49 wt% at 140 bar and 25 °C. 9a Improvements in gravimetric capacity to 5.07 wt% at 160 bar and 5.4 wt% at 120 bar were later demonstrated in Cr(III) alkyl hydride9b and V(III) alkyl hydride gels, 9c respectively. Surprisingly, the hydrogen adsorption of the Cr and V materials was measured as less than one kJ mol-1 H2 endothermic, suggesting that the complex heat management systems that thwart applications of hydrides and physisorption materials may not be required for onboard applications. While the hydrogen storage performance and thermodynamic neutrality of the V(III) alkyl hydride suggests that a system based around it may approach the US Department of Energy’s (DOE) gravimetric system goal of 5.5 wt %, previous research into battery materials has shown that vanadium compounds perform well as cathode materials for lithium-ion batteries.
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