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Optimal water concentration for aqueous Li⁺ intercalation in vanadyl phosphate.

ABSTRACT: Development of high-performance aqueous batteries is an important goal for energy sustainability owing to their environmental benignity and low fabrication costs. Although a layered vanadyl phosphate is one of the most-studied host materials for intercalation electrodes with organic electrolytes, little attention has been paid to its use in aqueous Li⁺ systems because of its excessive dissolution in water. Herein, by controlling the water concentration, we demonstrate the stable operation of a layered vanadyl phosphate electrode in an aqueous Li⁺ electrolyte. The combination of experimental analyses and density functional theory calculations reveals that reversible (de)lithiation occurs between dehydrated phases, which can only exist in an optimal water concentration.

SUBMITTER: Sun D

PROVIDER: S-EPMC8179479 | biostudies-literature | 2021 Feb

REPOSITORIES: biostudies-literature

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Optimal water concentration for aqueous Li<sup>+</sup> intercalation in vanadyl phosphate.

Sun Dan D Okubo Masashi M Yamada Atsuo A

Chemical science 20210211 12

Development of high-performance aqueous batteries is an important goal for energy sustainability owing to their environmental benignity and low fabrication costs. Although a layered vanadyl phosphate is one of the most-studied host materials for intercalation electrodes with organic electrolytes, little attention has been paid to its use in aqueous Li<sup>+</sup> systems because of its excessive dissolution in water. Herein, by controlling the water concentration, we demonstrate the stable opera ...[more]

PMID: 34163710

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Project description:Alkali ion intercalation is fundamental to battery technologies for a wide spectrum of potential applications that permeate our modern lifestyle, including portable electronics, electric vehicles, and the electric grid. In spite of its importance, the Nernstian nature of the charge transfer process describing lithiation of carbon has not been described previously. Here we use the ultrathin few-layer graphene (FLG) with micron-sized grains as a powerful platform for exploring intercalation and co-intercalation mechanisms of alkali ions with high versatility. Using voltammetric and chronoamperometric methods and bolstered by density functional theory (DFT) calculations, we show the kinetically facile co-intercalation of Li+ and K+ within an ultrathin FLG electrode. While changes in the solution concentration of Li+ lead to a displacement of the staging voltammetric signature with characteristic slopes ca. 54-58 mV per decade, modification of the K+/Li+ ratio in the electrolyte leads to distinct shifts in the voltammetric peaks for (de)intercalation, with a changing slope as low as ca. 30 mV per decade. Bulk ion diffusion coefficients in the carbon host, as measured using the potentiometric intermittent titration technique (PITT) were similarly sensitive to solution composition. DFT results showed that co-intercalation of Li+ and K+ within the same layer in FLG can form thermodynamically favorable systems. Calculated binding energies for co-intercalation systems increased with respect to the area of Li+-only domains and decreased with respect to the concentration of -K-Li- phases. While previous studies of co-intercalation on a graphitic anode typically focus on co-intercalation of solvents and one particular alkali ion, this is to the best of our knowledge the first study elucidating the intercalation behavior of two monovalent alkali ions. This study establishes ultrathin graphitic electrodes as an enabling electroanalytical platform to uncover thermodynamic and kinetic processes of ion intercalation with high versatility.

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Optimal water concentration for aqueous Li⁺ intercalation in vanadyl phosphate.

Publications

Optimal water concentration for aqueous Li<sup>+</sup> intercalation in vanadyl phosphate.

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Optimal water concentration for aqueous Li+ intercalation in vanadyl phosphate.

Publications

Optimal water concentration for aqueous Li<sup>+</sup> intercalation in vanadyl phosphate.

Similar Datasets

OmicsDI is part of the ELIXIR infrastructure

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Optimal water concentration for aqueous Li⁺ intercalation in vanadyl phosphate.