Redox Mechanisms upon the Lithiation of Wadsley-Roth Phases.

The Wadsley-Roth family of transition metal oxide phases are a promising class of anode materials for Li-ion batteries due to their open crystal structures and their ability to intercalate Li at high rates. Unfortunately, most early transition metal oxides that adopt a Wadsley-Roth crystal structure intercalate Li at voltages that are too high for most battery applications. First-principles electronic structure calculations are performed to elucidate redox mechanisms in Wadsley-Roth phases with the aim of determining how they depend on crystal structure.

Redox Mechanisms, Structural Changes, and Electrochemistry of the Wadsley-Roth LiTiNbO Electrode Material.

The TiNbO Wadsley-Roth phase is a promising anode material for Li-ion batteries, enabling fast cycling and high capacities. While already used in commercial batteries, many fundamental electronic and thermodynamic properties of LiTiNbO remain poorly understood. We report on an in-depth first-principles study of the redox mechanisms, structural changes, and electrochemical properties of LiTiNbO as a function of Li concentration.

Chemical and Structural Factors Affecting the Stability of Wadsley-Roth Block Phases.

Wadsley-Roth phases have emerged as highly promising anode materials for Li-ion batteries and are an important class of phases that can form as part of the oxide scales of refractory multiprinciple element alloys. An algorithmic approach is described to systematically enumerate two classes of Wadsley-Roth crystallographic shear structures. An analysis of algorithmically generated Wadsley-Roth phases reveals that a diverse set of oxide crystal structures belongs to the Wadsley-Roth family of phases.