Solvent Determines the Formation Pathway in Sol–Gel Synthesized Disordered Rock Salt Material for Lithium Ion Battery Application

Abstract

The increasing demand for lithium-ion batteries with high capacity and cycling stability, in combination with the scarcity of cobalt and nickel, has led to significant efforts to develop new cathode materials based on earth-abundant transition metals. Mn- and Ti-based disordered rock salt (DRX) cathodes are promising candidates fulfilling these requirements. However, their large-scale fabrication can be energy- and time-intensive using traditional fabrication methods, e.g., solid-state synthesis. The present study showcases sol–gel synthesis as an alternative method with control over the crystallization pathway through solvent choice. Dimethylformamide (DMF) aids the homogenization of the transition metals during early crystallization stages and formation of Li₂TiO₃ and LiMn₂O₄ intermediates before the DRX phase is formed. In contrast, 2-methoxyethanol (2-ME) shows transition metal segregation and formation of an additional transition metal intermediate (Ti₂MnO₄) while not resulting in phase-pure DRX material after calcination. Coin cells prepared with DMF-material yield higher capacity and cycling stability compared with 2-ME material.