Scalable and general synthesis of spinel manganese-based cathodes with hierarchical yolk–shell structure and superior lithium storage properties

Abstract

Hierarchical yolk–shell structured cathodes with controllable composition are potentially attractive materials for the fabrication of lithium-ion batteries, but they are difficult to synthesize. In this work, we present a simple, scalable, and general morphology-inheritance strategy to synthesize spinel manganese cathodes with a hierarchical yolk–shell structure. Starting from uniform Mn carbonate spheres prepared by an ultrafast and scalable microwave-assisted method, we show that the subsequent sintering results in the formation of Mn2O3 precursors with a yolk–shell structure, which can be effectively transferred to spinel manganese cathodes via simple impregnation and solid-state reaction. Owing to the simple and scalable nature of the present strategy, materials prepared through this approach have great potential as cathodes of lithium-ion batteries, where they can lead to high specific capacity, outstanding cyclability, and superior rate capability. In particular, both LiMn2O4 and LiNi0.5Mn1.5O4 with hierarchical yolk–shell structure achieved nearly theoretical capacity, without any apparent decay after 100 cycles at 1 C. Moreover, 80% of the initial discharge capacities of both samples can be maintained for up to 500 cycles at a high rate of 10 C.