Hydrothermal Production of Lithium Metal Silicate Powders with Controlled Properties for Application to Li-ion Batteries

Lithium metal silicates (Li2MSiO4, M = Fe or Mn) composed of abundant and non-toxic elements are important cathode materials for Li-ion batteries (LIB). In contrast to solid-state or sol-gel methods, hydrothermal synthesis conducted in pressure reactors is a favorable processing route as it provides the potential for scalable production and is environmentally benign. However, the key is to control the precipitation reaction to obtain powders with desired properties to meet battery specifications. Through a systematic study, we have found that Li2MSiO4 with tunable size from 300 nm to 1.5 μm can be produced by adjusting precursor concentrations, temperature, and reaction time. Under optimum conditions, high purity Li2MSiO4 with minimum defects were successfully produced and examined as an LIB cathode. The use of complexing agents promoted the formation of unique hollow particles via the self-assembling of elongated crystals. A four-step formation mechanism is proposed based on extensive characterizations with XRD, HR-TEM, SEM, and Mössbauer spectroscopy.