Calcination Heterogeneity in Li-Rich Layered Oxides: A Systematic Study of Li2CO3 Particle Size

• DOI: 10.1021/acs.chemmater.3c02404
• Publication Date: 2023-12-13T20:40:10Z
• Authors: Grace M. Busse; Peter M. Csernica; Kipil Lim; Junghwa Lee; Zhelong Jiang; Diego F. Rivera; Young Jin Kim; David A. Shapiro; William E. Gent; William C. Chueh
• Keywords: Thermogravimetry; Thermogravimetric analysis; Particle (ecology)

Li- and Mn-rich (LMR) layered oxide positive-electrode materials exhibit high energy density have earth-abundant compositions relative to conventional Ni-, Mn-, Co-oxides (NMCs). The lithiation of coprecipitated precursors is a key part the synthesis offers opportunities for tuning properties LMR materials. Whereas morphology transition metal has received substantial attention, that Li sources not. Using Li1.14Mn0.57Ni0.29O2 as model system, in this work, we establish detailed understanding calcination pathways via situ ex diffraction, spectroscopy, microscopy, thermogravimetry. Our work shows large Li2CO3 particle size modulates previously misunderstood thermogravimetric feature present at melting point during causes heterogeneity larger length scales (inter-secondary particle) than reported (intra-secondary particle). We found electrochemical performance largely insensitive heterogeneity. This highlights sensitivity conditions suggests design rules minimize oxides beyond LMR.