Quantitative image-analysis framework for precise discrimination of cation mixing in high-nickel NCM cathodes

•Developed an automated HAADF-STEM image-analysis framework eliminating observer bias.•Established an angular-deviation and regional-classification methodology for quantitative structural assessment.•Quantitatively discriminated Li/Ni cation mixing regimes in high-nickel NCM cathodes.•Enabled surfac...

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Vydáno v:	Materials science & engineering. B, Solid-state materials for advanced technology Ročník 323; s. 118801
Hlavní autoři:	Han, Jong Hyeok, Heo, Boseong, Ju, Myeong Jin, Kim, Youngjin, Chang, Joon Ha, Jeon, Hee-Jae
Médium:	Journal Article
Jazyk:	angličtina
Vydáno:	Elsevier B.V 01.01.2026
Témata:	Automated crystallographic characterization High-nickel cathode materials Image processing algorithms Li/Ni mixing Lithium-ion batteries Lithium-ion batteries Automated crystallographic characterization Li/Ni mixing High-nickel cathode materials Image processing algorithms
ISSN:	0921-5107
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Shrnutí:	•Developed an automated HAADF-STEM image-analysis framework eliminating observer bias.•Established an angular-deviation and regional-classification methodology for quantitative structural assessment.•Quantitatively discriminated Li/Ni cation mixing regimes in high-nickel NCM cathodes.•Enabled surface-specific evaluation of washing treatment effects through statistically rigorous image analysis. Quantitative assessment of Li/Ni mixing phenomena in high-nickel layered oxide cathode materials for lithiuim-ion batteries (LIBs) remain constrained by subjective visual interpretation limiting reproducibility and statistical rigor in atomic-scale characterization. Systematic image processing methodology incorporating Gaussian convolution filtering, adaptive threshold segmentation, morphological boundary refinement, and circular Hough transform detection enables automated extraction of crystallographic descriptors from atomic-scale images while eliminating observer-dependent interpretation variabilities. Comprehensive structural analysis reveals disparities between distinct Li/Ni mixing regimes, with inadequate cation interdiffusion exhibiting substantially elevated angular deviation frequencies and extensive misaligned region compared to enhanced mixing conditions. Crystallographic parameter investigation demonstrates interlayer spacing variations that reflect preservation of layered structure with compositional heterogeneities versus thermodynamically favorable arrangements. The underlying thermodynamics elucidates counterintuitive relationships wherein enhanced Li/Ni mixing promotes structural coherence through cooperative cation rearrangement approaching minimum energy configurations. These protocols achieve exceptional reproducibility, enabling systematic structure–property correlations essential for data-driven optimization in advanced material development.
ISSN:	0921-5107
DOI:	10.1016/j.mseb.2025.118801