Successive impingement of droplets after refining in supersonic plasma jet generally yields a submicron-sized lamellar coating with excellent comprehensive properties. Nevertheless, physical insight into the flattening and rapid solidification with crystallization behavior of supersonic impingement of refined droplets is difficult to understand. In this research, the content of refinement droplets reached 90% and displayed the multi-scale distribution of equiaxed grains. The boundary migration of equiaxed grains and anisotropic coalescence was found in the dynamic temperature gradient. Furthermore, an optimized model was established in order to accurately reproduce the multi-physical coupling process of supersonic impingement of single or two refined droplets, which was based on the numerical calculation of nonlinear equations (including the Mass and momentum, energy balance, Cahn–Hilliard, phase-field and orientational field equations). The size distribution and growth orientation of columnar grains within single or two flattened droplets were in good agreement with the experimental results. Epitaxial growth of columnar grains was found in the two-flattened droplet interface during the extremely rapid cooling stage. This optimized model could be an effective method in predicting the flattening and solidification with crystallization behavior of droplets during plasma spraying.
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