In general, you can specify the primary and secondary phases whichever way you prefer. It is a good idea, especially in more complicated problems, to consider how your choice will affect the ease of problem setup.
Also refer to this forum discussion: https://forum.ansys.com/forums/topic/secondary-mixture-phase-in-vof-model/
To understand more please refer theory guide: https://ansyshelp.ansys.com/account/secured?returnurl=/Views/Secured/corp/v222/en/flu_th/flu_th_sec_multiphase_vof.html
If you are not able to access the link, please refer to this forum discussion: Using Help with links (ansys.com)
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