Hazzah! I've finally figured out the process for casting the horses for the carousel.
Originally, the goal was to make a silicone mold of a horse that I sculpted, and then cast a silicone horse (with an armature inside) within that mold. From there, the plan was to make 12 molds of the silicone horse in the 12 positions of the zoetrope... but... making the silicone horse with the armature was A LOT more challenging than anticipated.
The silicone was too dense before it cured to get into all of the fine details of the mold—especially the legs of the horse. Once cured the silicone was not dense enough and even the most flexible armatures were tearing through. I began looking for a new material to cast in.
The solution that I have found is casting the horses in a two part urethane plastic with an armature. Although the product is fairly brittle, I am able to heat the plastic after curing and bend the legs into position. The armature holds the legs together where any cracks form, and I fill the cracks with Magic Sculpt (a resin with hardens overnight). This technique makes it so that I do not have to make an additional 12 molds and casts!
I have also started testing options for the paint pallet: