3DPrinting
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A couple of quick things I see as an old toolmaker.
The first photo looks pretty darned good actually. Nicely textured and worn rustic. The top of the mold as filled nicely and it has dried without warping from what I can tell. The flashing around the bottom of the tile is to be expected and required for air and excess material to escape and allow for better fill. It can be simply removed with say, a dremel tool.
To get your material to fill better with the paper medium, you will need to either apply more pressure, which probably will not do your 3D printed mold much good. Or you need to use a wetter and looser material to get it to flow better and more easily. A more finely ground material will also flow better than paper that is simply torn into little pieces by hand. A tighter fit between the plunger and the frame of the mold with also increase the detail of the edges. But you still need to allow room for air and excess material to escape.
As far as mold release, you probably need to finish the inside of your mold better. Those layer lines will act like little velcro hooks. Sanding, filling, and painting to a smooth surface is a requirement for a good release. With a proper finished mold surface, a light spray of PAM cooking oil should be all you need for this.
Thanks for the input, once I'm home I'll sand the interior walls a bit and maybe add a thin layer of resin and cure in order to leave it smooth.
I'll also look into getting something to better grind the paper, as I used a "retired" hand blender after I left the paper on hot water for a couple of hours. The paper kept getting stuck in the upper dome, making the blades useless.
Yeah, you might want to grind your paper dry to prevent that.