I'm not aware of anything that can do that, unfortunately. (and yeah, I misread the first post, whoops)
I had a 75Hz monitor (it's pretty much broken now from age) but EoSD never rose to 75fps, it always stayed at 60, even without vsync. Not sure what ZUN did there if yours goes higher.
Vsync pretty much controls the fps, it can't increase it while making the game play at the same speed as 60 fps. I never knew Touhou was even capable of doing that. Leave it to EoSD to do it, the most finicky of all the games. (PCB can be weird too, but it's more rare) Out of curiosity, does EoSD do that every time you load it up, or only sometimes/rarely?