Hi,
the typical frequency limit for your lyon module set (if you are talking about a 68020 module set) is 24,576 MHz, but obviously some do not work above 22 MHz - don't ask me why.
You need the corresponding crystal of course and a CPU able to work at these frequencies. IIRC 16 MHZ CPUs will work up to 24 MHz. Next you have to change the display module too, as the original display don't support such frequencies. Unfortunately it seems, that these displays are not available anymore.
I never got such a module set, nor i ever tuned one. Maybe someone else can tell you some more. As you tell us about your reasonable background, you might simply swap the crystal and check out for the highest possible frequency, your module set will work without any other changes. I don't think, there would be any risk. I guess, your module set is working at 12,288 MHz at the moment? Just try a 18,432 MHz crystal to get a 50% speed up. Either your module set will run stable, or it just do not start. In the ladder case you may try some slower crystals.
Concerning the Genius module set i don't know anything about tuning opportunities. Isn't it a 68030 Module set, already working at 33 MHz? I guess, there is no reasonable tuning possible, as long as you don't want to spend thousands of dollars, changing the whole system to a fast 68060 CPU...
Kind regards, Willi