I worry you will kill off the old hardware if I'm honest.
I had a MK2 which was overclocked and one day it give me a guru meditation error and it has never worked since.
Now you may think the CPU failed but this is not the case the CPU still works fine in my other accelerators.
Sadly these old accelerators have CPLD's which are not able to be duplicated at this moment in time, so when they fail that is usually the end of the card.
In my opinion at most I would not go over the 66mhz when overclocking these cards but that is my opinion.
In regards to my MKII which failed, it was overclocked at 80mhz with cooling on the CPU.
Now I've seen people try heat sinks on the custom chips on the card but there is no definitive proof that this will stop the failure of the CPLD's
Due to these being "Original Hardware" they still hold there value, so please take that in consideration if you do it, because a replacement is not just around the corner