This is good info.
According to estimations on the Atari CT60 page, something like 70% of the first masks can do 66MHz. Those are pretty good odds IMHO.
At what point do you find that you have to bump up the voltage?
If so, do you think that is due to the CPU or the board components? The board could easily be the weak link, they are using very old technology.
The Replay daughter boards seem to be having good luck with higher speeds, but of course the components are new and very fast compared to those from 1996.