Keep bumping up the the Vcore, PPL and MCH core slowly, putting emphasis on the Vcore rather than the PPL for longevity and stability. Raising the RAM timings was probably a good idea. I'd also raise the memory voltage a bit too but how far depends on how cool they stay and how well your MCH is cooled. Probably not over 2.2v for the memory.
From there it's just a matter of getting a feel for how much headroom you've gained by upping voltages. If you're experiencing instability just inch clocks down a little and voltages up a little.
Is your MCH passively or actively cooled? You're not going to get far without a fan, often replacing the default ones even. If your MCH is pretty warm to touch at stock voltages/speeds, I wouldn't recommend using much more than the CPU voltages for results. You may not get very far with just those though.