When I looked >= 1-2 years ago, the best single set for spare parts I found was the Volvo L350F wheel loader aka. "42030" [1] (each lego set is uniquely identified by a numeric id). It had the most power functions parts I could find, and probably gives you all the beams, wheels, gears, and other parts you need.
You can supplement your collection with specific parts from places like BrickLink [2] or even the lego.com store [3].
NOTE: Be warned that LEGO is changing their Power Functions plug shape. Most current sets are still on Power Functions 1.0, and new sets will eventually become 2.0
[1] https://www.amazon.com/technic-Volvo-L350F-wheel-loader/dp/B...
42043: - contains the pneumatic pump & tubes which are less common pieces - this is the only other large technic set I've bought (and I got it mainly for the pneumatic parts)
42009: - Lots of beam parts, but not many power functions parts included.