I can't see charging the caps higher as being realistic.
Due to the size of the capacitors, I think a decent sized battery in parallel is absolutely necessary: one that can potentially even take a starting load, even if it's not a full sized car battery. Hop in the car, turn the radio and lights on, fiddle with your phone for a minute before leaving, the car doesn't start and you're stranded - that's just not acceptable. Starting at the voltage an alternator charges, you can't have the key in the ignition without starting the car for more than a minute or two.
Given my experience with these, I feel like a set of caps in the range of 1000F+ is more appropriate for starting a car on their own. There's some forgiveness there.
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