Since Ascension: Storm of Souls is both a standalone and expansion to Ascension: Chronicle of the Godslayer, is there any reason to buy COTG? SOS adds new mechanics and seems to have better artwork.
I own all of the Ascension blocks and personally play CotG the most since the minimal mechanics allow it to be more accessible to my wife. I find it as a good introduction into the world of Ascension and then once she becomes more comfortable with it, I'll pull out the other blocks :-)
Not to be Captain Obvious, but you would buy CotG if you want the cards.
I quickly glanced at the card list and a few "must-haves" stuck out:
Enlightened: Master Dhartha, Twofold Askara, and Tablet of Time's Dawn (though you might NOT want the possibility of infinitely many turns...)
Mechana: all the constructs in this set are valuable, Burrower Mark II maybe not as much.