What are you trying to cool with an 80W TEC? I don't think it's going to get you where you want to go if you are gonna put it on a CPU.
As for what rail to put the pelt on you should look for the voltage it's designed to run at. Assuming it's a 12-15V pelt you should do ok running it on your PSU's +12v line. If it's an 18-24V pelt though you'll need another type of psu.
In any case, you'll probably need to put a load on the 5V line as well so you are getting a true 12V to the peltier. Otherwise it'll run more like 11.5V
Yes you'll want to get a cold plate with your peltier and choose a setup that allows you to really tighten down the peltier between your waterblock and the coldplate. Adequate TEC clamping pressure is an extremely important variable in peltier cooling.
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