I'll reply from a purely theoretical standpoint, since I freely admit that I've never used peltiers.
First thing to check before you ordered the peltiers would be to run a simulation of your heatload on the two peltiers. The manufacturers often provide a program or web app to estimate what wattage you need for a certain target temp. I don't think your current temps are bad for the setup that you have.
But.... you might have insufficient clamping pressure. Your voltage seems good, you have a cold plate and water cooling... unless the peltiers aren't getting enough cooling, you may be at the optimum for the equipement you have.
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