Can the thermodynamic information of a compound be calculated or must it be found emperically?
For gaseous compounds heat of formation can be calculated using quantum chemistry packages as a difference between energies, assigned by the package, though inaccuracies are possible. Entropy of formation is a bit trickier, it requires calculation of vibrational and rotational states, but still pretty straightforward. For condensed phase (liquids, solids) the situation is harder, as knowledge of structure of solid state must be known beforehand, or full exhaustive search of possible crystal structures must be performed.

In practice, however, both heat and entropy of formation are found experimentally.