Tetrahydrides crystallizing in the ThCr2 Si2 structure type have been predicted to become stable for a plethora of metals under pressure, and some have recently been synthesized. Through detailed first-principles investigations we show that the metal atoms within these symmetry MH4 compounds may be divalent, trivalent or tetravalent. The valence of the metal atom and its radius govern the bonding and electronic structure of these phases, and their evolution under pressure. The factors important for enhancing superconductivity include a large number of hydrogenic states at the Fermi level, and the presence of quasi-molecular H units whose bonds have been stretched and weakened (but not broken) via electron transfer from the electropositive metal, and via a Kubas-like interaction with the metal. Analysis of the microscopic mechanism of superconductivity in MgH4 , ScH4 and ZrH4 reveals that phonon modes involving a coupled libration and stretch of the H units leading to the formation of more complex hydrogenic motifs are important contributors towards the electron phonon coupling mechanism. In the divalent hydride MgH4 , modes associated with motions of the hydridic hydrogen atoms are also key contributors, and soften substantially at lower pressures.