Abstract Because of their possible role as model compounds for the structural units of carbon nitride C 3 N 4, the preparation, structural chemistry, and some representative reactions of tetra (amino) methanes have been (re) investigated. In the crystal, C (NMe 2) 4 (1) has a molecular geometry close to D 2a symmetry as proposed by theoretical calculations using state-of-the-art density functional methods. The coordination of the ...