A series of 2-aminopyrimidine derivatives, substituted at 5-and 6-positions, were synthesized. The reaction was carried out in a single step by treatment of the corresponding β-ketoester or β-aldehydoester with guanidine hydrochloride in the presence of K2CO3, in a microwave-assisted method without the requirement of solvent. A unique 1: 1 co-crystal structure was obtained which shows that a 6-phenyl-2-aminopyrimidinone forms a strong ...