Synthesis of pyrimidines from dinitrogen and carbon

The element nitrogen and nitrogenous compounds are vital to life. The synthesis of nitrogen-containing compounds using dinitrogen as the nitrogen source, not through ammonia, is of great interest and great value but remains a grand challenge. Herein, we describe a strategy to realize this transformation by combining the heterogeneous approach with the homogeneous methodology. The N(2) molecule was first fixed with carbon and LiH through a one-pot heterogeneous process, forming Li(2)CN(2) as an ‘activated’ nitrogen source with high efficiency. Then subsequent homogeneous treatments of Li(2)CN(2) to construct the organic synthon carbodiimide and the RNA/DNA building block pyrimidines were fulfilled. By using (15)N(2) as the feedstock, their corresponding (15)N-labeled carbodiimide and pyrimidines were readily obtained. This homogeneous–heterogeneous synergy strategy will open a new chapter for N(2) transformation.