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.