Synthesis of Pyrimidines from Dinitrogen and Carbon

Xianghui Shi^#, Qianru Wang^#, Chao Qin^#, Li-Jun Wu, Yuanjin Chen, Gao-Xiang Wang, Yongli Cai, Wenbo Gao, Teng He, Junnian Wei*, Jianping Guo*, Ping Chen*, Zhenfeng Xi*.

Natl. Sci. Rev. 2022. DOI: 10.1093/nsr/nwac168. (^#Authors contributed equally.)

  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 N₂ molecule was first fixed with carbon and LiH through a one-pot heterogeneous process, forming Li₂CN₂ as an ‘activated’ nitrogen source with high efficiency. Then subsequent homogeneous treatments of Li₂CN₂ to construct the organic synthon carbodiimide and the RNA/DNA building block pyrimidines were fulfilled. By using ¹⁵N₂ as the feedstock, their corresponding ¹⁵N-labeled carbodiimide and pyrimidines were readily obtained. This homogeneous-heterogeneous synergy strategy will open a new chapter for N₂ transformation.