Porous graphitic framework (PGF) is a two-dimensional (2D) material that has emerging energy applications. An archetype contains stacked 2D layers, the structure of which features a fully annulated aromatic skeleton with embedded heteroatoms and periodic pores. Due to the lack of a rational approach in establishing in-plane order under mild synthetic conditions, the structural integrity of PGF has remained elusive and ultimately limited its material performance. Here, we report the discovery of the unusual dynamic character of the C=N bonds in the aromatic pyrazine ring system under basic aqueous conditions, which enables the successful synthesis of a crystalline porous nitrogenous graphitic framework with remarkable in-plane order, as evidenced by powder X-ray diffraction studies and direct visualization using high-resolution transmission electron microscopy. The crystalline framework displays superior performance as a cathode material for lithium-ion batteries, outperforming the amorphous counterparts in terms of capacity and cycle stability.

多孔石墨骨架（PGF）是具有新兴能源应用的二维（2D）材料。原型包含堆叠的2D层，其结构具有带有嵌入的杂原子和周期性孔的完全环状芳族骨架。由于缺乏在温和的合成条件下建立面内秩序的合理方法，PGF的结构完整性仍然难以捉摸，并最终限制了其材料性能。在这里，我们报告了在碱性水溶液条件下在芳香族吡嗪环系统中C = N键异常动态特征的发现，这使得成功合成具有显着面内顺序的结晶性多孔氮石墨骨架成为可能，粉末X射线衍射研究和使用高分辨率透射电子显微镜的直接可视化证明了这一点。晶体框架作为锂离子电池的正极材料表现出卓越的性能，在容量和循环稳定性方面优于非晶态晶体。