Direct and efficient photocatalytic overall water splitting is crucial for the sustainable conversion and storage of renewable solar energy. Herein, we present the design of a carbon-rich graphitic carbon nitride (C_co-C₃N₄), prepared from a layered molecular cocrystal precursor. The cocrystal microsheets were synthesized using a facile hydrothermal process. Following two-step thermal treatment and liquid exfoliation, the product maintains the 2D morphology owing to the toptactic transformation process. The C_co-C₃N₄ exhibits an enhanced photogenerated electron-hole separation, high charge transport capacity, and prolonged lifetime of the carriers, relative to the g-C₃N₄ system. In the absence of any sacrificial reagent or co-catalyst, the C_co-C₃N₄ microsheets exhibit a high photocatalytic activity. The work presented in this report supplies a cocrystal route for the orderly molecular self-assembly of precursor materials to tailor the chemical compositions and electronic structures. Moreover, the generation of a highly efficient water-splitting photocatalyst has larger implications for sustainable energy applications.

直接和有效的光催化总水分解对于可再生太阳能的可持续转化和存储至关重要。本文中，我们介绍了一种由层状分子共晶前驱体制备的富碳石墨氮化碳（C _co -C ₃ N ₄）的设计。使用方便的水热工艺合成了共晶微片。经过两步热处理和液体剥离后，由于拓扑变换过程，产品保持了2D形态。相对于gC ₃，C _co -C ₃ N ₄表现出增强的光生电子-空穴分离，高电荷传输能力和延长的载流子寿命N ₄系统。在不存在任何牺牲试剂或助催化剂的情况下，C _co -C ₃ N ₄微片表现出高的光催化活性。本报告中介绍的工作为前体材料的有序分子自组装提供了一条共晶途径，以调整化学成分和电子结构。而且，高效水分解光催化剂的产生对于可持续能源应用具有更大的意义。