Structure optimization of photocatalyst graphitic carbon nitride (CN) is still a key endeavor. CN nanosheets were prepared via a facile one-pot copolymerization process, incorporating electron-withdrawing groups 5-cyanopyrimidine (CPM) and melamine under calcination. The synergistic effect of molecular doping and thermal induction effectively modulates the intrinsic electronic and band structure of CN. The post-optimized sample (CNM) exhibits a higher reduction potential, reduced nanosheet thickness, stronger crystallinity, and enhanced electron-holes separation efficiency, compared to pristine CN (CNM). Notably, significant morphological and textural alterations were observed in the modified CNM samples. Consequently, a remarkable enhancement in visible-light photocatalytic H evolution and CO reduction performance was achieved. Specifically, the CNM retained an H evolution rate of 166.4 µmol·h, which was 14.8-fold higher than that of CNM (11.3 µmol·h), along with a 31.6-fold increase in CO evolution efficiency. Molecular and textural engineering demonstrate their universal applicability for different comonomers. This study showcases the feasibility of synergizing thermal induction and copolymerization strategies for synthesizing high-efficiency CN-based photocatalysts with unique topology and structural precision.

中文翻译：

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氮化碳的协同共聚和热诱导：增强光催化性能和机理洞察

光催化剂石墨氮化碳（CN）的结构优化仍然是一个关键工作。CN 纳米片是通过简单的一锅共聚工艺制备的，在煅烧下掺入吸电子基团 5-氰基嘧啶 (CPM) 和三聚氰胺。分子掺杂和热感应的协同效应有效地调节了CN的本征电子和能带结构。与原始 CN (CNM) 相比，优化后的样品 (CNM) 表现出更高的还原电位、减小的纳米片厚度、更强的结晶度和增强的电子空穴分离效率。值得注意的是，在修改后的 CNM 样品中观察到显着的形态和结构变化。因此，可见光催化析氢和二氧化碳还原性能显着增强。具体而言，CNM 保留了 166.4 µmol·h 的 H 析出速率，比 CNM（11.3 µmol·h）高 14.8 倍，CO 析出效率提高了 31.6 倍。分子和结构工程证明了它们对不同共聚单体的普遍适用性。这项研究展示了协同热诱导和共聚策略来合成具有独特拓扑和结构精度的高效CN基光催化剂的可行性。