Modulation of the charge transfer dynamic in amorphous carbon nitride allotropic heterojunctions by an alternation in bridging functional groups for the heptazine‐ and triazine‐based fragments is demonstrated to boost the photocatalytic activity for hydrogen evolution. Pyrimidine‐bridged and NH‐bridged amorphous carbon nitride allotropic heterojunctions are synthesized by thermal polycondensation of a supramolecular complex. Due to the improved charge separation efficiency and visible‐light harvesting ability, both allotropic heterojunctions present more than tenfold enhanced photocatalytic activities for hydrogen evolution compared to the conventional heptazine‐based carbon nitride under visible‐light illumination. Moreover, the photocatalytic activity of the NH‐bridged carbon nitride allotropic heterojunction with type‐II charge transfer dynamic is superior to the pyrimidine‐bridged one with a Z‐scheme characteristic. The findings in this study emphasize that the electronic structure at the heterojunction interface governed by the bridging group greatly influences the charge transfer dynamic and therefore is a crucial factor driving the photocatalytic activity of carbon nitride allotropic heterojunctions.

中文翻译：

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桥接官能团控制非晶碳氮化物同素异质结中电荷转移的动力学，以实现高效的太阳能氢释放

通过改变基于庚嗪和三嗪的片段的桥接官能团，对无定形碳氮化物同素异质异质结中的电荷转移动力学进行了调节，从而提高了光催化氢的析出活性。嘧啶桥和NH桥的非晶氮化碳同素异质异质结是通过超分子复合物的热缩聚反应合成的。由于提高了电荷分离效率和可见光收集能力，与传统的庚嗪基氮化碳相比，两种同素异质结在可见光照射下均表现出十倍以上的增强光催化活性。此外，具有Ⅱ型电荷转移动力学的NH桥式氮化碳同素异质结的光催化活性优于具有Z方案特性的嘧啶桥式。这项研究的发现强调，由桥基控制的异质结界面上的电子结构会极大地影响电荷转移动力学，因此是驱动氮化碳同素异质结光催化活性的关键因素。