Efficiency of layered photocatalysts such as graphitic carbon nitride (g‐CN) is still too low due to the poor utilization of photoexcited‐charge carriers. The major drawback is that the weak van der Waals force among g‐CN layers is unfavorable for the charge transfer between the adjacent layers and the intrinsically π‐conjugated planes with inefficient random in‐plane charge migration. Herein, an atomically dispersed Pd layered photocatalyst with both bridged sites of adjacent layers and surface‐sites of g‐CN is demonstrated, providing directional charge‐transfer channels and targeting active sites for photocatalytic water reduction. Both theoretical prediction and empirical characterizations are conducted to achieve the successful synthesis of single‐atom engineered Pd/g‐CN hybrid and the excellent separation of charge transfer as well as the efficient photocatalytic hydrogen evolution, much better than that of the optimized Pt/g‐CN benchmark. The finding in this work provides a rational way for tailoring the performance and engineering of single‐atomic noble metal.

中文翻译：

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定向电荷转移通道和活性位点的单原子工程，用于光催化氢的释放

由于光激发电荷载流子利用率低，层状光催化剂（例如石墨碳氮化物（g-CN））的效率仍然太低。主要缺点是，g-CN层之间较弱的范德华力不利于相邻层与固有π共轭平面之间的电荷转移，且无效率的随机面内电荷迁移。在本文中，展示了原子分散的Pd层状光催化剂，该光催化剂具有相邻层的桥接位点和g-CN的表面位点，提供了定向电荷转移通道并靶向了光催化减水的活性位点。进行理论预测和经验表征均能成功完成单原子工程化Pd / g-CN杂化物的合成，出色的电荷转移分离以及有效的光催化氢释放，远优于优化的Pt / g。 ‐CN基准。这项工作的发现为调整单原子贵金属的性能和工程设计提供了一种合理的方法。