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Single-atom Engineering of Directional Charge Transfer Channels and Active Sites for Photocatalytic Hydrogen Evolution 
S. Cao, H. Li, T. Tong, H.-C. Chen, A. Yu, J. Yu*, and H. M. Chen* 
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.