Atomic-Level Insight into Optimizing the Hydrogen Evolution Pathway over a Co-1-N-4 Single-Site Photocatalyst

作者：Cao, Yuanjie; Chen, Si; Luo, Qiquan; Yan, Huan; Lin, Yue; Liu, Wei; Cao, Linlin; Lu, Junling^*; Yang, Jinlong; Yao, Tao^*; Wei, Shiqiang

来源：Angewandte Chemie - International Edition, 2017, 56(40): 12191-12196.

DOI：10.1002/anie.201706467

• atomic layer deposition
• cobalt
• graphitic carbon nitride
• photocatalytic hydrogen evolution
• single site catalysts

Knowledge of the photocatalytic H-2 evolution mechanism is of great importance for designing active catalysts toward a sustainable energy supply. An atomic-level insight, design, and fabrication of single-site Co-1-N-4 composite as a prototypical photocatalyst for efficient H-2 production is reported. Correlated atomic characterizations verify that atomically dispersed Co atoms are successfully grafted by covalently forming a Co-1-N-4 structure on g-C3N4 nanosheets by atomic layer deposition. Different from the conventional homolytic or heterolytic pathway, theoretical investigations reveal that the coordinated donor nitrogen increases the electron density and lowers the formation barrier of key Co hydride intermediate, thereby accelerating H-H coupling to facilitate H-2 generation. As a result, the composite photocatalyst exhibits a robust H-2 production activity up to 10.8molh(-1), 11 times higher than that of pristine counterpart.

• 出版日期2017-9-25
• 单位中国科学技术大学