Collaboration between Iridium Clusters and the {111} Dominant Facet of Cu<sub>2</sub>O for Triggering Efficient N<sub>2</sub> Photofixation
Wensheng Zhang, Qingmei Tan, Tianren Liu, Zhishan Liang, Youlin Huang, Ying He, Dongxue Han, Dongdong Qin, Li Niu
Abstract
The exploration of advanced photocatalysts for efficient N 2 reduction reaction (NRR) by integrating facet-engineering and realistic N 2 active sites is very promising, but it remains a challenge due to the absence of rational structural design and atomic-level insights into molecular N 2 activation. Herein, the same main group transition metal (e.g., Co, Rh, and Ir) clusters were ingeniously modified onto the dominant {111} crystal facet of Cu 2 O nanocrystal, aiming to track the synergistic effect of various N 2 active sites and facet-engineering for efficient N 2 photofixation. Intriguingly, further theoretical studies reveal that the incorporating Ir clusters can improve light absorption ability, accelerate photogenerated charge separation and transfer, and lower the reaction energy barrier, thereby expressively promoting the real photoreactivity. The present work offers a promising approach to cooperatively regulate the facet-engineering and N 2 active centers at the atomic level, expecting to guide innovative design of smart NRR systems.