Spatial Heterogeneity and Strong Coupling of Fe<sup>II</sup>/Fe<sup>III</sup> in an Individual Metal‐Organic Framework Nanoparticle for Efficient CO<sub>2</sub> Photoreduction
Yanting Zheng, Xiaoxin Shen, Mingxiong Lin, Mengyao Zhu, Bixia Yang, Jiawei Yan, Zanyong Zhuang, Yan Yu
Abstract
Abstract The synthesis and characterization of an Fe II /Fe III metal‐organic framework (MOF) nanocrystal with spatial heterogeneity that arises from the non‐uniform distribution of different valence states is disclosed. The Fe II /Fe III ‐Ni Prussian blue analog (PBA) delivers superior photocatalytic performance in the selective CO 2 reduction reaction thanks to the strong Fe II /Fe III coupling, with CO yield up to 12.27 mmol g −1 h −1 and 90.6% selectivity under visible‐light irradiation. Density functional theory calculation and experimental studies prove that the spatial heterogeneity of Fe II /Fe III in the individual MOF nanocrystal not only directs and expedites the charge transfer within a catalyst particle but also creates the heterogeneity of catalytically‐active Ni sites for efficient CO 2 photoreduction. The current findings add to a growing literature of materials with compositional heterogeneity and provide a reference for future research.