Electron Configuration Modulation of Nickel Single Atoms for Elevated Photocatalytic Hydrogen Evolution. Issue 17 (9th March 2020)

• Record Type: Journal Article
• Authors: Jin, Xixiong; Wang, Rongyan; Zhang, Lingxia; Si, Rui; Shen, Meng; Wang, Min; Tian, Jianjian; Shi, Jianlin
• Is Part Of: Angewandte Chemie international edition. Volume 59:Issue 17(2020)
• Page Start: 6827
• Page End: 6831
• Publication Date: 2020-03-09
• Subjects: electronic modulation -- photocatalysis -- polymeric carbon nitride -- single-atom catalysts -- transition metals; Chemistry -- Periodicals; 540
• DOI: 10.1002/anie.201914565
• Languages: English
• ISSNs: 1433-7851

Abstract

Abstract: The emerging metal single‐atom catalyst has aroused extensive attention in multiple fields, such as clean energy, environmental protection, and biomedicine. Unfortunately, though it has been shown to be highly active, the origins of the activity of the single‐atom sites remain unrevealed to date owing to the lack of deep insight on electronic level. Now, partially oxidized Ni single‐atom sites were constructed in polymeric carbon nitride (CN), which elevates the photocatalytic performance by over 30‐fold. The 3d orbital of the partially oxidized Ni single‐atom sites is filled with unpaired d‐electrons, which are ready to be excited under irradiation. Such an electron configuration results in elevated light response, conductivity, charge separation, and mobility of the photocatalyst concurrently, thus largely augmenting the photocatalytic performance. Abstract : The high catalytic activity of metal single atoms originates from their unique electronic configuration. By finely tuning the oxidation states of metal single atoms, their electronic configurations were modulated, resulting in more unpaired d‐orbital electrons and a markedly elevated photocatalytic activity.