Ni single atoms on carbon nitride for visible-light-promoted full heterogeneous dual catalysis

• Published in: Chemical science (Cambridge) 2022-07, Vol.13 (29), p.8536-8542
• Main Authors: Kwak, Minjoon, Bok, Jinsol, Lee, Byoung-Hoon, Kim, Jongchan, Seo, Youngran, Kim, Sumin, Choi, Hyunwoo, Ko, Wonjae, Hooch Antink, Wytse, Lee, Chan Woo, Yim, Guk Hee, Seung, Hyojin, Park, Chansul, Lee, Kug-Seung, Kim, Dae-Hyeong, Hyeon, Taeghwan, Yoo, Dongwon
• Format: Article
• Language: English
• Subjects: Carbon; Carbon nitride; Catalysis; Chemistry; Fine chemicals; Substrates; Transition metals
• ISSN: 2041-6520; 2041-6539
• DOI: 10.1039/d2sc02174a

Visible-light-driven organic transformations are of great interest in synthesizing valuable fine chemicals under mild conditions. The merger of heterogeneous photocatalysts and transition metal catalysts has recently drawn much attention due to its versatility for organic transformations. However, these semi-heterogenous systems suffered several drawbacks, such as transition metal agglomeration on the heterogeneous surface, hindering further applications. Here, we introduce heterogeneous single Ni atoms supported on carbon nitride (NiSAC/CN) for visible-light-driven C-N functionalization with a broad substrate scope. Compared to a semi-heterogeneous system, high activity and stability were observed due to metal-support interactions. Furthermore, through systematic experimental mechanistic studies, we demonstrate that the stabilized single Ni atoms on CN effectively change their redox states, leading to a complete photoredox cycle for C-N coupling. In this work, the first demonstration of heterogeneous photoredox C-N coupling is reported using Ni atoms on C 3 N 4 . Due to metal-support interactions, high activity and stability were observed during visible-light-driven C-N functionalization.