Orthogonal Dual Photocatalysis of Single Atoms on Carbon Nitrides for One-Pot Relay Organic Transformation.

Kim, Sumin; Bok, Jinsol; Lee, Byoung-Hoon; Choi, Hyunwoo; Seo, Youngran; Kim, Jiheon; Kim, Junhee; Ko, Wonjae et al. · ACS Nano · 2023

basic_science · Level V

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Abstract

Single-atom photocatalysis has shown potential in various single-step organic transformations, but its use in multistep organic transformations in one reaction systems has rarely been achieved. Herein, we demonstrate atomic site orthogonality in the M<sub>1</sub>/C<sub>3</sub>N<sub>4</sub> system (where M = Pd or Ni), enabling a cascade photoredox reaction involving oxidative and reductive reactions in a single system. The system utilizes visible-light-generated holes and electrons from C<sub>3</sub>N<sub>4</sub>, driving redox reactions (e.g., oxidation and fluorination) at the surface of C<sub>3</sub>N<sub>4</sub> and facilitating cross-coupling reactions (e.g., C-C and C-O bond formation) at the metal site. The concept is generalized to different systems of Pd and Ni, thus making the catalytic site-orthogonal M<sub>1</sub>/C<sub>3</sub>N<sub>4</sub> system an ideal photocatalyst for improving the efficiency and selectivity of multistep organic transformations.