A practical and scalable protocol for visible‐light‐accelerated arylation and alkylation of quinoxalin‐2(1H)‐ones with hydrazines is reported. In this protocol, a hydrazone‐based two‐dimensional covalent organic frameworks (2D‐COF‐1) was employed as the heterogeneous photocatalyst (PC). Due to its excellent photocatalytic properties, good chemical stability and heterogeneous nature, the present method exhibits high efficiency, good functional group tolerance, easy scalability and remarkable catalyst reusability. More importantly, it provides an alternative way that allows rapid access to various C3 arylated or alkylated quinoxalin‐2(1H)‐ones in a greener and sustainable manner.

A heterogeneous visible-light-induced tandem radical addition–cyclization of isocyanides by photoactive covalent organic frameworks was developed, delivering diverse phenanthridines with high reaction efficiency and easy catalyst recyclability.

The application of two-dimensional covalent organic frameworks (2D-COFs) as photoredox catalysts offers a sustainable alternative for visible-light-driven organic transformations. However, under highly complicated organic reaction conditions, maintaining their basic structure...

The merger of transition-metal catalysis and photoredox catalysis enables a balance between the elegant chemical transformation and the rational use of light energy. Previously, it was always accomplished with the...

Photoactive two‐dimensional covalent organic frameworks (2D‐COFs) have become promising heterogenous photocatalysts in visible‐light‐driven organic transformations. Herein, a visible‐light‐driven selective aerobic oxidation of various small organic molecules by using 2D‐COFs as the photocatalyst was developed. In this protocol, due to the remarkable photocatalytic capability of hydrazone‐based 2D‐COF‐1 on molecular oxygen activation, a wide range of amides, quinolones, heterocyclic compounds, and sulfoxides were obtained with high efficiency and excellent functional group tolerance under very mild reaction conditions. Furthermore, benefiting from the inherent advantage of heterogenous photocatalysis, prominent sustainability and easy photocatalyst recyclability, a drug molecule (modafinil) and an oxidized mustard gas simulant (2‐chloroethyl ethyl sulfoxide) were selectively and easily obtained in scale‐up reactions. Mechanistic investigations were conducted using radical quenching experiments and in situ ESR spectroscopy, all corroborating the proposed role of 2D‐COF‐1 in photocatalytic cycle.