The favorable exploitation of carbon nitride (CN) materials in photocatalysis for organic synthesis requires the appropriate fine-tuning of the CN structure. Here, we present a deep investigation of the structure/activity relationship of CN in the photocatalytic perfluoroalkylation of organic compounds. Four types of CN bearing subtle structural differences were studied via conventional characterization techniques and innovative nuclear magnetic resonance (NMR) experiments, correlating the different structures with the fundamental mechanistic nexus and especially highlighting the importance of the halogen bond strength between the reagent and the catalyst surface. The optimum catalyst exhibited an excellent performance, with a very wide reaction scope, and could prominently trigger the model reaction using natural sunlight. The work lays a platform for establishing a new approach in the development of heterogeneous photocatalysts for organic synthesis related to medical, agricultural, and material chemistry.

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Over the last decades, organic chemistry has taken a resolute step towards green catalytic synthesis. This tries to ensure efficient and sustainable base chemical production, while also safeguarding human health and environment. To this end, the development of novel, non-toxic and effective catalytic systems, capable of driving value-added chemical transformations in environmentally benign solvents (e. g. water) is highly desirable. Moreover, these new catalysts need to be metal-free, easy to prepare and potentially recyclable. Carbon dots, that are relatively new carbon-based nanoparticles, fulfil all these requirements owing to their outstanding physico-chemical features, thus emerging as promising nano-catalytic platforms. This Perspective highlights the recent advances in carbon dots synthesis and their applications in organic catalysis and photocatalysis, with particular attention to green non-metal-doped systems. Finally, forward-looking opportunities within this field are mentioned here.