Tailored amorphization of graphitic carbon nitride triggers superior photocatalytic C–C coupling towards the synthesis of perfluoroalkyl derivatives

Francesco Longobardo; Giuseppe Gentile; Alejandro Criado; Arianna Actis; Sara Colussi; Vladimiro Dal Santo; Mario Chiesa; Giacomo Filippini; Paolo Fornasiero; Maurizio Prato; Michele Melchionna

doi:10.1039/D1QM01077H

Tailored amorphization of graphitic carbon nitride triggers superior photocatalytic C–C coupling towards the synthesis of perfluoroalkyl derivatives†

Francesco Longobardo,

^a Giuseppe Gentile,^a Alejandro Criado,

^b Arianna Actis,^c Sara Colussi,

^d Vladimiro Dal Santo,^e Mario Chiesa,

^c Giacomo Filippini,

*^a Paolo Fornasiero,

^afg Maurizio Prato

^afhi and Michele Melchionna

*^af

Author affiliations

* Corresponding authors

^a Department of Chemical and Pharmaceutical Sciences, University of Trieste, Via L. Giorgieri 1, 34127 Trieste, Italy
E-mail: melchionnam@units.it, gfilippini@units.it

^b Universidade da Coruña, Centro de Investigacións Científicas Avanzadas (CICA), Rúa As Carballeiras, A Coruña, Spain

^c Department of Chemistry and NIS Centre of Excellence, University of Torino, Via Giuria 9, 10125 Torino, Italy

^d Dipartimento Politecnico, University of Udine, Unità di Ricerca INSTM Udine, via del Cotonificio 108, 33100 Udine, Italy

^e Consiglio Nazionale delle Ricerche – Istituto di Scienze Tecnologie Chimiche “Giulio Natta” (CNR-SCITEC), Via C. Golgi 19, I-20133 Milano, Italy

^f Consorzio Interuniversitario Nazionale per la Scienza e Tecnologia dei Materiali (INSTM), Unit of Trieste, via L. Giorgieri 1, 34127 Trieste, Italy

^g Istituto di Chimica dei Composti Organometallici (CNR-ICCOM), Via Madonna del Piano 10, Sesto Fiorentino, Italy

^h Center for Cooperative Research in Biomaterials (CIC biomaGUNE), Basque Research and Technology Alliance (BRTA), San Sebastián, Spain

ⁱ Ikerbasque, Basque Foundation for Science, Bilbao, Spain

Abstract

In this work, we explored a post-synthetic modification of the well-known graphitic carbon nitride (g-CN) by means of an “amorphization” treatment and evaluate the resulting change in photocatalytic activity towards the synthesis of valuable perfluoroalkyl derivatives. The as-prepared “super-amorphous” CN (SACN) exhibits a significant increase of the photocatalytic activity (up to a six-fold enhancement with the optimum structure with respect to g-CN), which originates from the lower degree of crystallinity of the CN and its reduced bandgap. The SACN photocatalysts display versatility and good tolerance towards functional group variations of the reagents, emerging as a potential new benchmark CN structure for heterogeneous organic photocatalysis.

Materials Chemistry Frontiers

Tailored amorphization of graphitic carbon nitride triggers superior photocatalytic C–C coupling towards the synthesis of perfluoroalkyl derivatives†

Abstract

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Tailored amorphization of graphitic carbon nitride triggers superior photocatalytic C–C coupling towards the synthesis of perfluoroalkyl derivatives

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