Dual-Function HKUST-1: Templating and Catalyzing Formation of Graphitic Carbon Nitride Quantum Dots Under Mild Conditions

Angew Chem Int Ed Engl. 2020 Nov 23;59(48):21499-21504. doi: 10.1002/anie.202009710. Epub 2020 Sep 17.

Abstract

Graphitic carbon nitride quantum dots (g-CNQDs) are highly promising photoresponsive materials. However, synthesis of monodispersed g-CNQDs remains challenging. Here we report the dual function of MOF [Cu3 BTC2 ] (HKUST-1) as a catalyst and template simultaneously to prepare g-CNQDs under mild conditions. Cyanamide (CA), a graphitic carbon nitride precursor, catalytically dimerized inside the larger MOF cavities at 90 °C and condensed into g-CNQDs at 120 °C in a controlled fashion. The HKUST-1 template was stable under the reaction conditions, leading to uniform g-CNQDs with a particle size of 2.22±0.68 nm. The as prepared g-CNQDs showed photoluminescence emission with a quantum yield of 3.1 %. This concept (MOF dual functionality) for catalyzing CA polycondensation (open metal sites (OMSs) effect) and controlling the produced particle size (pore-templating effect), together with the tunable MOF porosity, is expected to produce unique g-CNQDs with controllable size, morphology, and surface functionality.

Keywords: HKUST-1; MOF templating; cyanamide polycondensation; g-CNQDs; photoluminescence.