4.8 Article

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

Journal

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 59, Issue 48, Pages 21499-21504

Publisher

WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202009710

Keywords

cyanamide polycondensation; g-CNQDs; HKUST-1; MOF templating; photoluminescence

Funding

  1. Hefei National Laboratory for Physical Sciences at the Microscale, Hefei Science Center of Chinese Academy of Sciences
  2. National Natural Science Foundation of China (NSFC) [21571167, 51502282]
  3. Fundamental Research Funds for the Central Universities [WK2060190053]
  4. Anhui Province Natural Science Foundation [1608085MB28]
  5. CAS-TWAS President's PhD fellowship
  6. Alexander von Humboldt post-doctoral research fellowship
  7. DFG Priority Program 1928 COORNETs
  8. Projekt DEAL
  9. Fujian Institute of Innovation of Chinese Academy of Sciences

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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 [Cu3BTC2] (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 degrees C and condensed into g-CNQDs at 120 degrees 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.

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