Nitrogen-Rich Tetrazole–Amide-Functionalised Zn Metal–Organic Framework as Catalyst for Efficient Catalytic CO2 Cycloaddition with Epoxides

Paul, Anup; Garazade, Ismayil M.; Karmakar, Anirban; Khan, Rais Ahmad; Guedes da Silva, Maria Fátima C.; Nunes, Ana V. M.; Pombeiro, Armando J. L.

http://hdl.handle.net/10362/165592

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Autores

Guedes da Silva, Maria Fátima C.

Nunes, Ana V. M.

Pombeiro, Armando J. L.

Resumo(s)

In this study, we report the design, synthesis, and catalytic application of the novel nitrogen-rich Zn(II) MOF [Zn2(μ3-1κN,2κN′,3κO-HL)2(DMF)2]n·nH2O (HL2− = 4-((4-(1H-tetrazol-5-yl)phenyl)carbamoyl)benzoate), denoted as ZnMOF, for the efficient conversion of carbon dioxide (CO2) to cyclic carbonates via cycloaddition with epoxides. It was synthesised from a tetrazole appended amide-functionalised pro-ligand (H3L) and Zn(NO3)2·6H2O under hydrothermal conditions. The synthesised material was characterised namely by elemental analysis, infrared spectroscopy, powder X-ray diffraction (PXRD), and single-crystal X-ray diffraction analyses. The catalytic potential of ZnMOF was investigated in the CO2 cycloaddition reaction with various epoxides, with conversions ranging from 17% to 99%. The catalyst retained its activity across multiple reaction cycles, demonstrating its stability and reusability. The influence of co-catalysts on the reaction was explored, with tetrabutylammonium bromide (TBABr) emerging as the most effective one. A plausible reaction mechanism is proposed.

Descrição

This research was funded by the FCT and IST, Portugal, for financial support through “DL/57/2017” (contract no. IST-ID/197/2019). I.M.G. is grateful to the State Program for Increasing the International Competitiveness of the higher education system of the Republic of Azerbaijan in 2019–2023, Ministry of Science and Education Republic of Azerbaijan. R.A.K. gratefully acknowledged Researchers Supporting Project (Project number, RSP2023R400), King Saud University, Riyadh, KSA. Publisher Copyright: © 2023 by the authors.