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Triggering Lewis Acidic Nature through the Variation of Coordination Environment of Cd-Centers in 2D-Coordination Polymers

Cite this: Inorg. Chem. 2020, 59, 2, 1284–1294
Publication Date (Web):January 9, 2020
https://doi.org/10.1021/acs.inorgchem.9b02997
Copyright © 2020 American Chemical Society

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    Abstract

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    The rational design and successful synthesis of novel functional metal–organic frameworks relies on careful selection of metals and versatile organic ligands. A newly designed pyrazole-based dicarboxylate ligand, 5-(3,5-dimethyl-1H-pyrazol-1-yl) 1,3-benzenedicarboxylic acid (H2L), was utilized to obtain two new Cd-based coordination polymers I [Cd(L)(H2O)]·H2O and II [Cd(L)] under similar reaction conditions via solvothermal strategy. Single-crystal X-ray data confirmed that compound I exhibits a two-dimensional (2D) skeleton comprising pentagonal bipyramidal Cd-ions and an organic ligand moiety. Compound II has also formed a two-dimensional layer arrangement with the connectivity between trigonal bipyramidal Cd-ions and the organic ligand. Topological analysis revealed that compound I has formed unique 43.63 net topology while compound II has displayed a 44.62sql net topology with 2D frameworks. The Lewis acidic nature of both I and II containing a Cd2+ metal center has been correlated with the coordination number through dye adsorption–desorption and catalysis studies. The selective adsorption of anionic dye and the extent of adsorption are interrelated with the Cd-ion geometry. For the first time, the role of coordinated water molecule has been analyzed through heterogeneous catalysis reaction (i.e., cyanosilylation) with Cd-based 2D-coordination polymers (CPs). The plausible mechanisms have been proposed to explain the subsequent role of coordination number and environment in CPs.

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.inorgchem.9b02997.

    • Synthesis of the ligand, tables for bond length, bond angles, adsorption–desorption efficiency and catalytic activity, PXRD, IR, TGA, NMR, mass spectrometry results, a few figures of crystal structures, and adsorption–desorption plots (PDF)

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    CCDC 19508071950809 contain the supplementary crystallographic data for this paper. These data can be obtained free of charge via www.ccdc.cam.ac.uk/data_request/cif, or by emailing [email protected], or by contacting The Cambridge Crystallographic Data Centre, 12 Union Road, Cambridge CB2 1EZ, UK; fax: +44 1223 336033.

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