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Synthesis and XRD of Novel Ni4(µ3-O)4 Twist Cubane Cluster Using Three NNO Mixed Ligands: Hirshfeld, Spectral, Thermal and Oxidation Properties

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Abstract

A novel [Ni4(µ3-O)4] twisted cubane complex, Ni4Cl2(NN)2(ONN)2(NNO)2(H2O)2·2THF, was prepared from a crude mixture of three bidentate ligands. A mixture of ethyl 1-(hydroxymethyl)-3-methyl-1H-pyrazole-5-carboxylate (HONN) and ethyl 1-(hydroxyl-methyl)-5-methyl-1H-pyrazole-3-carboxylate (NNOH) were added to ethyl 3-methyl-1H-pyrazole-5-carboxylate (NNH) then mixed to NiCl2·6H2O solution under ambient conditions. Reaction progress was monitored via infrared and ultraviolet–visible spectroscopies and energy-dispersive X-ray spectroscopy was used to analyze the product. Reaction yields for cluster synthesis were very good. Single crystal structure determination for the cluster indicates a novel [Ni4(µ3-O)4] twisted cubane structure with octahedral geometry around each of the Ni(II) centers in Ni4Cl2(NN)2(ONN)2(NNO)2(H2O)2·2THF. The lattice is stabilized by hydrogen bonding and H–\( \pi \) stacking. Hirshfeld surface analysis (HSA) corroborates the single crystal structure determination results. The cluster displays significant thermal stability under open atmosphere conditions; it decomposes in three steps at high temperature. The cluster demonstrates promising results as a catalyst; it promoted the complete oxidation of catechol to o-Quinone in under mild conditions.

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Acknowledgements

Researchers Supporting Project number (RSP-2019/78), King Saud University, Riyadh, Saudi Arabia.

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Authors and Affiliations

  1. Laboratory of Applied and Environmental Chemistry (LCAE), Mohammed First University, Oujda, Morocco

    Abderrahim Titi, Rachid Touzani & Belkheir Hammouti

  2. Graduate School of Pure and Applied Sciences, University of Tsukuba, Tennodai 1-1-1, Tsukuba, Ibaraki, 305-8571, Japan

    Hiroki Oshio

  3. Department of Chemistry, Faculty of Science, Taibah University, Al-Madinah Al-Munawarah, Saudi Arabia

    Messali Mouslim

  4. Laboratory of Materials, Nanotechnology and Environment, Faculty of Sciences, Mohammed V University, Av. Ibn Battouta, Box 1014, Agdal-Rabat, Morocco

    Abdelkader Zarrouk

  5. Department of Chemistry, College of Science, King Saud University, Riyadh, 11451, P.O. Box 2455, Saudi Arabia

    Nabil Al-Zaqri & Ali Alsalme

  6. Department of Chemistry and Earth Sciences, Qatar University, PO Box 2713, Doha, Qatar

    Ismail Warad

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  1. Abderrahim Titi
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10876_2020_1780_MOESM1_ESM.docx

Supplementary material 3 (DOCX 414 kb). Fig. 1S Computed (a) dnorm surface, (b) shape index, (c) curvedness structures, and (d) inside/outside two-dimensional fingerprint plots.

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Titi, A., Oshio, H., Touzani, R. et al. Synthesis and XRD of Novel Ni4(µ3-O)4 Twist Cubane Cluster Using Three NNO Mixed Ligands: Hirshfeld, Spectral, Thermal and Oxidation Properties. J Clust Sci 32, 227–234 (2021). https://doi.org/10.1007/s10876-020-01780-0

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