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Chemical Manipulation of the Spin-Crossover Dynamics through Judicious Metal-Ion Dilution

  • Xiang Li
    Xiang Li
    School of Chemistry and Chemical Engineering, Nanjing University of Science and Technology, Nanjing 210094, P. R. China
    More by Xiang Li
  • Dong Zhang
    Dong Zhang
    School of Chemistry and Chemical Engineering, Nanjing University of Science and Technology, Nanjing 210094, P. R. China
    More by Dong Zhang
  • Yuqing Qian
    Yuqing Qian
    School of Chemistry and Chemical Engineering, Nanjing University of Science and Technology, Nanjing 210094, P. R. China
    More by Yuqing Qian
  • Wenxuan Liu
    Wenxuan Liu
    School of Chemistry and Chemical Engineering, Nanjing University of Science and Technology, Nanjing 210094, P. R. China
    More by Wenxuan Liu
  • Corine Mathonière*
    Corine Mathonière
    Univ. Bordeaux, CNRS, CRPP, UMR 5031, F-33600 Pessac, France
    Univ. Bordeaux, CNRS, Bordeaux INP, ICMCB, UMR 5026, F-33600 Pessac, France
    *Email: [email protected]
  • Rodolphe Clérac*
    Rodolphe Clérac
    Univ. Bordeaux, CNRS, CRPP, UMR 5031, F-33600 Pessac, France
    *Email: [email protected]
  • , and 
  • Xin Bao*
    Xin Bao
    School of Chemistry and Chemical Engineering, Nanjing University of Science and Technology, Nanjing 210094, P. R. China
    *Email: [email protected]
    More by Xin Bao
Cite this: J. Am. Chem. Soc. 2023, 145, 17, 9564–9570
Publication Date (Web):April 19, 2023
https://doi.org/10.1021/jacs.2c13697
Copyright © 2023 American Chemical Society

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    Abstract

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    In 2019, our groups described a unique FeII complex, [Fe(2MeL)(NCBH3)2] (2MeL = N,N’-dimethyl-N,N’-bis(2-pyridylmethyl)-1,2-ethanediamine) possessing a low-spin ground state that is not easily accessible due to the extremely slow dynamics of the high-spin to low-spin phase transition. Herein, we report the successful chemical manipulation of this spin-crossover (SCO) process through controlled metal-ion dilutions. The emergence or suppression of the thermally induced SCO behavior was observed depending on the radius of the metal ion used for the dilution (NiII or ZnII). Reversible photo-switching has been confirmed in all mixed-metal complexes whether the low-spin state is thermally accessible. Remarkably, the dilution with ZnII metal ions stabilizes HS FeII complexes with complete suppression of the thermally induced SCO process without destroying the reversible photoswitchability of the material.

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/jacs.2c13697.

    • Details of physical characterizations, view of molecular structures and crystal packings, additional magnetic plots and reflectivity spectra, crystal data and refinement details, and structural parameters (PDF)

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    CCDC 21430192143023 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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    Cited By

    This article is cited by 1 publications.

    1. Ying-Ying Wu, Zhao-Yang Li, Shuang Peng, Zi-Yi Zhang, Hao-Ming Cheng, Hang Su, Wen-Qi Hou, Feng-Lei Yang, Shu-Qi Wu, Osamu Sato, Jing-Wei Dai, Wei Li, Xian-He Bu. Two-Dimensional Spin-Crossover Molecular Solid Solutions with Tunable Transition Temperatures across 90 K. Journal of the American Chemical Society 2024, 146 (12) , 8206-8215. https://doi.org/10.1021/jacs.3c12905

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