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4-(Dimethylamino)pyridine (DMAP) as an Acid-Modulated Donor Ligand for PAH Dearomatization
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    4-(Dimethylamino)pyridine (DMAP) as an Acid-Modulated Donor Ligand for PAH Dearomatization
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    Department of Chemistry, University of Virginia, Charlottesville, Virginia 22904, United States
    Department of Chemistry, University of Richmond, Richmond, Virginia 23173, United States
    *E-mail for W.D.H.: [email protected]
    Other Access OptionsSupporting Information (2)

    Organometallics

    Cite this: Organometallics 2017, 36, 3, 543–555
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    https://doi.org/10.1021/acs.organomet.6b00780
    Published December 16, 2016
    Copyright © 2016 American Chemical Society

    Abstract

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    The dearomatization of naphthalene and anthracene is explored by their η2 coordination to {TpMo(NO)(MeIm)} and {TpMo(NO)(DMAP)} (where Tp = hydridotris(pyrazolyl)borate, MeIm = 1-methylimidazole, and DMAP = 4-(dimethylamino)pyridine). The DMAP and MeIm complexes have nearly identical redox properties and abilities to bind these polycyclic aromatic hydrocarbons (PAHs), but unlike MeIm, the DMAP ligand can be protonated at N while remaining bound to the metal. This action enhances the π-acidic properties of DMAP, resulting in greater stability of the molybdenum toward oxidation by acid. Utilizing this feature of the DMAP ligand, several new 1,2-dihydronaphthalenes and 1,2-dihydroanthracenes were prepared. Furthermore, it was found that acetals and Michael acceptors could function as electrophiles for the PAHs using the DMAP system, resulting in several new mono- and 1,4-dialkylated products.

    Copyright © 2016 American Chemical Society

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    Supporting Information

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    The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acs.organomet.6b00780.

    • 1H and 13C NMR spectra for selected compounds and stereochemical analysis for compound 10 (PDF)

    • Crystallographic data for 10 (CIF)

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    Cited By

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    This article is cited by 14 publications.

    1. Suraj W. Wajge, Chayan Das. An Alternate Approach of Cross-Linking XNBR via Ferric–Carboxylate Interaction Assisted by Dimethylaminopyridine. ACS Applied Polymer Materials 2024, 6 (6) , 3094-3104. https://doi.org/10.1021/acsapm.3c02625
    2. Mattéo Cayla, Dorian Sonet, Emilien Tarayre, Romain Bapt, Brigitte Bibal. Tandem Oxidative Dearomatizations of Diphenylanthracene Atropisomers. The Journal of Organic Chemistry 2023, 88 (18) , 13067-13075. https://doi.org/10.1021/acs.joc.3c01252
    3. Jacob A. Smith, Spenser R. Simpson, Karl S. Westendorff, Justin Weatherford-Pratt, Jeffery T. Myers, Justin H. Wilde, Diane A. Dickie, W. Dean Harman. η2 Coordination of Electron-Deficient Arenes with Group 6 Dearomatization Agents. Organometallics 2020, 39 (13) , 2493-2510. https://doi.org/10.1021/acs.organomet.0c00277
    4. Justin H. Wilde, Jeffery T. Myers, Diane A. Dickie, W. Dean Harman. Molybdenum-Promoted Dearomatization of Pyridines. Organometallics 2020, 39 (8) , 1288-1298. https://doi.org/10.1021/acs.organomet.0c00047
    5. Jeffery T. Myers, Justin H. Wilde, Michal Sabat, Diane A. Dickie, W. Dean Harman. Michael–Michael Ring-Closure Reactions for a Dihapto-Coordinated Naphthalene Complex of Molybdenum. Organometallics 2020, 39 (8) , 1404-1412. https://doi.org/10.1021/acs.organomet.0c00110
    6. Steven J. Dakermanji, Jacob A. Smith, Karl S. Westendorff, Emmit K. Pert, Andrew D. Chung, Jeffery T. Myers, Kevin D. Welch, Diane A. Dickie, W. Dean Harman. Electron-Transfer Chain Catalysis of η2-Arene, η2-Alkene, and η2-Ketone Exchange on Molybdenum. ACS Catalysis 2019, 9 (12) , 11274-11287. https://doi.org/10.1021/acscatal.9b04191
    7. Philip J. Shivokevich, Jeffery T. Myers, Jacob A. Smith, Jared A. Pienkos, Steven J. Dakermanji, Emmit K. Pert, Kevin D. Welch, Carl O. Trindle, W. Dean Harman. Enantioenriched Molybdenum Dearomatization: Dissociative Substitution with Configurational Stability. Organometallics 2018, 37 (23) , 4446-4456. https://doi.org/10.1021/acs.organomet.8b00027
    8. Benjamin K. Liebov and W. Dean Harman . Group 6 Dihapto-Coordinate Dearomatization Agents for Organic Synthesis. Chemical Reviews 2017, 117 (22) , 13721-13755. https://doi.org/10.1021/acs.chemrev.7b00480
    9. Jeffery T. Myers, Jacob A. Smith, Steven J. Dakermanji, Justin H. Wilde, Katy B. Wilson, Philip J. Shivokevich, and W. Dean Harman . Molybdenum(0) Dihapto-Coordination of Benzene and Trifluorotoluene: The Stabilizing and Chemo-Directing Influence of a CF3 Group. Journal of the American Chemical Society 2017, 139 (33) , 11392-11400. https://doi.org/10.1021/jacs.7b05009
    10. Jonathan Long, Lou Rocard, Elsa Van Elslande, Pascal Retailleau, Juan Xie, Nicolas Bogliotti. Light‐Promoted Basic Nitrogen Unmasking in Arene Ruthenium Complexes Derived from Z ‐Configured 2,2′‐Azobispyridine. Chemistry – A European Journal 2023, 29 (48) https://doi.org/10.1002/chem.202301301
    11. Jianli Chen, Xinyu Lin, Feng Xu, Kejie Chai, Minna Ren, Zhiqun Yu, Weike Su, Fengfan Liu. An Efficient Continuous Flow Synthesis for the Preparation of N-Arylhydroxylamines: Via a DMAP-Mediated Hydrogenation Process. Molecules 2023, 28 (7) , 2968. https://doi.org/10.3390/molecules28072968
    12. Olivia L. Duletski, Roark D. O’Neill, Charles Beasley, Molly O’Hagan, Michael T. Mock. Complexes of Groups 5–7 with N2, NO, and Other N-Containing Small Molecules. 2022, 772-841. https://doi.org/10.1016/B978-0-12-820206-7.00165-7
    13. . DMAP. 2020https://doi.org/10.1002/9783527809080.cataz05634
    14. Yu Luo, Weiwei Xie, Yuxing Huang, Teng Zhang, Bo Yang, Yizhen Liu, Xuechang Zhou, Junmin Zhang. Polydimethylsiloxane sponge supported DMAP on polymer brushes: Highly efficient recyclable base catalyst and ligand in water. Journal of Catalysis 2018, 367 , 264-268. https://doi.org/10.1016/j.jcat.2018.09.015

    Organometallics

    Cite this: Organometallics 2017, 36, 3, 543–555
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acs.organomet.6b00780
    Published December 16, 2016
    Copyright © 2016 American Chemical Society

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