Metal-ligand cooperation facilitates bond activation and catalytic hydrogenation with zinc pincer complexes
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A series of PNP zinc pincer complexes capable of bond activation via aromatization/dearomatization metal-ligand cooperation (MLC) were prepared and characterized. Reversible heterolytic N-H and H-H bond activation by MLC is shown, in which hemilability of the phosphorus linkers plays a key role. Utilizing this zinc pincer system, base-free catalytic hydrogenation of imines and ketones under relatively mild conditions is demonstrated. A detailed mechanistic study supported by computation implicates the key role of MLC in facili-tating effective catalysis. This approach offers a new strategy for (de)hydrogenation and other catalytic transformations mediated by zinc and other main group metals.
Rauch , M , Kar , S , Kumar , A , Avram , L , Shimon , L J W & Milstein , D 2020 , ' Metal-ligand cooperation facilitates bond activation and catalytic hydrogenation with zinc pincer complexes ' , Journal of the American Chemical Society , vol. 142 , no. 34 , pp. 14513-14521 . https://doi.org/10.1021/jacs.0c05500
Journal of the American Chemical Society
Copyright © 2020 American Chemical Society. This work has been made available online in accordance with publisher policies or with permission. Permission for further reuse of this content should be sought from the publisher or the rights holder. This is the author created accepted manuscript following peer review and may differ slightly from the final published version. The final published version of this work is available at https://doi.org/10.1021/jacs.0c05500
DescriptionWe thank the European Research Council (ERC AdG 692775) for support of this research. M.R. acknowledges the Zuckerman STEM Leadership Program for a research fellowship. S.K. acknowledges the Sustainability and Energy Research Initiative (SAERI) Weizmann Institute of Science for a research fellowship. A. K. is thankful to the Feinberg Graduate School for the Senior Postdoctoral Fellowship.
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