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Small Molecule Activation at the PNP Pincer-Supported Nickel Sites.
Acc Chem Res
November 2024
Department of Chemistry, Seoul National University, Seoul 08826, Republic of Korea.
ConspectusNickel pincer systems have recently attracted much attention for applications in various organometallic reactions and catalysis involving small molecule activation. Their exploration is in part motivated by the presence of nickel in natural systems for efficient catalysis. Among such systems, the nickel-containing metalloenzyme carbon monoxide dehydrogenase (CODH) efficiently and reversibly converts CO to CO at its active site.
View Article and Find Full Text PDFSelective Functionalization of Alkenes and Alkynes by Dinuclear Manganese Catalysts.
Acc Chem Res
October 2024
State Key Laboratory of Coordination Chemistry, Jiangsu Key Laboratory of Advanced Organic Materials, Chemistry and Biomedicine Innovation Center (ChemBIC), School of Chemistry and Chemical Engineering, Nanjing University, Nanjing 210023, China.
ConspectusAlkenes and alkynes are fundamental building blocks in organic synthesis due to their commercial availability, bench-stability, and easy preparation. Selective functionalization of alkenes and alkynes is a crucial step for the synthesis of value-added compounds. Precise control over these reactions allows efficient construction of complex molecules with new functionalities.
View Article and Find Full Text PDFMetalloradical Reactivity, Charge Transfer, and Atom Abstractions in a T-Shaped Iron(I) Complex.
Inorg Chem
March 2021
Anorganisch-Chemisches Institut, Universität Heidelberg, Im Neuenheimer Feld 276, 69120 Heidelberg, Germany.
A study of the reactivity of a T-shaped iron(I) complex supported by a carbazole-based PNP pincer ligand () has established its strongly reducing character and propensity to bind small molecules with concomitant transfer of charge and spin density. Metalloradical reactivity was observed in the reaction with the stable radical 2,2,6,6-tetramethylpiperidinyloxyl (TEMPO) yielding the corresponding Fe hydroxylaminato complex . Complex reacted rapidly and selectively with two molecules of carbon monoxide to give the corresponding low-spin dicarbonyl complex .
View Article and Find Full Text PDFLigand Protonation Triggers H Release from a Dinickel Dihydride Complex to Give a Doubly "T"-Shaped Dinickel(I) Metallodiradical.
Angew Chem Int Ed Engl
January 2021
Universität Göttingen, Institut für Anorganische Chemie, Tammannstrasse 4, 37077, Göttingen, Germany.
The dinickel(II) dihydride complex (1 ) of a pyrazolate-based compartmental ligand with β-diketiminato (nacnac) chelate arms (L ), providing two pincer-type {N } binding pockets, has been reported to readily eliminate H and to serve as a masked dinickel(I) species. Discrete dinickel(I) complexes (2 , 2 ) of L are now synthesized via a direct reduction route. They feature two adjacent T-shaped metalloradicals that are antiferromagnetically coupled, giving an S=0 ground state.
View Article and Find Full Text PDFOpening up the Valence Shell: A T-Shaped Iron(I) Metalloradical and Its Potential for Atom Abstraction.
Angew Chem Int Ed Engl
June 2020
Anorganisch-Chemisches Institut, Universität Heidelberg, Im Neuenheimer Feld 276, 69120, Heidelberg, Germany.
A thermally stable, T-shaped, d high-spin iron(I) complex was obtained by reduction of a PNP-supported ferrous chloride. Paramagnetic NMR spectroscopy combined with DFT modeling was used to analyze the electronic structure of the coordinatively highly unsaturated complex. The metalloradical character of the compound was demonstrated by the formation of a benzophenone ketyl radical complex upon addition of benzophenone.
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