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Characterization of a diferrous terminal hydride mechanistically relevant to the Fe-only hydrogenases.
TLDR
Crystallographic characterization shows that this model contains an asymmetrical semi-bridging CO trans to a terminal hydrido, as indicated in the Hred state in the D. desulfuricans enzyme.
Chelate control of diiron(I) dithiolates relevant to the [Fe-Fe]- hydrogenase active site.
TLDR
DFT calculations suggest that, relative to Fe2(S2C2H4)(CO)6, the enhanced electrophilicity of 1(CO)4 arises from the stabilization of a "rotated" transition state, which is favored by the unsymmetrically disposed donor ligands.
Water splitting by cooperative catalysis.
TLDR
A mononuclear Ru complex is shown to efficiently split water into H2 and O2 in consecutive steps through a heat- and light-driven process that might be the onset for new designs of catalytic water-splitting systems.
Neutral tridentate PNP ligands and their hybrid analogues: versatile non-innocent scaffolds for homogeneous catalysis.
TLDR
The chemistry of pyridine-derived, neutral ligands is discussed, with a specific focus on their non-innocent behavior and potential as facilitators for metal-mediated organic transformations.
New avenues for ligand-mediated processes--expanding metal reactivity by the use of redox-active catechol, o-aminophenol and o-phenylenediamine ligands.
TLDR
Redox-active ligands containing catechol, o-aminophenol or o-phenylenediamine moieties show great potential to be exploited as reversible electron reservoirs, donating or accepting electrons to activate substrates and metal centers and to enable new reactivity with both early and late transition as well as main group metals.
Ligands that store and release electrons during catalysis.
TLDR
A recently reported cobalt-mediated Negishi-type cross-coupling reaction provides an illustrative example of this concept and reveals its potential to develop new catalytic reactions with cheap, abundant metals.
Complexes with nitrogen-centered radical ligands: classification, spectroscopic features, reactivity, and catalytic applications.
TLDR
This Review should contribute to a better understanding of the (catalytic) reactivity of nitrogen-centered radical ligands and the role they play in tuning the reactsivity of coordination compounds.
Intramolecular redox-active ligand-to-substrate single-electron transfer: radical reactivity with a palladium(II) complex.
TLDR
Experimental and computational studies suggest a redox-noninnocent pathway wherein the redox"-active ligand facilitates intramolecular ligand-to-substrate single-electron transfer to generate an open-shell singlet "nitrene-sub substrate radical, ligand radical", enabling subsequent radical-type C-H amination reactivity with Pd(II).
Catalytic Synthesis of N-Heterocycles via Direct C(sp3)–H Amination Using an Air-Stable Iron(III) Species with a Redox-Active Ligand
TLDR
Readily available, well-defined, and air-stable 1 catalyzes the challenging intramolecular direct C(sp3)–H amination of unactivated organic azides to generate a range of saturated N-heterocycles with the highest turnover number (TON).
Reversible Redox Chemistry and Catalytic C(sp(3))-H Amination Reactivity of a Paramagnetic Pd Complex Bearing a Redox-Active o-Aminophenol-Derived NNO Pincer Ligand.
TLDR
Thorough removal of chlorinated impurities allows for modest catalytic turnover in the conversion of 4- phenylbutyl azide into N-protected 2-phenylpyrrolidine, which is the first example of a palladium-catalyzed radical-type transformation facilitated by a redox-active ligand as well as the first C-H amination mediated by ligand-to-substrate single-electron transfer.
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