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Synthesis, Structure, and Redox Reactivity of Ni Complexes Bearing a Redox and Acid-Base Non-innocent Ligand with Ni, Ni, and Ni Formal Oxidation States.
J Am Chem Soc
January 2025
Department of Chemistry and Nano Science, Ewha Womans University, Seoul 03760, Korea.
A series of Ni complexes bearing a redox and acid-base noninnocent tetraamido macrocyclic ligand, H-(TAML-4) {H-(TAML-4) = 15,15-dimethyl-5,8,13,17-tetrahydro-5,8,13,17-tetraaza-dibenzo[]cyclotridecene-6,7,14,16-tetraone}, with formal oxidation states of Ni, Ni, and Ni were synthesized and characterized structurally and spectroscopically. The X-ray crystallographic analysis of the Ni complexes revealed a square planar geometry, and the [Ni(TAML-4)] complex with the formal oxidation state of Ni was characterized to be [Ni(TAML-4)] with the oxidation state of the Ni ion and the one-electron oxidized TAML-4 ligand, TAML-4. The Ni oxidation state and the TAML-4 radical cation ligand, TAML-4, were supported by X-ray absorption spectroscopy and density functional theory calculations.
View Article and Find Full Text PDFNi Single Atoms/FeN Nanoparticles Supported by N-Doped Carbon Hollow Nanododecahedras with Nanotubes on the Surface for Efficient Electro-Reduction of CO to CO.
Small
January 2025
College of Materials Science and Engineering, Sichuan University, Chengdu, 610065, China.
The transition metal single atoms (SAs)-based catalysts with M-N coordination environment have shown excellent performance in electrocatalytic reduction of CO, and they have received extensive attention in recent years. However, the presence of SAs makes it very difficult to efficiently improve the coordination environment. In this paper, a method of direct high-temperature pyrolysis carbonization of ZIF-8 adsorbed with Ni and Fe ions is reported for the synthesis of Ni SAs and FeN nanoparticles (NPs) supported by the N-doped carbon (NC) hollow nanododecahedras (HNDs) with nanotubes (NTs) on the surface (Ni SAs/FeN NPs@NC-HNDs-NTs).
View Article and Find Full Text PDFHydrogen Tunneling and Conformational Motions in Nonadiabatic Proton-Coupled Electron Transfer between Interfacial Tyrosines in Ribonucleotide Reductase.
J Am Chem Soc
January 2025
Department of Chemistry, Yale University, New Haven, Connecticut 06520, United States.
Ribonucleotide reductase (RNR) is essential for DNA synthesis and repair in all living organisms. The mechanism of RNR requires long-range radical transport through a proton-coupled electron transfer (PCET) pathway spanning two different protein subunits. Herein, the direct PCET reaction between the interfacial tyrosine residues, Y356 and Y731, is investigated with a vibronically nonadiabatic theory that treats the transferring proton and all electrons quantum mechanically.
View Article and Find Full Text PDFHinged Carboxylate in the Artificial Distal Pocket of an Iron Porphyrin Enhances CO Electroreduction at Low Overpotential.
Adv Sci (Weinh)
January 2025
Université Paris-Saclay, CNRS, Institut de Chimie Moléculaire et des Matériaux d'Orsay, Orsay, 91400, France.
To efficiently capture, activate, and transform small molecules, metalloenzymes have evolved to integrate a well-organized pocket around the active metal center. Within this cavity, second coordination sphere functionalities are precisely positioned to optimize the rate, selectivity, and energy cost of catalytic reactions. Inspired by this strategy, an artificial distal pocket defined by a preorganized 3D strap is introduced on an iron-porphyrin catalyst (sc-Fe) for the CO-to-CO electrocatalytic reduction.
View Article and Find Full Text PDFPhotoacid-Catalyzed Esterification of Carboxylic Acids Using Eosin Y.
Org Lett
January 2025
Department of Chemistry, Indian Institute of Technology, Roorkee, Uttarakhand 247667, India.
A photoacid-catalyzed method for esterification is proposed wherein eosin Y is introduced as a photoacid and photoredox catalyst that can be activated with visible light and catalyze the esterification of carboxylic acids. The strategy presented here revealed that proton-coupled electron transfer (PCET) between eosin Y and carboxylic acid might facilitate the formation of a transient ketyl radical. This ketyl radical would subsequently undergo a single electron transfer and then couple with alkyl alcohols, yielding carboxylic esters in good to excellent yields.
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