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Densely populated macrocyclic dicobalt sites in ladder polymers for low-overpotential oxygen reduction catalysis.
Nat Commun
January 2025
College of Polymer Science and Engineering, State Key Laboratory of Polymer Materials Engineering, Sichuan University, 610065 Chengdu, China.
Dual-atom catalysts featuring synergetic dinuclear active sites, have the potential of breaking the linear scaling relationship of the well-established single-atom catalysts for oxygen reduction reaction; however, the design of dual-atom catalysts with rationalized local microenvironment for high activity and selectivity remains a great challenge. Here we design a bisalphen ladder polymer with well-defined densely populated binuclear cobalt sites on Ketjenblack substrates. The strong electron coupling effect between the fully-conjugated ladder structure and carbon substrates enhances the electron transfer between the cobalt center and oxygen intermediates, inducing the low-to-high spin transition for the 3d electron of Co(II).
View Article and Find Full Text PDFAnilido-Oxazoline-Ligated Iron Alkoxide Complexes for Living Ring-Opening Polymerization of Cyclic Esters with Controllability.
Inorg Chem
January 2025
Department of Chemistry, The Hong Kong University of Science and Technology, Kowloon, Hong Kong 999077, China.
Anilido-oxazoline-ligated iron complexes, including bis(anilido-oxazolinate) iron(II), mononuclear iron(II) alkyl and aryloxide, as well as the dinuclear analogues, were synthesized, and their catalytic performance on ring-opening polymerization (ROP) has been studied. Transmetalation of FeCl(THF) with in situ-generated anilido-oxazolinate lithium afforded the bis(anilido-oxazolinate) iron complexes and . Half-sandwich anilido-oxazolinate iron trimethylsilylalkyl complexes and could be synthesized in good yields via taking pyridine as an L-type ligand.
View Article and Find Full Text PDFNucleophilic Fluoride Anion Delivery from Triazacyclononane-Supported Molecular Ca-F Complexes.
Angew Chem Int Ed Engl
January 2025
Chemistry Research Laboratory, Department of Chemistry, University of Oxford, South Parks Road, Oxford, OX1 3QR, UK.
The major source of fluoride, namely calcium difluoride (CaF), is derived from the mineral fluorspar. Recent advances in the activation of CaF via mechanochemical methods have inspired investigation of the fundamental properties of Ca-F bonds in molecular complexes. However, the paucity of well-defined molecular Ca-F-containing complexes undermines systematic understanding of the factors governing nucleophilic fluoride delivery.
View Article and Find Full Text PDFA dinuclear nickel peroxycarbonate complex: CO addition promotes HO release.
Chem Commun (Camb)
August 2024
Willard Henry Dow Laboratory, Department of Chemistry, University of Michigan 930 N. University Avenue, Ann Arbor, MI 48109, USA.
Nickel coordination compounds featuring Ni-O bonds are key structural motifs in both bioinorganic and synthetic chemistries. They serve as precursors for organic substrate oxidation and are commonly invoked intermediates in water oxidation and oxygen reduction schemes. Herein, we disclose a series of well-defined dinuclear nickel complexes that, upon treatment with CO and HO, afford the first nickel-bound peroxycarbonate.
View Article and Find Full Text PDFEnabling nucleophilic reactivity in molecular calcium fluoride complexes.
Nat Chem
September 2024
Chemistry Research Laboratory, Department of Chemistry, University of Oxford, Oxford, UK.
Calcium fluoride is the ultimate source of all fluorochemicals. Current synthetic approaches rely on the use of HF, generated from naturally occurring fluorspar and sulfuric acid. Methods for constructing E-F bonds directly from CaF have long been frustrated by its high lattice energy, low solubility and impaired fluoride ion nucleophilicity.
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