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Heterogeneous Frustrated Lewis Pair Catalysts: Rational Structure Design and Mechanistic Elucidation Based on Intrinsic Properties of Supports.
Acc Chem Res
January 2025
The Wolfson Catalysis Centre, Department of Chemistry, University of Oxford, Oxford OX1 3QR, U.K.
ConspectusThe discovery of reversible hydrogenation using metal-free phosphoborate species in 2006 marked the official advent of frustrated Lewis pair (FLP) chemistry. This breakthrough revolutionized homogeneous catalysis approaches and paved the way for innovative catalytic strategies. The unique reactivity of FLPs is attributed to the Lewis base (LB) and Lewis acid (LA) sites either in spatial separation or in equilibrium, which actively react with molecules.
View Article and Find Full Text PDFSupramolecular dyads as photogenerated qubit candidates.
Nat Chem
January 2025
SAMS Research Group, Université de Strasbourg, CNRS, Institut Charles Sadron UPR 22, Strasbourg, France.
Molecular spin qubits have the advantages of synthetic flexibility and amenability to be tailored to specific applications. Among them, chromophore-radical systems have emerged as appealing qubit candidates. These systems can be initiated by light to form triplet-radical pairs that can result in the formation of quartet states by spin mixing.
View Article and Find Full Text PDFMolecular Processes That Control Organic Electrosynthesis in Near-Electrode Microenvironments.
J Am Chem Soc
January 2025
Department of Chemical and Biomolecular Engineering, New York University, Brooklyn, New York 11201, United States.
Electrosynthesis at an industrial scale offers an opportunity to use renewable electricity in chemical manufacturing, accelerating the decarbonization of large-scale chemical processes. Organic electrosynthesis can improve product selectivity, reduce reaction steps, and minimize waste byproducts. Electrochemical synthesis of adiponitrile (ADN) via hydrodimerization of acrylonitrile (AN) is a prominent example of industrial organic electrochemical processes, with annual production reaching 0.
View Article and Find Full Text PDF«Green-Ligand» in Metallodrugs Design-Cu(II) Complex with Phytic Acid: Synthetic Approach, EPR-Spectroscopy, and Antimycobacterial Activity.
Molecules
January 2025
N. S. Kurnakov Institute of General and Inorganic Chemistry, Russian Academy of Sciences, Leninsky Prosp. 31, 119991 Moscow, Russia.
The interaction of sodium phytate hydrate CHOP·xNa·yHO (phytNa) with Cu(OAc)·HO and 1,10-phenanthroline (phen) led to the anionic tetranuclear complex [Cu(HO)(phen)(phyt)]·2Na·2NH·32HO (), the structure of the latter was determined by X-ray diffraction analysis. The phytate is completely deprotonated; six phosphate fragments (with atoms P1-P6) are characterized by different spatial arrangements relative to the cyclohexane ring (1a5e conformation), which determines two different types of coordination to the complexing agents-P1 and P3, P4, and P6 have monodentate, while P2 and P5 are bidentately bound to Cu cations. The molecular structure of the anion complex is stabilized by a set of strong intramolecular hydrogen bonds involving coordinated water molecules.
View Article and Find Full Text PDFSpeciation of Potentially Carcinogenic Trace Nickel(II) Ion Levels in Human Saliva: A Sequential Metabolomics-Facilitated High-Field H NMR Investigation.
Metabolites
December 2024
Leicester School of Pharmacy, De Montfort University, Leicester LE1 9BH, UK.
Since the biological activities and toxicities of 'foreign' and/or excess levels of metal ions are predominantly determined by their precise molecular nature, here we have employed high-resolution H NMR analysis to explore the 'speciation' of paramagnetic Ni(II) ions in human saliva, a potentially rich source of biomolecular Ni(II)-complexants/chelators. These studies are of relevance to the corrosion of nickel-containing metal alloy dental prostheses (NiC-MADPs) in addition to the dietary or adverse toxicological intake of Ni(II) ions by humans. Unstimulated whole-mouth human saliva samples were obtained from n = 12 pre-fasted (≥8 h) healthy participants, and clear whole-mouth salivary supernatants (WMSSs) were obtained from these via centrifugation.
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