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A comprehensive approach for elucidating the interplay between 4f and 4f 5d configurations in Ln complexes.
Chem Sci
January 2025
Radioisotope Science and Technology Division, Oak Ridge National Laboratory Oak Ridge TN 37830 USA
Lanthanides (Ln) are typically found in the +3 oxidation state. However, in recent decades, their chemistry has been expanded to include the less stable +2 oxidation state across the entire series except promethium (Pm), facilitated by the coordination of ligands such as trimethylsilylcyclopentadienyl, CHSiMe (Cp'). The complexes have been the workhorse for the synthesis and theoretical study of the fundamental aspects of divalent lanthanide chemistry, where experimental and computational evidence have suggested the existence of different ground state (GS) configurations, 4f or 4f 5d, depending on the specific metal.
View Article and Find Full Text PDFAdvanced spectroscopic evidence for the sequestration of heavy metals via repetitive in situ synthesis of Fe oxide.
J Hazard Mater
January 2025
Department of Civil and Environmental Engineering, Seoul National University, 1 Gwanak-ro, Gwanak-gu, Seoul 08826, Republic of Korea. Electronic address:
The in situ synthesis of Fe oxide is an established method for stabilizing metals and metalloids (Me) in contaminated soils. Nevertheless, the potential for enhanced Me sequestration through repeated Fe oxide application and the fundamental mechanisms of this process yet to be systemically investigated. In this study, the means by which repetitive Fe oxide synthesis enhances the immobilization of Cd, Zn, and As was investigated using batch experiments.
View Article and Find Full Text PDFNidustrin A, cysteine-retained emestrin with a unique 18-membered macrocyclic lactone from the endophytic fungus Aspergillus nidulans.
Bioorg Chem
December 2024
Hubei Key Laboratory of Natural Medicinal Chemistry and Resource Evaluation, School of Pharmacy, Tongji Medical College, Huazhong University of Science and Technology, Wuhan 430030, PR China. Electronic address:
Nidustrin A (1), the first cysteine-retained emestrin featuring a unique sulfur-containing 18-membered macrocyclic lactone, along with four biogenetically related compounds (2-5), and one known analogue secoemestrin C (6), were isolated from the large-scale culture of Aspergillus nidulans, an endophytic fungus derived from the Whitmania pigra. Compounds 2 and 3 represent the second examples of noremestrin besides the previously reported noremestrin A, and the single crystal X-ray diffraction analysis of compound 2 provided solid evidence for the intriguing skeleton of noremestrin. Their structures were determined by extensive spectroscopic data, electronic circular dichroism calculations, and single-crystal X-ray diffraction.
View Article and Find Full Text PDFIsolated Neutral Organic Radical Unveiled Solvent-Radical Interaction in Highly Reducing Photocatalysis.
Angew Chem Int Ed Engl
January 2025
The University of Arizona, Chemistry and BioChemistry, 1306 E University Blvd, CSML 638, 85719, Tucson, UNITED STATES OF AMERICA.
Diffusion-limited kinetics is a key mechanistic debate when consecutive photoelectron transfer (conPET) is discussed in photoredox catalysis. In-situ generated organic photoactive radicals can access catalytic systems as reducing as alkaline metals that can activate remarkably stable bonds. However, in many cases, the extremely short-lived transient nature of these doublet state open-shell species has led to debatable mechanistic studies, hindering adoption and development.
View Article and Find Full Text PDFReplacement of the essential catalytic aspartate with serine leads to an active form of copper-containing nitrite reductase from the denitrifier Sinorhizobium meliloti 2011.
Biochim Biophys Acta Proteins Proteom
December 2024
Departamento de Física, Facultad de Bioquímica y Ciencias Biológicas, Universidad Nacional del Litoral and CONICET, S3000ZAA Santa Fe, Argentina.
Article Synopsis
- The study details the characterization of a mutated variant of copper-containing nitrite reductase (SmNirK) from S. meliloti, where the catalytic aspartate (Asp) is replaced with serine (Ser) via site-directed mutagenesis.
- The D134S variant retains the homotrimer structure and similar T1 electron transfer center to the wild-type, but shows altered electronic properties in the T2 active site, impacting its enzymatic efficiency and pH dependence.
- EPR studies reveal significant changes in the T2 properties due to the mutation, highlighting the role of T2 ligands in catalysis and suggesting a potential mechanism for electron transfer influenced by the Asp/Ser switch.
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