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Herein we present a series of new α-iminopyridine-based iron-PNN pincer complexes [FeBr2LPNN] (1), [Fe(CO)2LPNN] (2), [Fe(CO)2LPNN](BF4) (3), [Fe(F)(CO)2LPNN](BF4) (4), and [Fe(H)(CO)2LPNN](BF4) (5) with formal oxidation states ranging from Fe(0) to Fe(II) (LPNN = 2-[(di-tert-butylphosphino)methyl]-6-[1-(2,4,6-mesitylimino)ethyl]pyridine). The complexes were characterized by a variety of methods including (1)H, (13)C, (15)N, and (31)P NMR, IR, Mössbauer, and X-ray photoelectron spectroscopy (XPS) as well as electron paramagnetic resonance (EPR) and magnetic circular dichroism (MCD) spectroscopy, SQUID magnetometry, and X-ray crystallography, focusing on the assignment of the metal oxidation states. Ligand structural features suggest that the α-iminopyridine ligand behaves as a redox non-innocent ligand in some of these complexes, particularly in [Fe(CO)2LPNN] (2), in which it appears to adopt the monoanionic form. In addition, the NMR spectroscopic features ((13)C, (15)N) indicate the accumulation of charge density on parts of the ligand for 2. However, a combination of spectroscopic measurements that more directly probe the iron oxidation state (e.g., XPS), density functional theory (DFT) calculations, and electronic absorption studies combined with time-dependent DFT calculations support the description of the metal atom in 2 as Fe(0). We conclude from our studies that ligand structural features, while useful in many assignments of ligand redox non-innocence, may not always accurately reflect the ligand charge state and, hence, the metal oxidation state. For complex 2, the ligand structural changes are interpreted in terms of strong back-donation from the metal center to the ligand as opposed to electron transfer.
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http://dx.doi.org/10.1021/acs.inorgchem.5b00509 | DOI Listing |
Wei Sheng Yan Jiu
November 2024
West China School of Public Health, Sichuan University, Chengdu 610041, China.
Objective: To explore the possible mechanism of absorption of iron oxide nanoparticles into the human body through the gastrointestinal tract.
Methods: This article used Caco-2 monolayer cells as a cell model, prepared characterized iron oxide nanoparticles(Fe_2O_3 NPs) as suspensions, and intervened in Caco-2 cells. CCK-8 method, transwell method, and atomic spectrophotometer method were used to explore the effect of Fe_2O_3 NPs on the activity of Caco-2 cells and the absorption and transport of them through the Caco-2 monolayer cell model.
ACS Nano
December 2024
Department of Chemistry, Burke Laboratory, Dartmouth College, Hanover, New Hampshire 03755, United States.
This paper describes the use of the layered conductive metal-organic framework (MOF) (nickel)-(hexahydroxytriphenylene) [Ni(HHTP)] as a model system for understanding the process of self-assembly within this class of materials. We confirm and quantify experimentally the role of the oxidant in the synthetic process. Monitoring the deposition of Ni(HHTP) with infrared spectroscopy revealed that MOF formation is characterized by an initial induction period, followed by linear growth with respect to time.
View Article and Find Full Text PDFLangmuir
December 2024
School of Materials, Sun Yat-sen University, Shenzhen 518107, China.
Hydrogen sulfide (HS), carbonyl sulfide (COS), and dimethyl sulfide (DMS) are the primary sulfur compounds found in seawater, which cause pitting corrosion on the oxide passivation film of titanium, known as "the marine metals". In this study, density functional theory (DFT) was used to analyze the adsorption and surface electronic properties of these three small molecules on the anatase TiO(101) surface. The analysis was conducted through adsorption energy, work function, Mulliken charge population, and density of states (DOS).
View Article and Find Full Text PDFACS Appl Mater Interfaces
December 2024
Henan Key Laboratory of Crystalline Molecular Functional Materials, Key Laboratory of Special Environmental Functional Materials (Zhengzhou University), and College of Chemistry, Zhengzhou University, Zhengzhou 450001, China.
Four fundamental reactions are essential to harnessing energy from water sustainably: oxidation reduction reaction (ORR), oxygen reduction reaction (OER), hydrogen oxidation reaction (HOR), and hydrogen evolution reaction (HER). This review summarizes the research advancements in the electrocatalytic reaction of metal nanoclusters for water splitting. It covers various types of nanoclusters, particularly those at the size level, that enhance these catalytic reactions.
View Article and Find Full Text PDFPlant Physiol Biochem
December 2024
Department of Pomology, Faculty of Agriculture, Assiut University, Assiut, 71526, Egypt; Biology Research & Studies Institute, Assiut University, Assiut, 71526, Egypt. Electronic address:
Smart nanohybrid technology with potential advantages to plants has recently been developed formanaging the widespread pollution of heavy metals. Herein, we disclose a novel strategy to combat Pb stress in strawberry (Fragaria spp. cv.
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