The Fe(IV)oxo complex of a coordinatively flexible multidentate mono-carboxylato ligand is obtained by the one electron oxidation of a low spin Fe(III) precursor in water.
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Coordination engineering of heterogeneous high-valent Fe(IV)-oxo for safe removal of pollutants via powerful Fenton-like reactions.
Nat Commun
November 2024
Guangdong Basic Research Center of Excellence for Ecological Security and Green Development, Key Laboratory for City Cluster Environmental Safety and Green Development of the Ministry of Education, School of Ecology, Environment and Resources, Guangdong University of Technology, Guangzhou, P.R. China.
Article Synopsis
- Coordination engineering of Fe-N single-atom catalysts (Fe-N SACs) is proposed to enhance the generation of high-valent Fe(IV)-oxo (Fe=O), providing a solution to the traditional trade-off in activity and selectivity of reactive oxygen species.
- The new Fe-N SACs/peroxymonosulfate (PMS) system shows significant improvements in Fe=O production, allowing for the rapid removal of various pollutants within seconds.
- The study reveals that low-coordination Fe-N SACs promote efficient Fe=O generation, which selectively oxidizes sulfamethoxazole (SMX) into less toxic byproducts, while differently coordinated Fe=O can lead to the formation of more toxic azo compounds through
Revisiting the Iron(II)/Cobalt(II)-Based Homogenous Fenton-like Processes from the Standpoint of Diverse Metal-Oxygen Complexes.
Environ Sci Technol
September 2024
State Key Laboratory of Urban Water Resources and Environment, School of Environment, Harbin Institute of Technology, Harbin 150090, China.
The aqueous Fe-oxo complex and Fe-peroxy complex (e.g., ligand-assisted or interfacial Fe-hydroperoxo intermediates) have been recognized as crucial reactive intermediates for decontamination in iron-based Fenton-like processes.
View Article and Find Full Text PDFProton-triggered chemoselective halogenation of aliphatic C-H bonds with nonheme Fe-oxo complexes.
J Inorg Biochem
October 2024
Institut de Química Computacional i Catàlisi (IQCC), Departament de Química, Universitat de Girona, C/ Maria Aurèlia Capmany 69, 17003 Girona, Catalonia, Spain. Electronic address:
Halogenation of aliphatic C-H bonds is a chemical transformation performed in nature by mononuclear nonheme iron dependent halogenases. The mechanism involves the formation of an iron(IV)-oxo-chloride species that abstracts the hydrogen atom from the reactive C-H bond to form a carbon-centered radical that selectively reacts with the bound chloride ligand, a process commonly referred to as halide rebound. The factors that determine the halide rebound, as opposed to the reaction with the incipient hydroxide ligand, are not clearly understood and examples of well-defined iron(IV)-oxo-halide compounds competent in C-H halogenation are scarce.
View Article and Find Full Text PDFDioxygen Activation and N,N-Dihydroxylation Mechanism Involved in the Formation of N-Nitrosourea Pharmacophore in Streptozotocin Catalyzed by Nonheme Diiron Enzyme SznF.
Inorg Chem
October 2022
School of Chemistry and Chemical Engineering, Shandong University, Jinan, Shandong 250100, China.
SznF is a nonheme diiron-dependent enzyme that catalyzes the critical N-nitrosation involved in the formation of the N-nitrosourea moiety in the pancreatic cancer drug streptozotocin. The N-nitrosation contains two successive N-hydroxylation and N-nitrosation steps, which are carried out by two separate active sites, namely, the central domain and cupin domain. Recently, the crystal structure of SznF was obtained, and the central domain was proved to contain a diiron cofactor to catalyze the N-hydroxylation.
View Article and Find Full Text PDFUnmasking the Iron-Oxo Bond of the [(Ligand)Fe-OIAr] Complexes.
J Am Soc Mass Spectrom
September 2022
Department of spectroscopy and Catalysis, Institute for Molecules and Materials, Radboud University, Heyendaalseweg 135, 6525 AJ Nijmegen, The Netherlands.
ArIO (ArI = 2-(BuSO)CHI) is an oxidant used to oxidize Fe species to their Fe-oxo state, enabling hydrogen-atom transfer (HAT) and oxygen-atom transfer (OAT) reactions at low energy barriers. ArIO, as a ligand, generates masked Fe═O species of the type Fe-OIAr. Herein, we used gas-phase ion-molecule reactions and DFT calculations to explore the properties of masked iron-oxo species and to understand their unmasking mechanisms.
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