Selective functionalization of unactivated C-H bonds and ammonia production are extremely important industrial processes. A range of metalloenyzmes achieve these challenging tasks in biology by activating dioxygen and dinitrogen using cheap and abundant transition metals, such as iron, copper and manganese. High-valent iron-oxo and -nitrido complexes act as active intermediates in many of these processes. The generation of well-described model compounds can provide vital insights into the mechanism of such enzymatic reactions. Advances in the chemistry of model high-valent iron-oxo and -nitrido systems can be related to our understanding of the biological systems.
Download full-text PDF |
Source |
|---|---|
| http://dx.doi.org/10.1038/ncomms1718 | DOI Listing |
Publication Analysis
Top Keywords
Similar Publications
Switchable surface Fe sites for water/sediment remediation through enhanced selective oxidation and ROS regulation: Performance, mechanism and application.
J Hazard Mater
December 2024
State Key Laboratory of Hydraulics and Mountain River Engineering, Sichuan University, Chengdu, Sichuan 610065, China; School of Architecture and Environment, Sichuan University, Chengdu 610065, China. Electronic address:
Selective oxidation relying on high-valent iron-oxo species (Fe(IV/V)) is a promising way of effective organic decontamination. However, Fe(IV/V) formation and further purposeful reinforcement production are commonly insufficient and unsustainable. Herein, cerium (Ce) modification strategy was adopted for efficient micropollutants removal through boosting Fe(IV/V) generation.
View Article and Find Full Text PDFActivation of PAA at the Fe-N Sites by Boron Nitride Quantum Dots Enhanced Charge Transfer Generates High-Valent Metal-Oxo Species for Antibiotics Degradation.
Environ Sci Technol
December 2024
Department of Environmental Science and Engineering, School of Architecture and Environment, Sichuan University, Chengdu 610065, China.
Advanced oxidation processes (AOPs) based on peracetic acid (PAA) offer a promising strategy to address antibiotic wastewater pollution. In this study, Fe-doped graphitic carbon nitride (g-CN) nanomaterials were used to construct Fe-N sites, and the electronic structure was tuned by boron nitride quantum dots (BNQDs), thereby optimizing PAA activation for the degradation of antibiotics. The BNQDs-modified Fe-doped g-CN catalyst (BNQDs-FCN) achieved an excellent reaction rate constant of 0.
View Article and Find Full Text PDFElectric fields imbue enzyme reactivity by aligning active site fragment orbitals.
Proc Natl Acad Sci U S A
October 2024
Department of Chemistry and Biochemistry, University of California, Los Angeles, CA 90095.
It is broadly recognized that intramolecular electric fields, produced by the protein scaffold and acting on the active site, facilitate enzymatic catalysis. This field effect can be described by several theoretical models, each of which is intuitive to varying degrees. In this contribution, we show that a fundamental effect of electric fields is to generate electrostatic potentials that facilitate the energetic alignment of reactant frontier orbitals.
View Article and Find Full Text PDFPicolinic acid promotes organic pollutants removal in Fe(III)/periodate process: Mechanism and relationship between removal efficiency and pollutant structure.
Water Res
January 2025
School of Environment, Henan Normal University, Key Laboratory of Yellow River and Huai River Water Environment and Pollution Control, Ministry of Education, Henan Key Laboratory for Environmental Pollution Control, International Joint Laboratory on Key Techniques in Water Treatment, Henan Province, Henan Engineering Laboratory of Environmental Functional Materials and Pollution Control, Xinxiang, Henan 453007, PR China.
The application of Fe-catalyzed periodate (PI) processes is often limited by both the narrow applicable pH range and weak reaction between Fe(III) and oxidant. Here, the biodegradable picolinic acid (PICA) was used as one kind of chelating ligands (CLs) to enhance the removal of organic pollutants (OPs) at initial pH 3.0-8.
View Article and Find Full Text PDFTemperature-modulated morphological changes in MIL-88B(Fe)-derived iron-based materials triggering generation of the peroxymonosulfate nonradical pathway to degrade carbamazepine: The key role of iron nanoparticles and CN.
J Colloid Interface Sci
January 2025
Guangdong Key Laboratory of Environmental Catalysis and Health Risk Control, Guangdong Industrial Contaminated Site Remediation Technology and Equipment Engineering Research Center, School of Environmental Science and Engineering, Guangdong University of Technology, Guangzhou 510006, China.
Article Synopsis
- The study investigates how temperature changes affect the synthesis of a carbon-based nitrogen-doped MOF-derived composite catalyst (MN@C) made from MIL-88B(Fe) and its catalytic properties.
- It found that variations in iron nanoparticles and carbon/nitrogen content altered degradation pathways, with the MN@C-9 catalyst achieving 100% removal of carbamazepine in just 10 minutes.
- The catalyst maintains efficiency across various pH levels and water conditions, demonstrating the potential for effective removal of pollutants from pharmaceuticals and personal care products, while significantly reducing the toxicity of byproducts.
Want AI Summaries of new PubMed Abstracts delivered to your In-box?
Enter search terms and have AI summaries delivered each week - change queries or unsubscribe any time!