Unraveling Oxidation and Spin States of a ...
Document type :
Article dans une revue scientifique: Article original
DOI :
Permalink :
Title :
Unraveling Oxidation and Spin States of a Single Fe-Based Meso-Macroporous Silica Catalyst in Fenton-like Reaction by Magnetic Measurements
Author(s) :
Bellouard, Christine [Auteur]
Institut Jean Lamour [IJL]
Kim, Sanghoon [Auteur]
Laboratoire Lorrain de Chimie Moléculaire [L2CM]
Ghanbaja, Jaafar [Auteur]
Institut Jean Lamour [IJL]
Wojcieszak, Robert [Auteur]
Unité de Catalyse et Chimie du Solide (UCCS) - UMR 8181
Laboratoire Lorrain de Chimie Moléculaire [L2CM]
Canilho, Nadia [Auteur]
Laboratoire Lorrain de Chimie Moléculaire [L2CM]
Pasc, Andreea [Auteur]
Laboratoire Lorrain de Chimie Moléculaire [L2CM]
Institut Jean Lamour [IJL]
Kim, Sanghoon [Auteur]
Laboratoire Lorrain de Chimie Moléculaire [L2CM]
Ghanbaja, Jaafar [Auteur]
Institut Jean Lamour [IJL]
Wojcieszak, Robert [Auteur]
Unité de Catalyse et Chimie du Solide (UCCS) - UMR 8181
Laboratoire Lorrain de Chimie Moléculaire [L2CM]
Canilho, Nadia [Auteur]
Laboratoire Lorrain de Chimie Moléculaire [L2CM]
Pasc, Andreea [Auteur]
Laboratoire Lorrain de Chimie Moléculaire [L2CM]
Journal title :
Journal of Physical Chemistry C
Abbreviated title :
J. Phys. Chem. C
Volume number :
128
Pages :
8449–8457
Publisher :
American Chemical Society (ACS)
Publication date :
2024-05-11
ISSN :
1932-7447
English keyword(s) :
Catalysts
Iron
Magnetic properties
Quantum mechanics
Silica
Iron
Magnetic properties
Quantum mechanics
Silica
HAL domain(s) :
Chimie/Catalyse
English abstract : [en]
Single-atom catalysts are acknowledged for their superior efficiency compared to nanoparticles or clusters, primarily because of the enhanced accessibility of the catalytic center. Essential parameters for assessing their ...
Show more >Single-atom catalysts are acknowledged for their superior efficiency compared to nanoparticles or clusters, primarily because of the enhanced accessibility of the catalytic center. Essential parameters for assessing their performance are the metal loading degree and oxidation state of the individual catalytic sites. This is particularly the case in Fe-based Fenton-like reaction, in which both Fe2+ and Fe3+ are active but react with significantly different catalytic rates. While the elemental metal loading can be easily assessed by elemental analysis, the determination of the oxidation degree is more challenging. To do so, we designed single Fe-based meso-macroporous silica materials as catalysts for the degradation of methylene blue, an organic dye serving as a well-known model for the degradation of organic pollutants in wastewater. The silica materials were successfully synthesized by a sol–gel process through a combined templating mechanism with micelles and solid lipid nanoparticles of Fe-based surfactants. Magnetic measurements have revealed that half of the iron centers are in the Fe2+ state. The tracking of the Fenton like reaction through magnetic measurements agrees with the contribution of Fe2+ in the catalytic process. The magnetic response emerges as a valuable tool for quantifying and characterizing individual catalytic centers.Show less >
Show more >Single-atom catalysts are acknowledged for their superior efficiency compared to nanoparticles or clusters, primarily because of the enhanced accessibility of the catalytic center. Essential parameters for assessing their performance are the metal loading degree and oxidation state of the individual catalytic sites. This is particularly the case in Fe-based Fenton-like reaction, in which both Fe2+ and Fe3+ are active but react with significantly different catalytic rates. While the elemental metal loading can be easily assessed by elemental analysis, the determination of the oxidation degree is more challenging. To do so, we designed single Fe-based meso-macroporous silica materials as catalysts for the degradation of methylene blue, an organic dye serving as a well-known model for the degradation of organic pollutants in wastewater. The silica materials were successfully synthesized by a sol–gel process through a combined templating mechanism with micelles and solid lipid nanoparticles of Fe-based surfactants. Magnetic measurements have revealed that half of the iron centers are in the Fe2+ state. The tracking of the Fenton like reaction through magnetic measurements agrees with the contribution of Fe2+ in the catalytic process. The magnetic response emerges as a valuable tool for quantifying and characterizing individual catalytic centers.Show less >
Language :
Anglais
Audience :
Internationale
Popular science :
Non
Administrative institution(s) :
Université de Lille
CNRS
Centrale Lille
ENSCL
Univ. Artois
CNRS
Centrale Lille
ENSCL
Univ. Artois
Collections :
Research team(s) :
Valorisation des alcanes et de la biomasse (VAALBIO)
Submission date :
2024-06-12T21:02:07Z
2024-06-17T10:54:35Z
2024-06-17T10:54:35Z