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2. Impacts of functionalized organic surfaces in Mn oxides formation in situ monitored by electron microscopy

Author

Charlotte Dejean, Nathaly Ortiz Peña, Bénédicte Ménez, Cyril Gadal, Hélène Bouquerel, Damien Alloyeau, and Alexandre Gélabert

Abstract

Manganese oxide minerals are among the most powerful oxidizers on the Earth's surface. They are therefore key minerals both for the origin of life and exobiology issues but also for those concerning current biogeochemical cycles. Most of these manganese oxides are formed by biomineralization processes carried out by microorganisms that must be deciphered to better understand the fate of metals and metalloids in subsurface environments. A recent study showed that liquid-cell scanning transmission electron microscopy (LC-STEM) enables to monitor in situ the growth of Mn-bearing minerals onto Escherichia coli cells. This study has also highlighted the critical role of the chemical functions carried by cell surfaces and exopolymers during biomineralization. However, the contribution of the different functional groups associated to these biopolymers during mineral nucleation and growth remains poorly defined. In order to better assess the role played by these different chemical functions during biomineralization, functionalized polystyrene beads were used here as analogs of biological surfaces. In addition to control beads without functionalization, nine representative types of functionalization were selected, ranging from simple carboxylic and amino groups, to strong chelating agents such as nitrilotriacetic acid (NTA), or more complex proteins such as streptavidin and collagen. Each bead type was exposed to Mn(II)-bearing solution, and mineralization dynamics was continuously monitored in situ by LC-STEM. Mn mineralization was observed for all ten bead types with the formation of pyrolusite (MnO2) at the bead surfaces, as the result of changes in Mn redox state in solution triggered by radiolysis resulting from water and electron beam interactions. For all bead types, mineralization can be described as a nucleation step followed by the formation of larger dendritic structures. However, nucleation site densities, precipitates morphologies, as well as the overall mineral growth kinetics were found to vary significantly between the different grafted chemical functions. The bead surface charge, estimated by electrophoretic mobility, only partly explains these differences in mineralization dynamics. Steric effects, hydrophobicity as well as Mn affinity for the functional groups are certainly important parameters for Mn mineralization. As a result, this study brings interesting constraints on biomineralization processes driven by microorganisms.

Published
2023

4. The influence of <scp>l</scp>-aspartic acid on calcium carbonate nucleation and growth revealed by in situ liquid phase TEM

Author

Mariana M. Longuinho, Vinavadini Ramnarain, Nathaly Ortiz Peña, Dris Ihiawakrim, Rubén Soria-Martínez, Marcos Farina, Ovidiu Ersen, and André L. Rossi

Subjects
General Materials Science, General Chemistry, Condensed Matter Physics
Abstract

The l-Asp has a modulator function during CaCO3 crystallization by interaction with free calcium through coordinated bonds, forming vesicle-like structures during interaction CaCO3 nuclei.

Published
2022

5. Resolution of MoS2 nanosheets-induced pulmonary inflammation driven by nanoscale intracellular transformation and extracellular-vesicle shuttles

Author

Nathaly Ortiz Peña, Kondareddy Cherukula, Benjamin Even, Ding-Kun Ji, Sarah Razafindrakoto, Shiyuan Peng, Amanda K. A. Silva, Cécilia Ménard Moyon, Hervé Hillaireau, Alberto Bianco, Elias Fattal, Damien Alloyeau, and Florence Gazeau

Abstract

Pulmonary exposure to some engineered nanomaterials can cause chronic lesions as a result of unresolved inflammation. Among two-dimensional (2D) nanomaterials and graphene, MoS2 have received tremendous attention in optoelectronics and nanomedicine. Here we propose an integrated approach to follow up the transformation of MoS2 nanosheets at the nanoscale and their impact on the lung inflammation status over one month after a single inhalation in mice. Analysis of immune cells, alveolar macrophages, extracellular vesicles, and cytokine profiling in bronchoalveolar lavage fluid (BALF) showed that MoS2 nanosheets induced initiation of lung inflammation that was rapidly resolved despite the persistence of various biotransformed molybdenum-containing nanostructures in alveolar macrophages and extracellular vesicles up to one month. Using in situ liquid phase transmission electron microscopy experiments, we could evidence the dynamics of MoS2 nanosheets transformation triggered by reactive oxygen species. Three main transformation mechanisms were observed directly at the nanoscale level: 1) scrolling of the dispersed sheets leading to the formation of nanoscrolls and folded patches, 2) etching releasing soluble MoO4-, and 3) oxidation generating oxidized sheet fragments. Extracellular vesicles released in BALF were also identified as a potential shuttle of MoS2 nanostructures and their degradation products and more importantly as mediators of inflammation resolution.

Published
2022

6. Monitoring of CaCO

Author

Vinavadini, Ramnarain, Tristan, Georges, Nathaly, Ortiz Peña, Dris, Ihiawakrim, Mariana, Longuinho, Hervé, Bulou, Christel, Gervais, Clément, Sanchez, Thierry, Azaïs, and Ovidiu, Ersen

Subjects
Aspartic Acid, Magnetic Resonance Spectroscopy, Microscopy, Electron, Transmission, Carbonates, Calcium Carbonate
Abstract

Calcium carbonate (CaCO

Published
2022

7. In situ liquid transmission electron microscopy reveals self-assembly-driven nucleation in radiolytic synthesis of iron oxide nanoparticles in organic media

Author

Nathaly Ortiz Peña, Dris Ihiawakrim, Sorina Creţu, Geoffrey Cotin, Céline Kiefer, Sylvie Begin-Colin, Clément Sanchez, David Portehault, Ovidiu Ersen, Institut de Physique et Chimie des Matériaux de Strasbourg (IPCMS), Université de Strasbourg (UNISTRA)-Centre National de la Recherche Scientifique (CNRS)-Matériaux et Nanosciences Grand-Est (MNGE), Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Réseau nanophotonique et optique, Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Centre National de la Recherche Scientifique (CNRS), Novel Advanced Nano-Objects (LCMCP-NANO), Matériaux Hybrides et Nanomatériaux (LCMCP-MHN), Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), and Portehault, David

Subjects
[CHIM.INOR] Chemical Sciences/Inorganic chemistry, [CHIM.MATE] Chemical Sciences/Material chemistry, Aucun, General Materials Science, [CHIM.MATE]Chemical Sciences/Material chemistry, [CHIM.INOR]Chemical Sciences/Inorganic chemistry
Abstract

International audience; We have investigated the early stages of formation of iron oxide nanoparticles from iron stearate precursors in the presence of sodium stearate in an organic solvent by in situ liquid phase transmission electron microscopy (IL-TEM). Before nucleation, we have evidenced the spontaneous formation of vesicular assemblies made of iron polycation-based precursors sandwiched between stearate layers. Nucleation of iron oxide nanoparticles occurs within the walls of the vesicles, which subsequently collapse upon consumption of the iron precursors and growth of the nanoparticles. We then evidenced that fine control of the electron dose, and therefore of the local concentration of reactive iron species in the vicinity of the nuclei, enables controlling crystal growth and selecting the morphology of the resulting iron oxide nanoparticles. Such direct observation of the nucleation process templated by vesicular assemblies in a hydrophobic organic solvent sheds new light on the formation process of metal oxide nanoparticles and therefore opens ways for the synthesis of inorganic colloidal systems with tunable shape and size.

Published
2022

10. Correlative Microscopy Insight on Electrodeposited Ultrathin Graphite Oxide Films

Author

Nathaly Ortiz Peña, Stefan Stanescu, Dris Ihiawakrim, David Portehault, Ovidiu Ersen, Mircea V. Rastei, Clément Sanchez, Vincent Ball, Institut de Physique et Chimie des Matériaux de Strasbourg (IPCMS), Université de Strasbourg (UNISTRA)-Matériaux et nanosciences d'Alsace (FMNGE), Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Centre National de la Recherche Scientifique (CNRS)-Réseau nanophotonique et optique, Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA), Faculté de chirurgie dentaire - Strasbourg, Université de Strasbourg (UNISTRA), Chaire Chimie des matériaux hybrides, Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), and Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)

Subjects
Materials science, Graphite oxide, 02 engineering and technology, Electronic structure, 010402 general chemistry, 021001 nanoscience & nanotechnology, Electrochemistry, 01 natural sciences, 0104 chemical sciences, Electrochemical cell, chemistry.chemical_compound, Chemical engineering, chemistry, Transmission electron microscopy, [CHIM.ANAL]Chemical Sciences/Analytical chemistry, Microscopy, General Materials Science, [PHYS.PHYS.PHYS-CHEM-PH]Physics [physics]/Physics [physics]/Chemical Physics [physics.chem-ph], Physical and Theoretical Chemistry, 0210 nano-technology, Spectroscopy, ComputingMilieux_MISCELLANEOUS, Nanosheet
Abstract

Here, we present a correlative microscopic analysis of electrodeposited films from catechol solutions in aqueous electrolytes. The films were prepared in a miniaturized electrochemical cell and were analyzed by identical location transmission electron microscopy, scanning transmission X-ray microscopy, and atomic force microscopy. Thanks to this combined approach, we have shown that the electrodeposited films are constituted of ultrathin graphite oxide nanosheets. Detailed information about the electronic structure of the films was obtained by X-ray absorption near edge structure spectroscopy. These results show the large potential of soft electrochemical conditions for the bottom-up production of ultrathin graphite oxide nanosheet films via a one-pot green chemistry approach from simple organic building blocks.

Published
2020

11. Morphological and Structural Evolution of Co

Author

Nathaly, Ortiz Peña, Dris, Ihiawakrim, Madeleine, Han, Benedikt, Lassalle-Kaiser, Sophie, Carenco, Clément, Sanchez, Christel, Laberty-Robert, David, Portehault, and Ovidiu, Ersen

Abstract

Unveiling the mechanism of electrocatalytic processes is fundamental for the search of more efficient and stable electrode materials for clean energy conversion devices. Although several

Published
2019

12. Morphological and Structural Evolution of Co3O4 Nanoparticles Revealed by in Situ Electrochemical Transmission Electron Microscopy during Electrocatalytic Water Oxidation

Author

Nathaly Ortiz Peña, Christel Laberty-Robert, David Portehault, Sophie Carenco, Ovidiu Ersen, Clément Sanchez, Dris Ihiawakrim, Benedikt Lassalle-Kaiser, Madeleine Han, Institut de Physique et Chimie des Matériaux de Strasbourg (IPCMS), Université de Strasbourg (UNISTRA)-Centre National de la Recherche Scientifique (CNRS)-Matériaux et nanosciences d'Alsace (FMNGE), Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Réseau nanophotonique et optique, Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA), Novel Advanced Nano-Objects (LCMCP-NANO), Matériaux Hybrides et Nanomatériaux (LCMCP-MHN), Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Synchrotron SOLEIL (SSOLEIL), Centre National de la Recherche Scientifique (CNRS), Chaire Chimie des matériaux hybrides, Reactive Materials for Electrochemical Systems (LCMCP-RMES ), Agence Nationale de la Recherche ANR, ANR-16-CE05-0011,InSiChem,Etude ' in-situ ' et multiéchelle d'électrocatalyseurs pour la conversion d'énergie(2016), Université de Strasbourg (UNISTRA)-Matériaux et nanosciences d'Alsace (FMNGE), and Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Centre National de la Recherche Scientifique (CNRS)-Réseau nanophotonique et optique

Subjects
In situ, Materials science, General Engineering, Oxygen evolution, General Physics and Astronomy, Nanoparticle, 02 engineering and technology, [CHIM.MATE]Chemical Sciences/Material chemistry, 010402 general chemistry, 021001 nanoscience & nanotechnology, Electrochemistry, Electrocatalyst, 01 natural sciences, 7. Clean energy, Structural evolution, 0104 chemical sciences, Chemical engineering, Transmission electron microscopy, [CHIM.ANAL]Chemical Sciences/Analytical chemistry, General Materials Science, 0210 nano-technology, Cobalt oxide, ComputingMilieux_MISCELLANEOUS
Abstract

Unveiling the mechanism of electrocatalytic processes is fundamental for the search of more efficient and stable electrode materials for clean energy conversion devices. Although several in situ te...

Published
2019

13. Studying Electrocatalyts in Operando Conditions: Correlating TEM Imaging and X-Ray Spectroscopies

Author

Dris Ihiawakrim, Ovidiu Ersen, David Portehault, Sophie Carenco, Clément Sanchez, Nathaly Ortiz Peña, and Christel Laberty-Robert

Subjects
Materials science, X-ray, Analytical chemistry, 02 engineering and technology, 010402 general chemistry, 021001 nanoscience & nanotechnology, 0210 nano-technology, 01 natural sciences, Instrumentation, 0104 chemical sciences
Published
2019

14. New pyrazolino and pyrrolidino[60]fullerenes: the introduction of the hydrazone moiety for the formation of metal complexes

Author

Andrea Cabrera-Espinoza, Richard F. D'Vries, Manuel N. Chaur, Elkin L. Romero, Fabio Zuluaga, Monica Soto-Monsalve, and Nathaly Ortiz‐Peña

Subjects
chemistry.chemical_classification, Fullerene derivatives, Fullerene, Organic Chemistry, Hydrazone, 02 engineering and technology, 010402 general chemistry, 021001 nanoscience & nanotechnology, 01 natural sciences, 0104 chemical sciences, Metal, chemistry, visual_art, Polymer chemistry, 1,3-Dipolar cycloaddition, visual_art.visual_art_medium, Organic chemistry, Moiety, Physical and Theoretical Chemistry, 0210 nano-technology
Published
2016

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