Arnaud Demortiere

Arnaud Demortiere
French National Centre for Scientific Research | CNRS · RS2E/LRCS

PhD

About

111
Publications
20,669
Reads
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3,716
Citations
Introduction
In-situ and operando electron microscopy for battery materials. Nanomaterials, Nanocrystals, heterostructure and organic/inorganic composite materials. Self-organization and active colloids.
Additional affiliations
October 2014 - August 2015
RS2E
Position
  • Materials Scientist CNRS-CR1-Institute of Chemistry
October 2013 - September 2014
IIT/ Argonne NL
Position
  • Research Assistant
January 2010 - September 2013
Argonne National Laboratory
Position
  • Argonne National Lab
Education
September 2003 - April 2007
Sorbonne Université
Field of study
  • Nanomaterials

Publications

Publications (111)
Article
Full-text available
The segmentation of tomographic images of the battery electrode is a crucial processing step, which will have an additional impact on the results of material characterization and electrochemical simulation. However, manually labeling X-ray CT images (XCT) is time-consuming, and these XCT images are generally difficult to segment with histographical...
Article
Full-text available
Image perception plays a fundamental role in the tomography-based approaches for microstructure characterization and has a deep impact on all subsequent stages of image processing, such as segmentation and 3D analysis. The enhancement of image perception, however, frequently involves observer-dependence, which reflects user-to-user dispersion and u...
Preprint
Full-text available
Microstructural evolution of NMC secondary particles during the battery operation drives the electrochemical performance and impacts the Li-ion battery lifetime. In this work, we develop an in situ methodology using the FIB/SEM instrument to cycle single secondary particles of NMC active materials while following the modifications of their 3D morph...
Preprint
Full-text available
The demand for lithium ion batteries (LIBs) on the market has gradually risen, with production increasing every year. To meet industrial needs, the development of digital twins designed to optimize LIB manufacturing processes is essential. Here, by using LiNi0.33Co0.33Mn0.33O2 (NMC111) material as an example, we introduce the realistic particles sh...
Article
In this second of this series of papers, the use of two physics-based models to analyze the discharge performance of a set of high-energy-density electrodes is discussed. The measured set of parameters from the first part is implemented into these models. First, the regular Newman pseudo-2D model shows a large discrepancy against the experimental v...
Article
Physics-based models of the Li-ion battery promise to aid in deciphering and quantifying electrode limitations, thereby providing valuable insights for choosing the optimal electrode design for a specific application. However, to obtain relevant results from the models, a reliable set of input parameters is required. This work presents a combined e...
Article
For the first time, chemical surface modification, using an hybrid organic/inorganic approach and its impact on the electrochemical response of a nanometric lithium iron phosphate obtained by the facile solvothermal method using an organic capping agent is investigated. Removal of the capping agent was realized through different approaches, such as...
Cover Page
Full-text available
In‐Situ Cycling In article number 2100891, Demortiére and co‐workers demonstrate that in‐situ cycling of a LiMn1.5Ni0.5O4 thin‐film cathode in an electrochemical transmission electron microscope (TEM) holder reveals structural and morphologic changes upon (de)lithiation processes. (S)TEM images of the cycled thin‐film reveal the formation of voids,...
Article
In this article we demonstrate that in-situ cycling of a LiMn1.5Ni0.5O4 thin-film cathode in an electrochemical transmission electron microscope (TEM) holder reveals structural and morphologic changes upon (de)lithiation processes. (S)TEM images of the cycled thin-film reveal the formation of voids, cracks, and organic decomposition products. The 4...
Article
Performing high resolution 3D imaging with transmission X‐ray microscopy (TXM) in an in situ battery system is extremely challenging. We show herein a method to conduct an in situ nano‐X ray Computed Tomography (nano‐XCT) experiment assisted by the in‐line phase contrast technique for low Z elements in batteries. A carbon‐based O2‐cathode of Li‐O2...
Article
Micro-batteries are attractive miniaturized energy devices for new Internet of Things applications, but the lack of understanding of their degradation process during cycling hinders improving their performance. Here focused ion beam (FIB)-lamella from LiMn1.5Ni0.5O4 (LMNO) thin-film cathode is in situ cycled in a liquid electrolyte inside an electr...
Article
Environmental stability is a major bottleneck of perovskite solar cells. Only a handful of studies are investigating the effect of moisture on the structural degradation of the absorber. They mostly rely on ex situ experiments and on completely degraded samples which restrict the assessment on initial and final stage. By combining in situ X-ray dif...
Article
Li3PS4 is an attractive solid-electrolyte material that possesses high RT ionic conductivity (10⁻⁴ S.cm⁻¹) but the effects of specific synthesis parameters on the material's local structure and transport properties still demand clarifications. Herein, we highlight the substantial effects of cooling breaks in the mechanochemical synthesis procedure...
Article
Full-text available
This is a critical review of artificial intelligence/machine learning (AI/ML) methods applied to battery research. It aims at providing a comprehensive, authoritative, and critical, yet easily understandable, review of general interest to the battery community. It addresses the concepts, approaches, tools, outcomes, and challenges of using AI/ML as...
Conference Paper
All solid state Li-ion micro-battery is a promising candidate to power miniaturized sensors for Internet of things (IOT) and other electronic devices. In recent times, the spinel LiMn 1.5 Ni 0.5 O 4 (LNMO) has demonstrated as a potential positive electrode material for Li-ion thin film batteries offering a theoretical capacity of 147 mAh/g (65 µAh/...
Article
Thick electrodes with high active material loadings have been intensively studied over the last couple of decades in pursuit of achieving high energy density systems. To optimize and enhance the electrochemical performance of such electrodes, one has to control the pore morphology by, for example, varying the pore size and shape, and the level of p...
Article
Full-text available
Li-O2 batteries offer a high theoretical discharge capacity due to the formation of light discharged species such as Li2O2, which fill the porous positive electrode. However, in practice, it is challenging to reach the theoretical capacity and completely utilize the full electrode pore volume during discharge. With the formation of discharge produc...
Article
We describe and demonstrate an optimization-based X-ray image reconstruction framework called Adorym. Our framework provides a generic forward model, allowing one code framework to be used for a wide range of imaging methods ranging from near-field holography to fly-scan ptychographic tomography. By using automatic differentiation for optimization,...
Article
Despite significant progress in the field of tomography, capturing the carbon binder domain (CBD) morphology presented in the Li‐ion electrode remains challenging, due to its low attenuation coefficient. In this work, quantitative phase contrast X‐ray nano‐holotomography is used as a straightforward approach that provides a large reconstructed volu...
Preprint
Full-text available
We describe and demonstrate an optimization-based x-ray image reconstruction framework called Adorym. Our framework provides a generic forward model, allowing one code framework to be used for a wide range of imaging methods ranging from near-field holography to and fly-scan ptychographic tomography. By using automatic differentiation for optimizat...
Article
Full-text available
In this work, in situ X‐ray diffraction (XRD), in operando liquid‐cell transmission electron microscopy (TEM) and ex situ solid‐state (ss)NMR spectroscopy are combined with time‐resolved spectroscopies to reveal new insights about the degradation mechanisms of methylammonium lead halide (MAPbI3) under 85% relative humidity (RH) at different length...
Article
Full-text available
The tortuosity factor of porous battery electrodes is an important parameter used to correlate electrode microstructure with performance through numerical modeling. Therefore, having an appropriate method for the accurate determination of tortuosity factors is critical. This paper presents a numerical approach, based on simulations performed on num...
Article
Compared to conventional Li/Na-ion batteries, in which reversible energy storage relies on the use of redox active transition metal oxides as positive electrodes, the metal-O 2 battery systems would theoretically offer greater energy density owing to the use of the redox of gaseous oxygen using conductive and light carbon electrodes. Although in so...
Article
It’s well known that the Li-O 2 battery can achieve theoretically ¹ ten times as much energy density (5200Wh/kg) as Li-ion battery but often limited in reality on the capacity and the cycling. In this system, the carbon cathode provides merely a framework for the lithium peroxide deposition but is not an active material. The dissolved oxygen in the...
Conference Paper
All solid state Li-ion micro-battery is a promising candidate to power miniaturized sensors for Internet of things (IOT) and other electronic devices. The LiNi 0.5 Mn 1.5 O 4 spinel (LNMO) is a potential positive electrode material for Li-ion micro-batteries offering a theoretical capacity of 147 mAh/g (65 µAh/cm ² /µm for a bulk density of 4.47 g/...
Article
The tortuosity factor of porous electrode microstructure is a crucial input parameter for numerical models of batteries as it strongly influences the electrode performance. As such, it is very important to have a method to determine this parameter accurately, based on a definition that reflects the design of the cell. Various experimental methods h...
Article
A further development of the rechargeable and long-lasting ion-batteries requires a comprehensive study of a plenty of processes undergoing on micro- and nano-scale in cathode active material during battery charge/discharge cycle. The discharge process results in significant transformations of the cathode’s structure while trying to accommodate the...
Article
Full-text available
We investigated the lithium peroxide (Li2O2) and pore size distribution in lithium-O2 battery electrodes at different states of charge using transmission X-ray microscopy coupled with Zernike phase contrast to carry out nano-Computed Tomography. We report that such technique enables, at the nanoscale, to distinguish light elements such as carbon an...
Article
In the literature, reported 3D-resolved models rely on oversimplifications, such as an implicit representation of the carbon-binder domains (CBD) through the use of effective parameters for porosity and tortuosity or by merging CBD with the Active Material (AM) as a single solid phase. This work’s novelty relies on the explicit representation of CB...
Article
Operando Liquid-electrochemical TEM for Monitoring Growth and Dissolution Steps of NaO2 Cubes in Na-O2 Battery - Volume 25 Supplement - Walid Dachraoui, Lukas Lutz, Lee. R. Johnson, Peter G. Bruce, Jean-Marie Tarascon, Alexis Grimaud, Arnaud Demortière
Article
In Situ Electron Diffraction using Liquid-Electrochemical TEM for Monitoring Structural Transformation in Single Crystals Of Cathode Materials for Li-Ion Batteries - Volume 25 Supplement - Olesia M. Karakulina, Walid Dachraoui, Artem M. Abakumov, Joke Hadermann, Arnaud Demortière
Article
Investigation of the Oxidation Reaction of LiFePO4 Cathode Material using Environmental TEM - Volume 25 Supplement - Matthieu Bugnet, Thierry Epicier, Martial Duchamp, Nadir Recham, Tristan Lombard, Christian Masquelier, Arnaud Demortière
Article
Full-text available
Manipulating the atomic structure of semiconductors is a fine way to tune their properties. The rationalization of their modified properties is, however, particularly challenging as defects locally disrupt the long-range structural ordering, and a deeper effort is required to fully describe their structure. In this work, we investigated the photoel...
Article
The fabrication of high energy density on chip Li-ion micro-battery with high power capabilities is still a major challenge. For planar micro-batteries, thick electrode is mandatory for the energy issue but the rate capability of such thick layer is limited by the kinetic of the lithium ion within the film. In this work, sputtered LiMn1.5Ni0.5O4 (L...
Article
Full-text available
Micro‐supercapacitors (MSC) are considered as promising miniaturized electrochemical energy storage devices for Internet of Things applications. Unfortunately, the technological readiness level of these devices is still at the lab scale with the development of individual prototypes due to the difficulty to produce high performance porous electrode...
Article
The templating approach is a powerful method for preparing porous electrodes with interconnected well-controlled pore sizes and morphologies. The optimization of the pore architecture design facilitates electrolyte penetration and provides a rapid diffusion path for lithium ion, which becomes even more crucial for thick porous electrodes. In the pr...
Article
We developed in the present paper the synthesis of a new AB3-type compound LaMg2Ni5Al4 by mechanical alloying (MA) process. X-ray diffraction analysis (XRD) was used to determine the structural properties and the phase evolution of the powder mixtures. Two different synthesis pathways have been investigated. The first starting from elemental metals...
Article
Full-text available
Colloidal semiconductor nanocrystals are commonly grown with a shell of a second semiconductor material to obtain desired physical properties, such as increased photoluminescence quantum yield. However, the growth of a lattice-mismatched shell results in strain within the nanocrystal, and this strain has the potential to produce crystalline defects...
Article
Full-text available
The templating approach is a powerful method for preparing porous electrodes with interconnected well-controlled pore sizes and morphologies. The optimization of the pore architecture design facilitates electrolyte penetration and provides a rapid diffusion path for lithium ions, which becomes even more crucial for thick porous electrodes. Here, Na...
Article
While large dispersions in electrochemical performance have been reported for lithium oxygen batteries in the literature, they have not been investigated in any depth. The variability in the results is often assumed to arise from differences in cell design, electrode structure, handling and cell preparation at different times. An accurate theoretic...
Article
Full-text available
In contrast to monovalent lithium or sodium ions, the reversible insertion of multivalent ions such as Mg2+ and Al3+ into electrode materials remains an elusive goal. Here, we demonstrate a new strategy to achieve reversible Mg2+ and Al3+ insertion in anatase TiO2, achieved through aliovalent doping, to introduce a large number of titanium vacancie...
Article
Full-text available
The fabrication of high-performance on-chip 3D micro-supercapacitors (MSCs) based on MnO2 pseudocapacitive binder-free thin film electrodes (<500 nm thick) with interdigitated topology is reported. An original technological process easily scalable to pilot production line is proposed on 3 in. silicon wafers. High areal energy (>10 µW h cm−2) and po...
Article
Full-text available
The areal energy density of on-chip micro-supercapacitors should be improved in order to obtain autonomous smart miniaturized sensors. To reach this goal, high surface capacitance electrode (>100 mF cm−2) has to be produced while keeping low the footprint area. For carbide-derived carbon (CDC) micro-supercapacitors, the properties of the metal carb...
Article
Full-text available
The oxygen evolution reaction (OER) is of prime importance in multiple energy storage devices; however, deeper mechanistic understanding is required to design enhanced electrocatalysts for the reaction. Current understanding of the OER mechanism based on oxygen adsorption on a metallic surface site fails to fully explain the activity of iridium and...
Chapter
Liquid cell electron microscopy is a developing technique that allows us to apply the powerful capabilities of the electron microscope to image and analyze materials immersed in liquid. We are thus able to examine liquid based processes in materials science and physics that are traditionally inaccessible with conventional TEM. The liquid/bias seale...
Chapter
Lithium-Sulfur batteries are thought to be the future of Li-ion batteries thanks to their high theoretical specific capacity (1675 mAh.g⁻¹) and low-cost. However, the real-life application of Lithium-Sulfur batteries is still hindered by limitations such as the formation of highly insulating and insoluble species at the cathode (e.g. Li2S), mechani...
Chapter
Microwave assisted synthesis of metallic nanoparticles is an attractive way for the elaboration of electrocatalysts using energy efficient processes. This method consists in the use of a weak reducing agent that acts as solvent with high boiling point at the same time. Among the possible solvents, diethylene glycol is one of the most suitable molec...
Chapter
Over the past fifteen years, the Platform of Electron Microscopy at the University of Picardy Jules Verne (PME UPJV) has been developing in situ scanning electron microscopy techniques to successfully observe polymer [1] and solid or liquid electrolyte lithium-ion batteries cycling in the scanning electron microscope (figure 1). In situ Electron Mi...
Chapter
This last decade, fundamental studies of electrochemical phenomena have been slowed down by a lack of effective in situ (and operando) experimental setup, which is able to clearly identify structural modifications inside and at the surface of electrode materials. The evolution of microstructures, the appearance of cracks and porosities and the tran...
Article
The oxygen evolution reaction (OER) is of prime importance in multiple energy storage devices; however, deeper mechanistic understanding is required to design enhanced electrocatalysts for the reaction. Current understanding of the OER mechanism based on oxygen adsorption on a metallic surface site fails to fully explain the activity of iridium and...
Conference Paper
Full-text available
div class="title"> In-Situ Liquid/Bias Transmission Electron Microscopy to Visualize the Electrochemical Lithiation/Delithiation Behaviors of LiFe 0.5 Mn 0.5 PO 4 - Volume 22 Issue S5 - Walid Dachraoui, Olesia Kurkulina, Joke Hadermann, Arnaud Demortière