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Electrode Materials: Fabrication, Properties, and Applications

A special issue of Materials (ISSN 1996-1944). This special issue belongs to the section "Electronic Materials".

Deadline for manuscript submissions: closed (31 December 2021) | Viewed by 31342

Special Issue Editor

Université Paris-Saclay, CEA, CNRS, NIMBE, Laboratoire d’Etude des Eléments Légers LEEL, 91191 Gif-sur-Yvette, France
Interests: Ion Beam Analysis; Solid State Chemistry; Li-ion and Li-air batteries
Special Issues, Collections and Topics in MDPI journals

Special Issue Information

Dear Colleagues,

The success of the energy transition will depend on our capacity to produce, transport, consume, and store energy reliably on a large scale and at a low cost. Electrode materials play an important role in the development of renewable energies. Rechargable batteries are the most appropriate and promising systems. Nowadays, Li-ion batteries (LIBs) dominate the global market for energy storage devices and are used in a variety of applications from portable electronic devices to electrical grid storage and electric vehicles. However, its specific capacity and energy density seem to reach their limits and will be insufficient for the long-term needs of our society. New insertion or conversion materials for electrodes need to be synthesized, in order to provide high energy or high power, sufficient autonomy and low ageing.

The choice of electrode materials determines the electrochemical performances of LIBs. But the synthesis methods are crucial for the properties. Decreasing the particle size and controlling their morphology can improve the electrochemical properties. The substitution of cations by other ions or defects plays a role in electrochemical performances (working potential, electronic and ionic conductivity and consequently the energy density).The present Special Issue is focused on electrode materials preparation and characterization for rechargeable batteries (including lithium-ion, metal-ion and all-solid-state batteries)  but can be extended to supercapacitor electrodes.

We kindly invite you to submit a manuscript for this Special Issue “Electrode Materials: Fabrication, Properties and Applications.” Full papers, communications, and reviews are all welcome.

Dr. Suzy Surblé
Guest Editor

Manuscript Submission Information

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Submitted manuscripts should not have been published previously, nor be under consideration for publication elsewhere (except conference proceedings papers). All manuscripts are thoroughly refereed through a single-blind peer-review process. A guide for authors and other relevant information for submission of manuscripts is available on the Instructions for Authors page. Materials is an international peer-reviewed open access semimonthly journal published by MDPI.

Please visit the Instructions for Authors page before submitting a manuscript. The Article Processing Charge (APC) for publication in this open access journal is 2600 CHF (Swiss Francs). Submitted papers should be well formatted and use good English. Authors may use MDPI's English editing service prior to publication or during author revisions.

Keywords

  • negative and positive electrodes for Li-ion batteries or post Li-ion batteries (Na-ion, Mg-ion, all-solid-state batteries)
  • supercapacitor electrodes
  • nanomaterials
  • synthesis of organic/inorganic materials
  • electrochemical properties

Published Papers (10 papers)

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Research

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14 pages, 3332 KiB  
Article
MIL-53 Metal–Organic Framework as a Flexible Cathode for Lithium-Oxygen Batteries
by Yujie Zhang, Ben Gikonyo, Hicham Khodja, Magali Gauthier, Eddy Foy, Bernard Goetz, Christian Serre, Servane Coste Leconte, Vanessa Pimenta and Suzy Surblé
Materials 2021, 14(16), 4618; https://doi.org/10.3390/ma14164618 - 17 Aug 2021
Cited by 4 | Viewed by 3313
Abstract
Li-air batteries possess higher specific energies than the current Li-ion batteries. Major drawbacks of the air cathode include the sluggish kinetics of the oxygen reduction (OER), high overpotentials and pore clogging during discharge processes. Metal–Organic Frameworks (MOFs) appear as promising materials because of [...] Read more.
Li-air batteries possess higher specific energies than the current Li-ion batteries. Major drawbacks of the air cathode include the sluggish kinetics of the oxygen reduction (OER), high overpotentials and pore clogging during discharge processes. Metal–Organic Frameworks (MOFs) appear as promising materials because of their high surface areas, tailorable pore sizes and catalytic centers. In this work, we propose to use, for the first time, aluminum terephthalate (well known as MIL-53) as a flexible air cathode for Li-O2 batteries. This compound was synthetized through hydrothermal and microwave-assisted routes, leading to different particle sizes with different aspect ratios. The electrochemical properties of both materials seem to be equivalent. Several behaviors are observed depending on the initial value of the first discharge capacity. When the first discharge capacity is higher, no OER occurs, leading to a fast decrease in the capacity during cycling. The nature and the morphology of the discharge products are investigated using ex situ analysis (XRD, SEM and XPS). For both MIL-53 materials, lithium peroxide Li2O2 is found as the main discharge product. A morphological evolution of the Li2O2 particles occurs upon cycling (stacked thin plates, toroids or pseudo-spheres). Full article
(This article belongs to the Special Issue Electrode Materials: Fabrication, Properties, and Applications)
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15 pages, 2676 KiB  
Article
Electrochemical Investigation of Curcumin–DNA Interaction by Using Hydroxyapatite Nanoparticles–Ionic Liquids Based Composite Electrodes
by Merve Uca, Ece Eksin, Yasemin Erac and Arzum Erdem
Materials 2021, 14(15), 4344; https://doi.org/10.3390/ma14154344 - 03 Aug 2021
Cited by 10 | Viewed by 2233
Abstract
Hydroxyapatite nanoparticles (HaP) and ionic liquid (IL) modified pencil graphite electrodes (PGEs) are newly developed in this assay. Electrochemical impedance spectroscopy (EIS), scanning electron microscopy (SEM), energy-dispersive X-ray spectroscopy (EDX), and cyclic voltammetry (CV) were applied to examine the microscopic and electrochemical characterization [...] Read more.
Hydroxyapatite nanoparticles (HaP) and ionic liquid (IL) modified pencil graphite electrodes (PGEs) are newly developed in this assay. Electrochemical impedance spectroscopy (EIS), scanning electron microscopy (SEM), energy-dispersive X-ray spectroscopy (EDX), and cyclic voltammetry (CV) were applied to examine the microscopic and electrochemical characterization of HaP and IL-modified biosensors. The interaction of curcumin with nucleic acids and polymerase chain reaction (PCR) samples was investigated by measuring the changes at the oxidation signals of both curcumin and guanine by differential pulse voltammetry (DPV) technique. The optimization of curcumin concentration, DNA concentration, and the interaction time was performed. The interaction of curcumin with PCR samples was also investigated by gel electrophoresis. Full article
(This article belongs to the Special Issue Electrode Materials: Fabrication, Properties, and Applications)
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11 pages, 2893 KiB  
Article
Novel Lithium-Ion Capacitor Based on a NiO-rGO Composite
by Qi An, Xingru Zhao, Shuangfu Suo and Yuzhu Bai
Materials 2021, 14(13), 3586; https://doi.org/10.3390/ma14133586 - 27 Jun 2021
Cited by 1 | Viewed by 1651
Abstract
Lithium-ion capacitors (LICs) have been widely explored for energy storage. Nevertheless, achieving good energy density, satisfactory power density, and stable cycle life is still challenging. For this study, we fabricated a novel LIC with a NiO-rGO composite as a negative material and commercial [...] Read more.
Lithium-ion capacitors (LICs) have been widely explored for energy storage. Nevertheless, achieving good energy density, satisfactory power density, and stable cycle life is still challenging. For this study, we fabricated a novel LIC with a NiO-rGO composite as a negative material and commercial activated carbon (AC) as a positive material for energy storage. The NiO-rGO//AC system utilizes NiO nanoparticles uniformly distributed in rGO to achieve a high specific capacity (with a current density of 0.5 A g−1 and a charge capacity of 945.8 mA h g−1) and uses AC to provide a large specific surface area and adjustable pore structure, thereby achieving excellent electrochemical performance. In detail, the NiO-rGO//AC system (with a mass ratio of 1:3) can achieve a high energy density (98.15 W h kg−1), a high power density (10.94 kW kg−1), and a long cycle life (with 72.1% capacity retention after 10,000 cycles). This study outlines a new option for the manufacture of LIC devices that feature both high energy and high power densities. Full article
(This article belongs to the Special Issue Electrode Materials: Fabrication, Properties, and Applications)
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16 pages, 3584 KiB  
Article
Electrochemically Activated Screen-Printed Carbon Sensor Modified with Anionic Surfactant (aSPCE/SDS) for Simultaneous Determination of Paracetamol, Diclofenac and Tramadol
by Jędrzej Kozak, Katarzyna Tyszczuk-Rotko, Magdalena Wójciak and Ireneusz Sowa
Materials 2021, 14(13), 3581; https://doi.org/10.3390/ma14133581 - 26 Jun 2021
Cited by 10 | Viewed by 1993
Abstract
In this work, an electrochemically activated screen-printed carbon electrode modified with sodium dodecyl sulfate (aSPCE/SDS) was proposed for the simultaneous determination of paracetamol (PA), diclofenac (DF), and tramadol (TR). Changes of surface morphology and electrochemical behaviour of the electrode after the electrochemical activation [...] Read more.
In this work, an electrochemically activated screen-printed carbon electrode modified with sodium dodecyl sulfate (aSPCE/SDS) was proposed for the simultaneous determination of paracetamol (PA), diclofenac (DF), and tramadol (TR). Changes of surface morphology and electrochemical behaviour of the electrode after the electrochemical activation with H2O2 and SDS surface modification were studied by scanning electron microscopy (SEM), cyclic voltammetry (CV), and electrochemical impedance spectroscopy (EIS). The influence of various parameters on the responses of the aSPCE/SDS such as pH and concentration of the buffer, SDS concentration, and techniques parameters were investigated. Using optimised conditions (Eacc. of −0.4 V, tacc. of 120 s, ΔEA of 150 mV, ν of 250 mV s−1, and tm of 10 ms), the aSPCE/SDS showed a good linear response in the concentration ranges of 5.0 × 10−8–2.0 × 10−5 for PA, 1.0 × 10−9–2.0 × 10−7 for DF, and 1.0 × 10−8–2.0 × 10−7 and 2.0 × 10−7–2.0 × 10−6 mol L−1 for TR. The limits of detection obtained during the simultaneous determination of PA, DF, and TR are 1.49 × 10−8 mol L−1, 2.10 × 10−10 mol L−1, and 1.71 × 10−9 mol L−1, respectively. The selectivity of the aSPCE/SDS was evaluated by examination of the impact of some inorganic and organic substances that are commonly present in environmental and biological samples on the responses of PA, DF, and TR. Finally, the differential pulse adsorptive stripping voltammetric (DPAdSV) procedure using the aSPCE/SDS was successfully applied for the determination of PA, DF, and TR in river water and serum samples as well as pharmaceuticals. Full article
(This article belongs to the Special Issue Electrode Materials: Fabrication, Properties, and Applications)
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19 pages, 3817 KiB  
Article
Electrode Design for MnO2-Based Aqueous Electrochemical Capacitors: Influence of Porosity and Mass Loading
by Camille Douard, Laurence Athouël, David Brown, Olivier Crosnier, Guillaume Rebmann, Oliver Schilling and Thierry Brousse
Materials 2021, 14(11), 2990; https://doi.org/10.3390/ma14112990 - 01 Jun 2021
Cited by 17 | Viewed by 3245
Abstract
The purpose of this study is to highlight the influence of some fabrication parameters, such as mass loading and porosity, which are not really elucidated and standardized during the realization of electrodes for supercapacitors, especially when using metal oxides as electrode materials. Electrode [...] Read more.
The purpose of this study is to highlight the influence of some fabrication parameters, such as mass loading and porosity, which are not really elucidated and standardized during the realization of electrodes for supercapacitors, especially when using metal oxides as electrode materials. Electrode calendering, as one stage during the fabrication of electrodes, was carried out step-by-step on manganese dioxide electrodes to study the decreasing porosity effect on the electrochemical performance of a MnO2 symmetric device. One other crucial parameter, the mass loading, which has to be understood and well used for realistic supercapacitors, was investigated concurrently. Gravimetric, areal and volumetric capacitances are highlighted, varying the porosity for low-, medium- and large-mass loading. Low-loading leads to the best specific capacitances but is not credible for realistic supercapacitors, except for microdevices. Down 50% porosities after calendering, capacitances are increased and become stable faster, suggesting a faster wettability of the dense electrodes by the electrolyte, especially for high-mass loading. EIS experiments performed on electrodes without and with calendering lead to a significant decrease of the device’s time response, especially at high loading. A high-mass loading device seems to work as a power battery, whereas electrode calendaring, which allows decreasing the time response, leads to an electrical behavior closer to that expected for a supercapacitor. Full article
(This article belongs to the Special Issue Electrode Materials: Fabrication, Properties, and Applications)
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11 pages, 3205 KiB  
Article
Composite Fe3O4-MXene-Carbon Nanotube Electrodes for Supercapacitors Prepared Using the New Colloidal Method
by Wenyu Liang and Igor Zhitomirsky
Materials 2021, 14(11), 2930; https://doi.org/10.3390/ma14112930 - 29 May 2021
Cited by 10 | Viewed by 3404
Abstract
MXenes, such as Ti3C2Tx, are promising materials for electrodes of supercapacitors (SCs). Colloidal techniques have potential for the fabrication of advanced Ti3C2Tx composites with high areal capacitance (CS). This paper [...] Read more.
MXenes, such as Ti3C2Tx, are promising materials for electrodes of supercapacitors (SCs). Colloidal techniques have potential for the fabrication of advanced Ti3C2Tx composites with high areal capacitance (CS). This paper reports the fabrication of Ti3C2TX-Fe3O4-multiwalled carbon nanotube (CNT) electrodes, which show CS of 5.52 F cm−2 in the negative potential range in 0.5 M Na2SO4 electrolyte. Good capacitive performance is achieved at a mass loading of 35 mg cm−2 due to the use of Celestine blue (CB) as a co-dispersant for individual materials. The mechanisms of CB adsorption on Ti3C2TX, Fe3O4, and CNTs and their electrostatic co-dispersion are discussed. The comparison of the capacitive behavior of Ti3C2TX-Fe3O4-CNT electrodes with Ti3C2TX-CNT and Fe3O4-CNT electrodes for the same active mass, electrode thickness and CNT content reveals a synergistic effect of the individual capacitive materials, which is observed due to the use of CB. The high CS of Ti3C2TX-Fe3O4-CNT composites makes them promising materials for application in negative electrodes of asymmetric SC devices. Full article
(This article belongs to the Special Issue Electrode Materials: Fabrication, Properties, and Applications)
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16 pages, 25325 KiB  
Article
High Capacity Nanocomposite Layers Based on Nanoparticles of Carbon Materials and Ruthenium Dioxide for Potassium Sensitive Electrode
by Nikola Lenar, Robert Piech and Beata Paczosa-Bator
Materials 2021, 14(5), 1308; https://doi.org/10.3390/ma14051308 - 09 Mar 2021
Cited by 9 | Viewed by 1822
Abstract
This work presents the new concept of designing ion-selective electrodes based on the use of new composite materials consisting of carbon nanomaterials and ruthenium dioxide. Using two different materials varying in microstructure and properties, we could obtain one material for the mediation layer [...] Read more.
This work presents the new concept of designing ion-selective electrodes based on the use of new composite materials consisting of carbon nanomaterials and ruthenium dioxide. Using two different materials varying in microstructure and properties, we could obtain one material for the mediation layer that adopted features coming of both components. Ruthenium dioxide characterized by high electrical capacity and mixed electronic-ionic transduction and nano-metric carbon materials were reportedly proved to improve the properties of ion-selective electrodes. Initially, only the materials and then the final electrodes were tested in the scope of the presented work, using scanning and transmission electron microscope, contact angle microscope, and various electrochemical techniques, including electrochemical impedance spectroscopy and chronopotentiometry. The obtained results confirmed beneficial influence of the designed nanocomposites on the ion-selective electrodes’ properties. Nanosized structure, high capacity (characterized by the electrical capacitance value from approximately 5.5 mF for GR + RuO2 and CB + RuO2, up to 14 mF for NT + RuO2) and low hydrophilicity (represented by the contact angle from 60° for GR+RuO2, 80° for CB+RuO2, and up to 100° for NT + RuO2) of the mediation layer materials, allowed us to obtain water layer-free potassium-selective electrodes, characterized by rapid and stable potentiometric response in a wide range of concentrations-from 10−1 to 10−6 M K+. Full article
(This article belongs to the Special Issue Electrode Materials: Fabrication, Properties, and Applications)
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10 pages, 2938 KiB  
Article
Enhanced Electrochemical Performance Promoted by Tin in Silica Anode Materials for Stable and High-Capacity Lithium-Ion Batteries
by Xuli Ding, Daowei Liang and Hongda Zhao
Materials 2021, 14(5), 1071; https://doi.org/10.3390/ma14051071 - 25 Feb 2021
Cited by 20 | Viewed by 2496
Abstract
Although the silicon oxide (SiO2) as an anode material shows potential and promise for lithium-ion batteries (LIBs), owing to its high capacity, low cost, abundance, and safety, severe capacity decay and sluggish charge transfer during the discharge–charge process has caused a [...] Read more.
Although the silicon oxide (SiO2) as an anode material shows potential and promise for lithium-ion batteries (LIBs), owing to its high capacity, low cost, abundance, and safety, severe capacity decay and sluggish charge transfer during the discharge–charge process has caused a serious challenge for available applications. Herein, a novel 3D porous silicon oxide@Pourous Carbon@Tin (SiO2@Pc@Sn) composite anode material was firstly designed and synthesized by freeze-drying and thermal-melting self-assembly, in which SiO2 microparticles were encapsulated in the porous carbon as well as Sn nanoballs being uniformly dispersed in the SiO2@Pc-like sesame seeds, effectively constructing a robust and conductive 3D porous Jujube cake-like architecture that is beneficial for fast ion transfer and high structural stability. Such a SiO2@Pc@Sn micro-nano hierarchical structure as a LIBs anode exhibits a large reversible specific capacity ~520 mAh·g−1, initial coulombic efficiency (ICE) ~52%, outstanding rate capability, and excellent cycling stability over 100 cycles. Furthermore, the phase evolution and underlying electrochemical mechanism during the charge–discharge process were further uncovered by cyclic voltammetry (CV) investigation. Full article
(This article belongs to the Special Issue Electrode Materials: Fabrication, Properties, and Applications)
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13 pages, 10754 KiB  
Article
Electrochemical Performance Enhancement of Micro-Sized Porous Si by Integrating with Nano-Sn and Carbonaceous Materials
by Tiantian Yang, Hangjun Ying, Shunlong Zhang, Jianli Wang, Zhao Zhang and Wei-Qiang Han
Materials 2021, 14(4), 920; https://doi.org/10.3390/ma14040920 - 15 Feb 2021
Cited by 3 | Viewed by 2570
Abstract
Silicon is investigated as one of the most prospective anode materials for next generation lithium ion batteries due to its superior theoretical capacity (3580 mAh g−1), but its commercial application is hindered by its inferior dynamic property and poor cyclic performance. [...] Read more.
Silicon is investigated as one of the most prospective anode materials for next generation lithium ion batteries due to its superior theoretical capacity (3580 mAh g−1), but its commercial application is hindered by its inferior dynamic property and poor cyclic performance. Herein, we presented a facile method for preparing silicon/tin@graphite-amorphous carbon (Si/Sn@G–C) composite through hydrolyzing of SnCl2 on etched Fe–Si alloys, followed by ball milling mixture and carbon pyrolysis reduction processes. Structural characterization indicates that the nano-Sn decorated porous Si particles are coated by graphite and amorphous carbon. The addition of nano-Sn and carbonaceous materials can effectively improve the dynamic performance and the structure stability of the composite. As a result, it exhibits an initial columbic efficiency of 79% and a stable specific capacity of 825.5 mAh g−1 after 300 cycles at a current density of 1 A g−1. Besides, the Si/Sn@G–C composite exerts enhanced rate performance with 445 mAh g−1 retention at 5 A g−1. This work provides an approach to improve the electrochemical performance of Si anode materials through reasonable compositing with elements from the same family. Full article
(This article belongs to the Special Issue Electrode Materials: Fabrication, Properties, and Applications)
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Review

Jump to: Research

25 pages, 3506 KiB  
Review
A Critical Review for an Accurate Electrochemical Stability Window Measurement of Solid Polymer and Composite Electrolytes
by Adrien Méry, Steeve Rousselot, David Lepage and Mickaël Dollé
Materials 2021, 14(14), 3840; https://doi.org/10.3390/ma14143840 - 09 Jul 2021
Cited by 39 | Viewed by 7035
Abstract
All-solid-state lithium batteries (ASSLB) are very promising for the future development of next generation lithium battery systems due to their increased energy density and improved safety. ASSLB employing Solid Polymer Electrolytes (SPE) and Solid Composite Electrolytes (SCE) in particular have attracted significant attention. [...] Read more.
All-solid-state lithium batteries (ASSLB) are very promising for the future development of next generation lithium battery systems due to their increased energy density and improved safety. ASSLB employing Solid Polymer Electrolytes (SPE) and Solid Composite Electrolytes (SCE) in particular have attracted significant attention. Among the several expected requirements for a battery system (high ionic conductivity, safety, mechanical stability), increasing the energy density and the cycle life relies on the electrochemical stability window of the SPE or SCE. Most published works target the importance of ionic conductivity (undoubtedly a crucial parameter) and often identify the Electrochemical Stability Window (ESW) of the electrolyte as a secondary parameter. In this review, we first present a summary of recent publications on SPE and SCE with a particular focus on the analysis of their electrochemical stability. The goal of the second part is to propose a review of optimized and improved electrochemical methods, leading to a better understanding and a better evaluation of the ESW of the SPE and the SCE which is, once again, a critical parameter for high stability and high performance ASSLB applications. Full article
(This article belongs to the Special Issue Electrode Materials: Fabrication, Properties, and Applications)
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