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Augustyn V.,University of California at Los Angeles | Come J.,University Paul Sabatier | Come J.,CNRS RS2E | Lowe M.A.,Cornell University | And 8 more authors.
Nature Materials | Year: 2013

Pseudocapacitance is commonly associated with surface or near-surface reversible redox reactions, as observed with RuO2 ·xH 2O in an acidic electrolyte. However, we recently demonstrated that a pseudocapacitive mechanism occurs when lithium ions are inserted into mesoporous and nanocrystal films of orthorhombic Nb2O5 (T-Nb2O5; refs,). Here, we quantify the kinetics of charge storage in T-Nb2O5: currents that vary inversely with time, charge-storage capacity that is mostly independent of rate, and redox peaks that exhibit small voltage offsets even at high rates. We also define the structural characteristics necessary for this process, termed intercalation pseudocapacitance, which are a crystalline network that offers two-dimensional transport pathways and little structural change on intercalation. The principal benefit realized from intercalation pseudocapacitance is that high levels of charge storage are achieved within short periods of time because there are no limitations from solid-state diffusion. Thick electrodes (up to 40 μm thick) prepared with T-Nb2O5 offer the promise of exploiting intercalation pseudocapacitance to obtain high-rate charge-storage devices. © 2013 Macmillan Publishers Limited. All rights reserved.

Augustyn V.,University of California at Los Angeles | Simon P.,University Paul Sabatier | Simon P.,CNRS RS2E | Dunn B.,University of California at Los Angeles
Energy and Environmental Science | Year: 2014

Electrochemical energy storage technology is based on devices capable of exhibiting high energy density (batteries) or high power density (electrochemical capacitors). There is a growing need, for current and near-future applications, where both high energy and high power densities are required in the same material. Pseudocapacitance, a faradaic process involving surface or near surface redox reactions, offers a means of achieving high energy density at high charge-discharge rates. Here, we focus on the pseudocapacitive properties of transition metal oxides. First, we introduce pseudocapacitance and describe its electrochemical features. Then, we review the most relevant pseudocapacitive materials in aqueous and non-aqueous electrolytes. The major challenges for pseudocapacitive materials along with a future outlook are detailed at the end. This journal is © 2014 the Partner Organisations.

Larcher D.,CNRS Laboratory of Chemistry and Reactivity of Solids | Larcher D.,Alistore European Research Institute | Larcher D.,CNRS RS2E | Tarascon J.-M.,Alistore European Research Institute | And 3 more authors.
Nature Chemistry | Year: 2015

Ever-growing energy needs and depleting fossil-fuel resources demand the pursuit of sustainable energy alternatives, including both renewable energy sources and sustainable storage technologies. It is therefore essential to incorporate material abundance, eco-efficient synthetic processes and life-cycle analysis into the design of new electrochemical storage systems. At present, a few existing technologies address these issues, but in each case, fundamental and technological hurdles remain to be overcome. Here we provide an overview of the current state of energy storage from a sustainability perspective. We introduce the notion of sustainability through discussion of the energy and environmental costs of state-of-the-art lithium-ion batteries, considering elemental abundance, toxicity, synthetic methods and scalability. With the same themes in mind, we also highlight current and future electrochemical storage systems beyond lithium-ion batteries. The complexity and importance of recycling battery materials is also discussed. © 2014 Macmillan Publishers Limited. All rights reserved.

Ellis B.L.,Aix - Marseille University | Knauth P.,Aix - Marseille University | Knauth P.,French National Center for Scientific Research | Knauth P.,CNRS RS2E | And 3 more authors.
Advanced Materials | Year: 2014

The miniaturization of power sources aimed at integration into micro- and nano-electronic devices is a big challenge. To ensure the future development of fully autonomous on-board systems, electrodes based on self-supported 3D nanostructured metal oxides have become increasingly important, and their impact is particularly significant when considering the miniaturization of energy storage systems. This review describes recent advances in the development of self-supported 3D nanostructured metal oxides as electrodes for innovative power sources, particularly Li-ion batteries and electrochemical supercapacitors. Current strategies for the design and morphology control of self-supported electrodes fabricated using template, lithography, anodization and self-organized solution techniques are outlined along with different efforts to improve the storage capacity, rate capability, and cyclability. © 2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Franco A.A.,CNRS Laboratory of Chemistry and Reactivity of Solids | Franco A.A.,CNRS RS2E
RSC Advances | Year: 2013

This review focuses on the role of physical theory and computational electrochemistry for fundamental understanding, diagnostics and design of new electrochemical materials and operation conditions for energy storage through rechargeable Li ion batteries (LIBs). More particularly, deep insight based on multiscale physical modelling techniques, spanning scales from few atoms to the device level, can advise about the materials behaviour and aging and how components with optimal specifications could be made and how they can be integrated into operating devices. Concepts and different existing multiscale modelling methodologies are presented and some of the ongoing efforts within the community to understand from physical multiscale modelling and numerical simulation electrochemical mechanisms and degradation processes in LIBs are discussed. Finally, major challenges and perspectives in multiscale modelling for battery applications are highlighted. © 2013 The Royal Society of Chemistry.

Masquelier C.,CNRS Laboratory of Chemistry and Reactivity of Solids | Masquelier C.,French National Center for Scientific Research | Masquelier C.,CNRS RS2E | Croguennec L.,CNRS Laboratory of Condensed Matter Chemistry, Bordeaux | And 2 more authors.
Chemical Reviews | Year: 2013

The concept of investigating three-dimensional frameworks based on the NASICON structure as hosts for reversible insertion/extraction of alkali cations (electrodes) arose in the mid 1980s mostly from concerns about possible stability or reactivity versus metallic Na (or Li) when used as solid electrolytes. The NASICON framework was used by Goodenough in the late 1980s as a very demonstrative example of the possibility for the chemist to elaborate electrode materials functioning at controlled operating voltages. Noticeably, these structures have been recently investigated by three independent groups as model compounds for the understanding of complex Li NMR signals in paramagnetic compounds, and useful insights into the activation energies for hopping between the lithium sites were provided.

Brousse T.,University of Nantes | Brousse T.,CNRS RS2E | Belanger D.,University of Quebec at Montréal | Long J.W.,U.S. Navy
Journal of the Electrochemical Society | Year: 2015

There are an increasing number of studies regarding active electrode materials that undergo faradaic reactions but are used for electrochemical capacitor applications. Unfortunately, some of these materials are described as "pseudocapacitive" materials despite the fact that their electrochemical signature (e.g., cyclic voltammogram and charge/discharge curve) is analogous to that of a "battery"material, as commonly observed for Ni(OH)2 and cobalt oxides in KOH electrolyte. Conversely, true pseudocapacitive electrode materials such as MnO2 display electrochemical behavior typical of that observed for a capacitive carbon electrode. The difference between these two classes of materials will be explained, and we demonstrate why it is inappropriate to describe nickel oxide or hydroxide and cobalt oxide/hydroxide as pseudocapacitive electrode materials. © The Author(s) 2015. Published by ECS.

Croguennec L.,CNRS Laboratory of Condensed Matter Chemistry, Bordeaux | Croguennec L.,Alistore European Research Institute | Croguennec L.,CNRS RS2E | Palacin M.R.,CSIC - Institute of Materials Science | Palacin M.R.,Alistore European Research Institute
Journal of the American Chemical Society | Year: 2015

The lithium-ion battery technology is rooted in the studies of intercalation of guest ions into inorganic host materials developed ca. 40 years ago. It further turned into a commercial product, which will soon blow its 25th candle. Intense research efforts during this time have resulted in the development of a large spectrum of electrode materials together with deep understanding of the underlying structure-property relationships that govern their performance. This has enabled an ever increasing electrochemical yield together with the diversification of the technology into several subfamilies, tailoring materials to application requirements. The present paper aims at providing a global and critical perspective on inorganic electrode materials for lithium-ion batteries categorized by their reaction mechanism and structural dimensionality. Specific emphasis is put on recent research in the field, which beyond the chemistry and microstructure of the materials themselves also involves considering interfacial chemistry concepts alongside progress in characterization techniques. Finally a short personal perspective is provided on some plausible development of the field. © 2015 American Chemical Society.

Simon P.,University Paul Sabatier | Simon P.,CNRS RS2E | Gogotsi Y.,Drexel University
Accounts of Chemical Research | Year: 2013

Securing our energy future is the most important problem that humanity faces in this century. Burning fossil fuels is not sustainable, and wide use of renewable energy sources will require a drastically increased ability to store electrical energy. In the move toward an electrical economy, chemical (batteries) and capacitive energy storage (electrochemical capacitors or supercapacitors) devices are expected to play an important role. This Account summarizes research in the field of electrochemical capacitors conducted over the past decade.Overall, the combination of the right electrode materials with a proper electrolyte can successfully increase both the energy stored by the device and its power, but no perfect active material exists and no electrolyte suits every material and every performance goal. However, today, many materials are available, including porous activated, carbide-derived, and templated carbons with high surface areas and porosities that range from subnanometer to just a few nanometers. If the pore size is matched with the electrolyte ion size, those materials can provide high energy density. Exohedral nanoparticles, such as carbon nanotubes and onion-like carbon, can provide high power due to fast ion sorption/desorption on their outer surfaces. Because of its higher charge-discharge rates compared with activated carbons, graphene has attracted increasing attention, but graphene had not yet shown a higher volumetric capacitance than porous carbons.Although aqueous electrolytes, such as sodium sulfate, are the safest and least expensive, they have a limited voltage window. Organic electrolytes, such as solutions of [N(C2H5) 4]BF4 in acetonitrile or propylene carbonate, are the most common in commercial devices. Researchers are increasingly interested in nonflammable ionic liquids. These liquids have low vapor pressures, which allow them to be used safely over a temperature range from -50 C to at least 100 C and over a larger voltage window, which results in a higher energy density than other electrolytes.In situ characterization techniques, such as nuclear magnetic resonance (NMR), small-angle X-ray scattering (SAXS) and small-angle neutron scattering (SANS), and electrochemical quartz crystal microbalance (EQCM) have improved our understanding of the electrical double layer in confinement and desolvation of ions in narrow pores. Atomisitic and continuum modeling have verified and guided these experimental studies. The further development of materials and better understanding of charged solid-electrolyte interfaces should lead to wider use of capacitive energy storage at scales ranging from microelectronics to transportation and the electrical grid. Even with the many exciting results obtained using newer materials, such as graphene and nanotubes, the promising properties reported for new electrode materials do not directly extrapolate to improved device performance. Although thin films of nanoparticles may show a very high gravimetric power density and discharge rate, those characteristics will not scale up linearly with the thickness of the electrode. © 2012 American Chemical Society.

Monconduit L.,Alistore European Research Institute | Monconduit L.,CNRS RS2E
Journal of Physical Chemistry C | Year: 2014

Nowadays conversion-type electrode materials definitively lie as the core of any research programs related to Li-ion batteries. Requirements are high capacity, good rate capability, and a long cycle life. Indeed, the goal of much lithium battery research is to achieve the highest energy density battery as possible. In the case of pnictide materials, such performances are the results of the following conversion reaction: MxXy + 2yLi ↔ xM0 + yLi3X (X = P, Sb; M = Fe, Ni, Co,...). However, these materials are still suffering from serious issues such as (i) low Coulombic efficiency, (ii) high polarization, (iii) poor cycle life (volume expansion), and (iv) limited rate capability that unfortunately still prevent them for any close commercial viability. In this article, the most recent research developments of our group and through collaborations in this specific field will be reported. In the interest of overcoming the limitations listed above, a cautious and rigorous scrutinizing of the electrochemical behavior of any studied materials is necessary. In our research group, we have extensive experience in the use of sophisticated in and ex situ characterization tools, in the aim to probe bulk pnictide in the Li batteries and the electrolyte/ electrode surface as well. Indeed, thanks to these methods, we could unambiguously show that electrochemical conversion reactions are leading to some unstable phases, which cannot be synthesized via common chemical reaction paths. One can observe the key role of the solid/solid Li3X/M 0 interfaces in the reversibility of the conversion mechanism. Contrarily, during the process, the solid/liquid electrode/electrolyte interfaces are subject to continuous parasitic reactions which drastically limit the cycle life of the battery. Fortunately, both nanostructuration of the pnictide electrodes as well as the confinement of pnictide into a porous carbon matrix play a great role in improving the performance of the cell mainly due (i) to the shortening of the distance over which Li+ diffuses or (ii) to the buffer effect of the carbon matrix against the local volume change during the charge and discharge process. © 2014 American Chemical Society.

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