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Tarascon J.-M.,CNRS Laboratory of Chemistry and Reactivity of Solids | Tarascon J.-M.,Alistore European Research Institute
Philosophical Transactions of the Royal Society A: Mathematical, Physical and Engineering Sciences | Year: 2010

Batteries are a major technological challenge in this new century as they are a key method to make more efficient use of energy. Although today's Li-ion technology has conquered the portable electronic markets and is still improving, it falls short of meeting the demands dictated by the powering of both hybrid electric vehicles and electric vehicles or by the storage of renewable energies (wind, solar). There is room for optimism as long as we pursue paradigm shifts while keeping in mind the concept of materials sustainability. Some of these concepts, relying on new ways to prepare electrode materials via eco-efficient processes, on the use of organic rather than inorganic materials or new chemistries will be discussed. Achieving these concepts will require the inputs of multiple disciplines. © 2010 The Royal Society.

Rousse G.,University Pierre and Marie Curie | Tarascon J.M.,Collège de France | Tarascon J.M.,CNRS Laboratory of Chemistry and Reactivity of Solids
Chemistry of Materials | Year: 2014

Electrochemical storage has become an integral part of our mobile society and great hopes are being placed in Li-ion batteries to meet future demands dictated by the upcoming electric vehicle (EV) and grid application markets. Batteries with greater autonomy and comprising materials having minimal environmental footprint need to be developed. This calls for both innovative chemistry and new concepts. Currently battery researchers are turning their attention to the design of polyanionic electrodes made up of abundant elements. Here we review recent studies which have led to the synthesis of new sulfate-based polyanionic compounds such as AMSO4X (A = Li, Na, K; M = Fe, Mn, Ni, Co; X = F, OH) and Li2M(SO4)2 (M = Fe, Co, Mn). We highlight their rich crystal chemistry, comment on structural-electrochemical relationships, and report on the feasibility of using the Fe-based compounds as positive electrodes in secondary Li-ion batteries. Additionally, we present premises for an electrochemical-magnetism correlation and offer an outlook on the future of polyanionic compounds. © 2013 American Chemical Society.

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.

Sathiya M.,CSIR - Central Electrochemical Research Institute | Prakash A.S.,CSIR - Central Electrochemical Research Institute | Ramesha K.,CSIR - Central Electrochemical Research Institute | Tarascon J.-M.,CNRS Laboratory of Chemistry and Reactivity of Solids | Shukla A.K.,Indian Institute of Science
Journal of the American Chemical Society | Year: 2011

Functionalized multiwalled carbon nanotubes (CNTs) are coated with a 4-5 nm thin layer of V2O5 by controlled hydrolysis of vanadium alkoxide. The resulting V2O5/CNT composite has been investigated for electrochemical activity with lithium ion, and the capacity value shows both faradaic and capacitive (nonfaradaic) contributions. At high rate (1 C), the capacitive behavior dominates the intercalation as 2/3 of the overall capacity value out of 2700 C/g is capacitive, while the remaining is due to Li-ion intercalation. These numbers are in agreement with the Trasatti plots and are corroborated by X-ray photoelectron spectroscopy (XPS) studies on the V2O5/CNTs electrode, which show 85% of vanadium in the +4 oxidation state after the discharge at 1 C rate. The cumulative high-capacity value is attributed to the unique property of the nano V2O 5/CNTs composite, which provides a short diffusion path for Li +-ions and an easy access to vanadium redox centers besides the high conductivity of CNTs. The composite architecture exhibits both high power density and high energy density, stressing the benefits of using carbon substrates to design high performance supercapacitor electrodes. © 2011 American Chemical Society.

Kassem M.,CNRS Laboratory of Chemistry and Reactivity of Solids | Delacourt C.,CNRS Laboratory of Chemistry and Reactivity of Solids
Journal of Power Sources | Year: 2013

A series of graphite/LFP commercial cells, stored under 3 different conditions of temperature (30, 45, and 60 °C) and SOC (30, 65, and 100%) during up to 8 months, are disassembled and analyzed in order to identify aging phenomena. The recovered positive and negative electrodes are studied using X-ray diffraction, scanning electron microscopy, Fourier transform infrared spectroscopy, and electrochemical testing. The maximum lithium stoichiometry in the recovered cathodes, derived both from XRD data and from electrochemical titration, decreases with an increase of storage temperature and storage SOC. This result confirms that the capacity fade of the commercial cells is caused by the loss of cyclable lithium. From capacity measurements on individual electrodes, any loss of active material is ruled out. Cyclable lithium loss arises from the growth of the solid electrolyte interphase at the anode, as outlined by the presence of a thick and fluffy film at the graphite particle surface for severe aging conditions (e.g., T = 60 °C and SOC = 100%) and an increase of the impedance. Evidence for side reactions at the LFP electrode is provided as well, as demonstrated by the presence of F-rich particles and an impedance increase for the electrodes that aged the most. © 2013 Elsevier B.V. All rights reserved.

Bruce P.G.,University of St. Andrews | Freunberger S.A.,University of St. Andrews | Hardwick L.J.,University of St. Andrews | Hardwick L.J.,University of Liverpool | Tarascon J.-M.,CNRS Laboratory of Chemistry and Reactivity of Solids
Nature Materials | Year: 2012

Li-ion batteries have transformed portable electronics and will play a key role in the electrification of transport. However, the highest energy storage possible for Li-ion batteries is insufficient for the long-term needs of society, for example, extended-range electric vehicles. To go beyond the horizon of Li-ion batteries is a formidable challenge; there are few options. Here we consider two: Ligair (O 2) and LigS. The energy that can be stored in Ligair (based on aqueous or non-aqueous electrolytes) and LigS cells is compared with Li-ion; the operation of the cells is discussed, as are the significant hurdles that will have to be overcome if such batteries are to succeed. Fundamental scientific advances in understanding the reactions occurring in the cells as well as new materials are key to overcoming these obstacles. The potential benefits of Ligair and LigS justify the continued research effort that will be needed.

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.

Poizot P.,CNRS Laboratory of Chemistry and Reactivity of Solids | Dolhem F.,University of Picardie Jules Verne
Energy and Environmental Science | Year: 2011

The fundamental challenge of the 21st century that mankind has to face is definitely energy supply, its storage and conversion in a way that necessarily protects the environment. For 250 years, the tremendous development of humanity has been founded on the harnessing of fossil fuels (coal, crude oil then natural gas) as primary energy due to their high energy density values and the easiness of access. However, this global pattern of energy supply and use is unsustainable. Global warming and finite fossil-fuel supplies call for a radical change in the energy mix to favour renewable energy sources. Without being exhaustive, we tackle in this article the tricky energy question and associated environmental issues as personally perceived. The eminent role of electric energy produced from decarbonized sources in a future sustainable economy is particularly highlighted as well as the issues of its needed storage. The possible and foreseen hindrances of electrochemical energy storage devices, focusing on the lithium-ion technology, are presented in parallel with the possible pathways to make such a technology greener in synergy with the rise of a biomass-based industry. © 2011 The Royal Society of Chemistry.

Melot B.C.,CNRS Laboratory of Chemistry and Reactivity of Solids | Melot B.C.,University of Southern California | Tarascon J.-M.,CNRS Laboratory of Chemistry and Reactivity of Solids
Accounts of Chemical Research | Year: 2013

To meet the growing global demand for energy while preserving the environment, it is necessary to drastically reduce the world's dependence on non-renewable energy sources. At the core of this effort will be the ability to efficiently convert, store, transport and access energy in a variety of ways. Batteries for use in small consumer devices have saturated society; however, if they are ever to be useful in large-scale applications such as automotive transportation or grid-storage, they will require new materials with dramatically improved performance. Efforts must also focus on using Earth-abundant and nontoxic compounds so that whatever developments are made will not create new environmental problems.In this Account, we describe a general strategy for the design and development of new insertion electrode materials for Li(Na)-ion batteries that meet these requirements. We begin by reviewing the current state of the art of insertion electrodes and highlighting the intrinsic material properties of electrodes that must be re-engineered for extension to larger-scale applications. We then present a detailed discussion of the relevant criteria for the conceptual design and appropriate selection of new electrode chemical compositions.We describe how the open-circuit voltage of Li-ion batteries can be manipulated and optimized through structural and compositional tuning by exploiting differences in the electronegativity among possible electrode materials. We then discuss which modern synthetic techniques are most sustainable, allowing the creation of new materials via environmentally responsible reactions that minimize the use of energy and toxic solvents. Finally, we present a case study showing how we successfully employed these approaches to develop a large number of new, useful electrode materials within the recently discovered family of transition metal fluorosulfates. This family has attracted interest as a possible source of improved Li-ion batteries in larger scale applications and benefits from a relatively "green" synthesis. © 2013 American Chemical Society.

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