Electrochemical energy storage is one of the main societal challenges of this century. The performances of classical lithium-ion technology based on liquid electrolytes have made great advances in the past two decades, but the intrinsic instability of liquid electrolytes results in safety issues. Solid polymer electrolytes would be a perfect solution to those safety issues, miniaturization and enhancement of energy density. However, as in liquids, the fraction of charge carried by lithium ions is small (<20%), limiting the power performances. Solid polymer electrolytes operate at 80 °C, resulting in poor mechanical properties and a limited electrochemical stability window. Here we describe a multifunctional single-ion polymer electrolyte based on polyanionic block copolymers comprising polystyrene segments. It overcomes most of the above limitations, with a lithium-ion transport number close to unity, excellent mechanical properties and an electrochemical stability window spanning 5 V versus Li(+)/Li. A prototype battery using this polyelectrolyte outperforms a conventional battery based on a polymer electrolyte.
International audiencePursuing the electrochemical evaluation vs. Li of carbonyl-based cyclic structures deriving from the oxocarbon family, polyketones with N-cyclic structure are investigated to probe the potential modifications. In this communication, we specifically report on the electrochemical investigation of our first selected family of heterocycles based on the 2,3,5,6-tetraketopiperazine unit. Working in a systematic way, a series of tetraketopiperazine molecules with quite different R groups as substituents (i.e., phenyl, allyl and propyl functions) have been synthesized and characterized. Such small molecules were found to rapidly solubilise in commonly used electrolytes. To bypass this issue, we have prepared an oligomeric form via acyclic diene metathesis (ADMET). Preliminary results on the poly-N,N'-diallyl-2,3,5,6-tetraketopiperazine oligomer show a sustained reversible capacity of 110 mAh/g at near 2.45 V. The insight gained from this work is the fact that two intracyclic nitrogen atoms or a lithiated ene-diolate functionality in the C6-based polyketone cyclic structure induces a similar tuning of the redox potential
SummaryThe state of the art of conversion reactions of metal hydrides (MH) with lithium is presented and discussed in this review with regard to the use of these hydrides as anode materials for lithium-ion batteries. A focus on the gravimetric and volumetric storage capacities for different examples from binary, ternary and complex hydrides is presented, with a comparison between thermodynamic prediction and experimental results. MgH2 constitutes one of the most attractive metal hydrides with a reversible capacity of 1480 mA·h·g−1 at a suitable potential (0.5 V vs Li+/Li0) and the lowest electrode polarization (<0.2 V) for conversion materials. Conversion process reaction mechanisms with lithium are subsequently detailed for MgH2, TiH2, complex hydrides Mg2MHx and other Mg-based hydrides. The reversible conversion reaction mechanism of MgH2, which is lithium-controlled, can be extended to others hydrides as: MHx + xLi+ + xe− in equilibrium with M + xLiH. Other reaction paths—involving solid solutions, metastable distorted phases, and phases with low hydrogen content—were recently reported for TiH2 and Mg2FeH6, Mg2CoH5 and Mg2NiH4. The importance of fundamental aspects to overcome technological difficulties is discussed with a focus on conversion reaction limitations in the case of MgH2. The influence of MgH2 particle size, mechanical grinding, hydrogen sorption cycles, grinding with carbon, reactive milling under hydrogen, and metal and catalyst addition to the MgH2/carbon composite on kinetics improvement and reversibility is presented. Drastic technological improvement in order to the enhance conversion process efficiencies is needed for practical applications. The main goals are minimizing the impact of electrode volume variation during lithium extraction and overcoming the poor electronic conductivity of LiH. To use polymer binders to improve the cycle life of the hydride-based electrode and to synthesize nanoscale composite hydride can be helpful to address these drawbacks. The development of high-capacity hydride anodes should be inspired by the emergent nano-research prospects which share the knowledge of both hydrogen-storage and lithium-anode communities.
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