Journal ArticleDOI
Reversible anionic redox chemistry in high-capacity layered-oxide electrodes
Mariyappan Sathiya,Gwenaëlle Rousse,Kannadka Ramesha,C.P. Laisa,Hervé Vezin,Moulay Tahar Sougrati,Moulay Tahar Sougrati,Marie-Liesse Doublet,Dominique Foix,Danielle Gonbeau,Danielle Gonbeau,Wesley Walker,Annigere S. Prakash,M. Ben Hassine,M. Ben Hassine,Loic Dupont,Loic Dupont,Jean-Marie Tarascon,Jean-Marie Tarascon +18 more
TLDR
In this article, the reactivity of a class of high-capacity oxides with a single redox cation has been investigated and it has been shown that these oxides exhibit sustainable reversible capacities as high as 230 mAh/g−1 and good cycling behavior with no signs of voltage decay.Abstract:
Li-ion batteries have contributed to the commercial success of portable electronics and may soon dominate the electric transportation market provided that major scientific advances including new materials and concepts are developed. Classical positive electrodes for Li-ion technology operate mainly through an insertion-deinsertion redox process involving cationic species. However, this mechanism is insufficient to account for the high capacities exhibited by the new generation of Li-rich (Li1+xNiyCozMn(1−x−y−z)O2) layered oxides that present unusual Li reactivity. In an attempt to overcome both the inherent composition and the structural complexity of this class of oxides, we have designed structurally related Li2Ru1−ySnyO3 materials that have a single redox cation and exhibit sustainable reversible capacities as high as 230 mA h g−1. Moreover, they present good cycling behaviour with no signs of voltage decay and a small irreversible capacity. We also unambiguously show, on the basis of an arsenal of characterization techniques, that the reactivity of these high-capacity materials towards Li entails cumulative cationic (Mn+→M(n+1)+) and anionic (O2−→O22−) reversible redox processes, owing to the d-sp hybridization associated with a reductive coupling mechanism. Because Li2MO3 is a large family of compounds, this study opens the door to the exploration of a vast number of high-capacity materials.read more
Citations
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Journal ArticleDOI
Heteroanionic Materials by Design: Progress Toward Targeted Properties.
TL;DR: The field of anion engineering in oxide-based compounds aims to tune physical properties by incorporating additional anions of different size, electronegativity, and charge as discussed by the authors, which can span a more complex atomic structure design palette and interaction space than the homoanionic oxide-only analogs.
Journal ArticleDOI
Molecular Orbital Principles of Oxygen-Redox Battery Electrodes
Masashi Okubo,Atsuo Yamada +1 more
TL;DR: It is shown that a π-type molecular orbital plays an important role in stabilizing the oxidized oxygen that emerges upon the charging process, providing a solid foundation toward improved oxygen-redox positive electrode materials for high energy-density batteries.
Journal ArticleDOI
Cationic and anionic redox in lithium-ion based batteries
TL;DR: What anionic redox is and the nature of the transition metal and oxygen bond is defined accompanied by three subsequent sections bridging the redox spectrum from pure anionic, to a mix of cationic and anionic and purecationic.
Journal ArticleDOI
Lithium manganese oxyfluoride as a new cathode material exhibiting oxygen redox
Robert A. House,Liyu Jin,Urmimala Maitra,Kazuki Tsuruta,James W. Somerville,Dominic P. Förstermann,Felix Massel,Laurent Duda,Matthew R. Roberts,Peter G. Bruce +9 more
TL;DR: In this paper, the authors reported the discovery of lithium manganese oxyfluoride, specifically the composition, Li1.95, with a high capacity to store charge of 280 mA h g−1 (corresponding to 960 W h kg−1).
Journal ArticleDOI
Atomic Resolution Structural and Chemical Imaging Revealing the Sequential Migration of Ni, Co, and Mn upon the Battery Cycling of Layered Cathode
TL;DR: This work highlights that Ni ions, though acting as the dominant redox species in many LTMO, are labile to migrate to cause lattice disordering upon battery cycling, while the Mn ions are more stable as compared with Ni and Co and can act as pillar to stabilize layered structure.
References
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Generalized Gradient Approximation Made Simple
TL;DR: A simple derivation of a simple GGA is presented, in which all parameters (other than those in LSD) are fundamental constants, and only general features of the detailed construction underlying the Perdew-Wang 1991 (PW91) GGA are invoked.
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Journal ArticleDOI
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Journal ArticleDOI
Issues and challenges facing rechargeable lithium batteries
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Journal ArticleDOI
Building better batteries
TL;DR: Researchers must find a sustainable way of providing the power their modern lifestyles demand to ensure the continued existence of clean energy sources.