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
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Performance and design considerations for lithium excess layered oxide positive electrode materials for lithium ion batteries
TL;DR: The Li-excess oxide compound is one of the most promising positive electrode materials for next generation batteries exhibiting high capacities of >300 mA h g−1 due to the unconventional participation of the oxygen anion redox in the charge compensation mechanism as discussed by the authors.
Journal ArticleDOI
Redox activity of surface oxygen anions in oxygen-deficient perovskite oxides during electrochemical reactions
TL;DR: It is proposed that a narrow electronic state of significant oxygen 2p character near the Fermi level exchanges electrons with the oxygen adsorbates, highlighting the importance of surface anion-redox chemistry in oxygen-deficient transition-metal oxides.
Journal ArticleDOI
Atomic cobalt as an efficient electrocatalyst in sulfur cathodes for superior room-temperature sodium-sulfur batteries.
Binwei Zhang,Tian Sheng,Y. Y. Liu,Yunxiao Wang,Lei Zhang,Weihong Lai,Li Wang,Jianping Yang,Qinfen Gu,Shulei Chou,Hua-Kun Liu,Shi Xue Dou +11 more
TL;DR: A sulfur host comprised of atomic cobalt-decorated hollow carbon nanospheres is synthesized to enhance sulfur reactivity and to electrocatalytically reduce polysulfide into the final product, sodium sulfide.
Journal ArticleDOI
Structure-Induced Reversible Anionic Redox Activity in Na Layered Oxide Cathode
Xiaohui Rong,Jue Liu,Enyuan Hu,Yijin Liu,Yi Wang,Jinpeng Wu,Xiqian Yu,Katharine Page,Yong-Sheng Hu,Wanli Yang,Hong Li,Xiao-Qing Yang,Liquan Chen,Xuejie Huang +13 more
TL;DR: In this paper, a P3-type Na 0.6 [Li 0.2 Mn 0.8 ]O 2 with reversible capacity from pure ARR was studied, and the interlayer O-O distance (peroxo-like O -O dimer, 2.506(3) A), associated with oxidization of oxygen anions, was directly detected by using a neutron total scattering technique.
Journal ArticleDOI
Injection of oxygen vacancies in the bulk lattice of layered cathodes
Pengfei Yan,Jianming Zheng,Zhen-Kun Tang,Zhen-Kun Tang,Arun Devaraj,Guoying Chen,Khalil Amine,Ji-Guang Zhang,Li-Min Liu,Chongmin Wang +9 more
TL;DR: A coupled redox dynamic that needs to be taken into account when designing high-capacity layered cathode materials for high-voltage lithium-ion batteries is unveiled.
References
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Journal ArticleDOI
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.
Journal ArticleDOI
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Journal ArticleDOI
Revised effective ionic radii and systematic studies of interatomic distances in halides and chalcogenides
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Journal ArticleDOI
Issues and challenges facing rechargeable lithium batteries
TL;DR: A brief historical review of the development of lithium-based rechargeable batteries is presented, ongoing research strategies are highlighted, and the challenges that remain regarding the synthesis, characterization, electrochemical performance and safety of these systems are discussed.
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.