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28 March 2024
 
  » arxiv » 1811.5964

 Article overview


High Reversibility of Lattice Oxygen Redox in Na-ion and Li-ion Batteries Quantified by Direct Bulk Probes of both Anionic and Cationic Redox Reactions
Kehua Dai ; Jinpeng Wu ; Zengqing Zhuo ; Qinghao Li ; Shawn Sallis ; Jing Mao ; Guo Ai ; Chihang Sun ; Zaiyuan Li ; William E. Gent ; William C. Chueh ; Yi-de Chuang ; Rong Zeng ; Zhi-xun Shen ; Feng Pan ; Shishen Yan ; Louis F. J. Piper ; Zahid Hussain ; Gao Liu ; Wanli Yang ;
Date 14 Nov 2018
AbstractThe reversibility and cyclability of anionic redox in battery electrodes hold the key to its practical employments. Here, through mapping of resonant inelastic X-ray scattering (mRIXS), we have independently quantified the evolving redox states of both cations and anions in Na2/3Mg1/3Mn2/3O2. The bulk-Mn redox emerges from initial discharge and is quantified by inverse-partial fluorescence yield (iPFY) from Mn-L mRIXS. Bulk and surface Mn activities likely lead to the voltage fade. O-K super-partial fluorescence yield (sPFY) analysis of mRIXS shows 79% lattice oxygen-redox reversibility during initial cycle, with 87% capacity sustained after 100 cycles. In Li1.17Ni0.21Co0.08Mn0.54O2, lattice-oxygen redox is 76% initial-cycle reversible but with only 44% capacity retention after 500 cycles. These results unambiguously show the high reversibility of lattice-oxygen redox in both Li-ion and Na-ion systems. The contrast between Na2/3Mg1/3Mn2/3O2 and Li1.17Ni0.21Co0.08Mn0.54O2 systems suggests the importance of distinguishing lattice-oxygen redox from other oxygen activities for clarifying its intrinsic properties.
Source arXiv, 1811.5964
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