期刊
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
卷 138, 期 35, 页码 11211-11218出版社
AMER CHEMICAL SOC
DOI: 10.1021/jacs.6b05111
关键词
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资金
- EPSRC
- SUPREGEN program
- Swedish Research Council (VR)
- Diamond Light Source as part of the Energy Materials Block Allocation Group [SP14239]
- Office of Science, Office of Basic Energy Sciences, US Department of Energy [DE-AC02-05CH11231]
- EPSRC [EP/I029273/1, EP/M009521/1, EP/L019469/1, EP/I029273/2, EP/M009394/1] Funding Source: UKRI
- Engineering and Physical Sciences Research Council [EP/M009394/1, EP/M009521/1, EP/I029273/1, EP/I029273/2, EP/L019469/1] Funding Source: researchfish
Conventional intercalation cathodes for lithium batteries store charge in redox reactions associated with the transition metal cations, e.g., Mn3+/4+ in LiMn2O4, and this limits the energy storage of Li-ion batteries. Compounds such as Li[Li0.2Ni0.2Mn0.6]O-2 exhibit a capacity to store charge in excess of the transition metal redox reactions. The additional capacity occurs at and above 4.5 V versus Li+/Li. The capacity at 4.5 V is dominated by oxidation of the O-2(-) anions accounting for similar to 0.43 e(-)/formula unit, with an additional 0.06 e(-)/formula unit being associated with O loss from the lattice. In contrast, the capacity above 4.5 V is mainly O loss, similar to 0.08 e(-)/formula. The O redox reaction involves the formation of localized hole states on O during charge, which are located on O coordinated by (Mn4+/Li+). The results have been obtained by combining operando electrochemical mass spec on 180 labeled Li[Li0.2Ni0.2Mn0.6]O-2 with XANES, soft X-ray spectroscopy, resonant inelastic X-ray spectroscopy, and Raman spectroscopy. Finally the general features of O redox are described with discussion about the role of comparatively ionic (less covalent) 3d metal oxygen interaction on anion redox in lithium rich cathode materials.
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