Journal
NATURE COMMUNICATIONS
Volume 10, Issue -, Pages -Publisher
NATURE PUBLISHING GROUP
DOI: 10.1038/s41467-019-13240-z
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Funding
- Deutsche Forschungsgemeinschaft (DFG) [SFB 595]
- Bundesministerium fur Bildung und Forschung (BMBF) [05K16VK2]
- China Scholarship Council (CSC)
- Helmholtz-OCPC Postdoc-Program
- CALIPSOplus [730872]
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One major challenge in the field of lithium-ion batteries is to understand the degradation mechanism of high-energy lithium- and manganese-rich layered cathode materials. Although they can deliver 30 % excess capacity compared with today's commercially- used cathodes, the so-called voltage decay has been restricting their practical application. In order to unravel the nature of this phenomenon, we have investigated systematically the structural and compositional dependence of manganese-rich lithium insertion compounds on the lithium content provided during synthesis. Structural, electronic and electrochemical characterizations of LixNi0.2Mn0.6Oy with a wide range of lithium contents (0.00 <= x <= 1.52, 1.07 <= y < 2.4) and an analysis of the complexity in the synthesis pathways of monoclinic-layered Li[Li0.2Ni0.2Mn0.6]O-2 oxide provide insight into the underlying processes that cause voltage fading in these cathode materials, i.e. transformation of the lithium-rich layered phase to a lithium-poor spinel phase via an intermediate lithium-containing rock-salt phase with release of lithium/oxygen.
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