Is it universal that the layered-spinel structure can improve electrochemical performance?

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The introduction of spinel phase to form the layered-spinel structure (LSS) is an effective way to improve the electrochemical performance of Li-and Mn-rich layered oxides (LMR).But is this structure universal for all LMR systems?In this work,different Mn/Ni ratio systems with the LSS are discussed in detail.It is found that,high discharge capacity (200.8 mA h g-1 at 1C rate;1C =250 mA h g-1) as well as high capacity-retention (94% at 1C rate after 100 cycles) can be achieved by forming the LSS for low-Ni system(Mn/Ni =5.0).However,the capacity retention decreases severely in the high-Ni system (Mn/Ni =3.5,2.6).For example,when the ratio of Mn/Ni is 3.5,the capacity-retention of the layered-spinel sample was only 65.8%,compared to the 83% of the original LMR sample.The Ex-situ XRD,XPS,and HRTEM results demonstrate that the introduction of spinel phase in high-Ni system accelerates the transition and collapse of the crystal structure.This work provides guidance for optimizing the proportions of ele-ments and the design of structures for the LMR.
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