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structural self-reconstruction strategy empowering Ni-rich layered cathodes with low-strain for superior cyclabilities

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Nano Research 2023年第4期16卷 4950-4960页

作者： Zhouliang Tan Yunjiao Li Xiaoming Xi Shijie Jiang Xiaohui Li Xingjie Shen Panpan Zhang Zhenjiang He School of Metallurgy and Environment Central South UniversityChangsha 410083China Engineering Research Center of the Ministry of Education for Advanced Battery Materials Central South UniversityChangsha 410083China Changsha Research Institute of Mining and Metallurgy Changsha 410083China Office of Laboratory and Equipment Management Xinjiang UniversityUrumqi 830000China

The key to hindering the commercial application of Ni-rich layered cathode is its severe structural and interface degradation during the undesired phase transition(hexagonal to hexagonal(H2→H3)),degenerating from the build-up of mechanical strain and undesired parasitic ***,a perovskite Li_(0.35)La_(0.55)TiO_(3)(LLTO)layer is built onto Ni-rich cathodes crystal to induce layered@spinel@perovskite heterostructure to solve the root cause of capacity *** exploration based on structure characterizations,in situ X-ray diffraction techniques,and first-principles calculations demonstrate that such a unique heterostructure not only can improve the ability of the host structure to withstand the mechanical strain but also provides fast diffusion channels for lithium ions as well as provides a protective barrier against electrolyte ***,the LLTO modified LiNi_(0.9)Co_(0.05)Mn_(0.05)O_(2)cathode manifests an unexpected cyclability with an extremely high-capacity retention of≈94.6%after 100 cycles,which is superior to the pristine LiNi_(0.9)Co_(0.05)Mn_(0.05)O_(2)(79.8%).Furthermore,this modified electrode also shows significantly enhanced cycling stability even withstanding a high cut-off voltage of 4.6 *** surface self-reconstruction strategy provides deep insight into the structure/interface engineering to synergistically stabilize structure stability and regulate the physicochemical properties of Ni-rich cathodes,which will also unlock a new perspective of surface interface engineering for layered cathode materials.

关键词： Ni-rich layered oxides cathode structural self-reconstruction phase transition mechanical strain first-principal calculation

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