首页|Homogenous coating of Li+conductive Li5AlO4 on single-crystalline nonstoichiometric Li1.04Ni0.92Al0.04O2 for rechargeable lithium-ion batteries

Homogenous coating of Li+conductive Li5AlO4 on single-crystalline nonstoichiometric Li1.04Ni0.92Al0.04O2 for rechargeable lithium-ion batteries

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Cobalt-free,nickel-rich LiNi1-xAlxO2(x ≤ 0.1)is an attractive cathode material because of high energy den-sity and low cost but suffers from severe structural degradation and poor rate performance.In this study,we propose a molten salt-assisted synthesis in combination with a Li-refeeding induced aluminum seg-regation strategy to prepare Li5AlO4-coated single-crystalline slightly Li-rich Li1.04Ni0.92Al0.04O2.The sym-biotic formation of Li5AlO4 from reaction between molten lithium hydroxide and doped aluminum in the bulk ensures a high lattice matching between the Ni-rich oxide and the homogenous conductive Li5AlO4 that permits high Li+conductivity.Benefiting from mitigated undesirable side reactions and phase evo-lution,the Li5AlO4-coated single-crystalline Li1.04Ni0.92Al0.04O2 delivers a high specific capacity of 220.2 mA h g-1 at 0.1 C and considerable rate capability(182.5 mA h g-1 at 10 C).Besides,superior capac-ity retention of 90.8％is obtained at 1/3 C after 100 cycles in a 498.1 mA h pouch full cell.Furthermore,the particulate morphology of Li1.04Ni0.92Al0.04O2 remains intact after cycling at a cutoff voltage of 4.3 V,whereas slightly Li-deficient Li0.98Ni0.97Al0.05O2 features intragranular cracks and irreversible lattice dis-tortion.The results highlight the value of molten salt-assisted synthesis and Li-refeeding induced ele-mental segregation strategy to upgrade Ni-based layered oxide cathode materials for advanced Li-ion batteries.

Aluminum segregationSurface coatingNonstoichiometric oxidesMolten synthesisCathode materials

Guoyu Ding、Shizhou Wang、Jinhan Li、Ziyan Wu、Jiayu Chen、Jiayong Du、Xinhui Huang、Kuiming Liu、Yudong Zhang、Zhonghan Wu、Yiyang Peng、Qiancheng Zhao、Meng Yu、Fangyi Cheng

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Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education),Engineering Research Center of High-efficiency Energy Storage (Ministry of Education),College of Chemistry,Nankai University,Tianjin 300071,China

Key Laboratory of Advanced Energy Materials Chemistry(Ministry of Education),Engineering Research Center of High-efficiency Energy Storage(Ministry of Education),College of Chemistry,Nankai University,Tianjin 300071,China

State Key Laboratory of Advanced Chemical Power Sources,Nankai University,Tianjin 300071,China

Haihe Laboratory of Sustainable Chemical Transformations,Tianjin 300192,China

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China National Funds for Distinguished Young ScientistsNational Natural Science Foundation of ChinaJilin Scientific and Technological Development Program

219255032183500420220301018GX

2024

10.1016/j.jechem.2024.03.063

能源化学
中国科学院大连化学物理研究所 中国科学院成都有机化学研究所

能源化学

CSTPCDEI
影响因子：0.654
ISSN：2095-4956
年,卷(期)：2024.95(8)