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ACS Applied Materials & Interfaces · 2022 · IF 10.383

Li-Deficient Materials-Decoration Restrains Oxygen Evolution Achieving Excellent Cycling Stability of Li-Rich Mn-Based Cathode

Xueqian Ji,Yuxing Xu,Qing Xia,Yuncheng Zhou,Jiechen Song,Hailan Feng,Pengfei Wang,Jun Yang,Qiangqiang Tan

With the increasing demand for high energy density and rapid charging performance, Li-rich materials have been the up and coming cathodes for next-generation lithium-ion batteries. However, because of oxygen evolution and structural instability, the commercialization of Li-rich materials is extremely retarded by their poor electrochemical performances. In this work, Li-deficient materials Li0.3NbO2 and (Nb0.62Li0.15)TiO3 are applied to functionalize the surface of Li1.2Mn0.54Ni0.13Co0.13O2, aiming to suppress oxygen evolution and increase structural stability in LIBs. In addition, a fast Li-ion transport channel is beneficial to enhance Li+ diffusion kinetics. The results demonstrate that the electrodes decorated with Li0.3NbO2 and (Nb0.62Li0.15)TiO3 materials exhibit more stable cycling stability after long-term cycling and outstanding rate capability.

研究领域: 材料科学 · 电化学
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IONICS · 2019 ·Vol. 25 ·期 12 ·5681-5688 · IF 2.289

Adorned Li-rich Li1.2Ni0.13Co0.13Mn0.54O2 with LiAlO2 for improved electrochemical properties in lithium-ion batteries

Wang Li-Zhen,Yang Wei,Lv Teng-Fei,Gao Ke-Zheng,Yan Ji

In this paper, core-shell like LiAlO 2 -coated Li 1.2 Ni 0.13 Co 0.13 Mn 0.54 O 2 composite was synthesized by an improved solvothermal method. The surface of the material becomes rough after LiAlO 2 coating with a thickness of 5–10 nm. Meanwhile, the surface-coating component with the layer structure α-LiAlO 2 can change the dispersion of transition metal elements. When tested in 2.0–4.8 V at 0.05 °C, the initial discharge capacity of the LiAlO 2 -coated sample is 206.4 mAh g −1 with the columbic efficiency of 78.0%, which is higher than that of the pristine Li-rich Li 1.2 Ni 0.13 Co 0.13 Mn 0.54 O 2 sample. Further tested under 1 C rate, the coated sample possesses 151.4 mAh g −1 of specific capacity and maintains 149.0 mAh g −1 after 50 cycles with the capacity retention of 98.4%. The improved reversible capacity, rate capability, and cycling durability of the Li 1.2 Ni 0.13 Co 0.13 Mn 0.54 O 2 material are attributed to the synergistic effect of surface coating of highly Li-conductive LiAlO 2 and the fuzzy interface between LiAlO 2 and Li 1.2 Ni 0.13 Co 0.13 Mn 0.54 O 2 .

研究领域: 材料科学 · 能源存储
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ACS Applied Energy Materials · 2019 · IF 0

Novel Ordered Rocksalt-Type Lithium-Rich Li2Ru1–xNixO3−δ (0.3 ≤ x ≤ 0.5) Cathode Material with Tunable Anionic Redox Potential

Shiyao Zheng,Feng Zheng,Haodong Liu,Guiming Zhong,Jue Wu,Min Feng,Qihui Wu,Wenhua Zuo,Chaoyu Hong,Yan Chen,Ke An,Ping Liu,Shunqing Wu,Yong Yang

In this work, a series of ordered rocksalt (OR) type Li-rich Li2Ru1–xNixO3−δ (LRNxO, 0.3 ≤ x ≤ 0.5) are successfully synthesized and investigated for the first time. X-ray diffraction and neutron powder diffraction patterns exhibit an obvious phase transition from layered to an OR structure as the Ni content gradually increases from x = 0 to x = 0.5, which leads to different electrochemical behaviors. In the case of OR-LRN0.4O, an ∼350 mV decrease of the oxygen oxidation potential compared with Li2RuO3 (LRO) is observed from around 4.2 to 3.85 V, which is confirmed by both X-ray photelectron O 1s spectra and dQ/dV results. The role of Ni substitution on the oxygen redox reaction is studied by first-principles calculations, and it is concluded that the formation of the OR structure caused by Ni substitution is the main reason for lowering the oxygen oxidation potential. In addition, the average discharge voltage of OR-LRN0.4O is also enhanced compared with LRO. This work provides a novel innovative strategy to modulate and control the oxygen anion redox reaction for high-energy-density Li-rich materials, which shed light on the fundamental understanding and optimizing of the anion redox process in Li-rich materials.

研究领域: 材料科学 · 电化学
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JOURNAL OF POWER SOURCES · 2025 · IF 7.9

An integrated strategy of surface coating and dual-element doping to enhance electrochemical performances of Li-rich layered oxide for lithium-ion batteries

Zhenbo Wang,Xiaoyan Guo,Guowei Zhang,Lu Sai,Hongzhe Wang,Ying Bai,Huiling Zhao

Li-rich oxides are one kind of promising cathodes for the advanced lithium-ion batteries owing to ultrahigh specific discharge capacity and low cost. Whereas, their high energy density stemmed from oxygen anion redox easily triggers irreversible phase transition and oxygen release, simultaneously companied with low initial Coulombic efficiency, rapid capacity degradation and poor cycling stability. Herein, an integrated strategy of Li 0.35 La 0.55 TiO 3 (LLTO) coating and Ti 4+ /La 3+ dual-element doping is introduced to improve the electrochemical performances of Li 1.2 Mn 0.56 Ni 0.17 Co 0.07 O 2 (LMNCO) via facile sol-gel method and annealing treatment. Various characterizations including in-situ XRD and DEMS demonstrate that LLTO coating can accelerate Li + diffusion and alleviate side reactions at cathode-electrolyte interface, meanwhile Ti 4+ /La 3+ -doping can stabilize lattice oxygen and restrain oxygen release in the charge-discharge process. Electrochemical test results manifest that the LLTO-modified LMNCO cathode exhibits excellent rate property and long-term cycling stability, e.g. , a discharge capacity of 153.6 mAh g −1  at 5C, and a superior capacity retention of 83 % after 400 cycles at 1C. This work presents one simple strategy for the modification of Li-rich material to rationally utilize TM cationic and oxygen anionic redox reactions, and to promote the electrochemical performance and structure stability of layered-structure cathode in long-term cycling even under elevated temperature.

研究领域: 材料科学 · 电化学
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JOURNAL OF MATERIALS SCIENCE · 2023 ·Vol. 58 ·期 36 ·14440-14451 · IF 4.5

Effect of surface structure on electrochemical properties in Li1.2Ni0.2Ti0.6O2 cathode material

Zhou Yuncheng,Xu Yuxing,Feng Hailan,Song Jiechen,Yan Mengxiao,Jian Haoyu,Zhuge Fuchang,Tan Qiangqiang

The Li-excess disordered rock salt cathode material, Li 1.2 Ni 0.2 Ti 0.6 O 2 , was synthesized via the sol–gel method to investigate the impact of different sintering temperatures on its structure, morphology, and electrochemical performance. X-ray diffraction (XRD) analysis revealed a cubic rock salt structure for the material. Raman spectroscopy indicated the presence of short-range-ordered domains of Li 2 TiO 3 and LiNiO 2 in the samples. The XPS results confirmed the existence of an oxygen vacancy structure on the sample’s surface. Morphological observations demonstrated that micron-scale secondary particles agglomerated with nanoscale primary particles, resulting in a nano-microstructure formation. Electrochemical testing conducted at room temperature within a voltage range of 1.5 ~ 4.8 V showed that the sample sintered at 600 °C exhibited the highest specific discharge capacity of approximately 304.4 mAh g −1 at 20 mA g −1 . The influence of surface structure on electrochemical properties in disordered rock salt cathode materials is elucidated through interactions between small primary particles and surface oxygen vacancies.

研究领域: 材料科学 · 电化学 · 无机化学 · 能源存储 · 固体化学
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ELECTROCHIMICA ACTA · 2022 · IF 7.336

Suppressing oxygen vacancies on the surface of Li-rich material as a high-energy cathode via high oxygen affinity Ca0.95Bi0.05MnO3 coating

Xueqian Ji,Yuxing Xu,Yuncheng Zhou,Jiechen Song,Hailan Feng,Pengfei Wang,Jun Yang,Fuchang Zhuge,Haijiao Xie,Qiangqiang Tan

Because of high energy density and work voltage, the Li-rich materials are considered to be one of the most promising next-generation lithium-ion batteries. However, the commercial applications are limited by the capacity loss, poor rate capability, and voltage decay during cycling. Herein, functionalizing the surface of Li 1.2 Mn 0.54 Ni 0.13 Co 0.13 O 2 by Ca 0.95 Bi 0.05 MnO 3 is proposed, which suppresses the formation of the oxygen vacancies and maintains structural stability by high oxygen affinity and alleviative electrolyte corrosion. Electrochemical tests demonstrate that this admirable electrode delivers excellent cycling stability. The Li-rich electrode decorated with 5 wt.% Ca 0.95 Bi 0.05 MnO 3 exhibits a stable capacity retention of 86.5% at 0.1C after 200 cycles and an excellent full cell performance with the energy retention of 95.4% at 0.1C after 100 cycles. Moreover, the voltage decay of the modified material is restrained from 5.02 to 3.07 mV per cycle over 200 cycles. The finding here sheds new light on the development of the better Li-rich cathodes for improving electrochemical performance of electrode materials.

研究领域: 材料科学 · 电化学 · 能源存储 · 锂离子电池 · 功能材料 · 固态化学 · 电极工程
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