Constructing compatible interface between Li7La3Zr2O12 solid electrolyte and LiCoO2 cathode for stable cycling performances at 4.5 V

Yang, Dong; Su, Panzhe; He, Guanjie; Zhao, Huiling; Bai, Ying

doi:10.1039/d1nr01079d

Cited by 10 publications

(6 citation statements)

References 84 publications

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enable the use of Li metal anodes, [6][7][8][9][10] the research on Li/LLZO interface [11][12][13][14][15][16] and the compatibility of LLZO with current cathode chemistries [17][18][19][20][21] has progressed at an impressive pace. However, despite these stunning recent developments, the electrochemical performance and energy density of batteries based on LLZO SSE are far below the required levels.

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confidence: 99%

Intermediate‐Stage Sintered LLZO Scaffolds for Li‐Garnet Solid‐State Batteries

Okur

Zhang

Karabay

et al. 2023

Advanced Energy Materials

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While significant progress has been achieved in the field of Li‐garnet solid‐state batteries, their further development, is hindered by the formation of cavities at the Li7La3Zr2O12 (LLZO)/Li interface at practically relevant current densities and areal capacities exceeding 1 mA cm−2 and 1 mAh cm−2. As a result, the cells exhibit limited cycling stability due to the inhomogeneous distribution of the applied current density, and therefore, the formation of Li dendrites. Another aspect of high importance is associated with the development of the fabrication methodology of thin LLZO electrolytes for achieving the high energy density of Li‐garnet solid‐state batteries. To contribute to these two challenging problems, in this work, a facile intermediate‐stage sintering method of 50‐µm thin and porous LLZO membranes with a mean pore size of 2.5 µm is presented. The employment of such porous LLZO membranes not only provides an effective means of mitigating the formation of voids at the LLZO/Li interface due to the increased LLZO/Li surface area, but also maximizes achievable energy densities. It is demonstrated that fabricated porous LLZO membranes exhibit long cycling stability of over 1480 h at a current density of 0.5 mA cm−2.

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confidence: 99%

Intermediate‐Stage Sintered LLZO Scaffolds for Li‐Garnet Solid‐State Batteries

Okur

Zhang

Karabay

et al. 2023

Advanced Energy Materials

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“…Furthermore, as displayed in Figure 1e,f, the high‐resolution transmission electron microscopy (HR‐TEM) images show typical lattice spaces of 0.24 and 0.32 nm in the core and modified region originating from the LCO (101) and Pr 6 O 11 (111) planes. [ 35,36 ] Simultaneously, the XPS signals of Pr 3d for LCO and LCO@PrO‐1% samples compared in Figure , Supporting Information reveal the existence of Pr 6 O 11 in LCO@PrO material. As illustrated in Figure , Supporting Information, the element mapping further demonstrates that Pr element is evenly dispersed, also distinctly verifying that Pr 6 O 11 is successfully and uniformly coated on the surface of LiCoO 2 .…”

Section: Resultsmentioning

confidence: 87%

Easily Obtaining Excellent Performance High‐voltage LiCoO₂ via Pr₆O₁₁ Modification

Huang

Gao

et al. 2022

Energy & Environ Materials

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Up to now, LiCoO 2 (LCO) cathode material still occupies an important position in the consumer electronics market due to its ultra-high tap density and volumetric energy density. [1][2][3][4] It is reported that increasing the charging cutoff potential, usually larger than 4.4 V corresponding to more than removal amount of 0.6 Li + in LiCoO 2 , can effectively improve the energy density of the LCO. [5,6] However, it will also cause a sharp decline in the cycling performance originated from a series of phase transitions for high-voltage LiCoO 2 (H-LCO). [7][8][9] Herein, the release of surface oxygen and the loss of cobalt ions are other main reasons for the capacity attenuation of H-LCO. [10,11] Typically, in the low-voltage region, the LCO will undergo the insulator-to-metal phase transition, and the hexagonal structure H-1 phase will gradually transform into hexagonal structure H-2 phase. When the charging voltage reaches 4.2 V, the LCO material delivers a reversible transformation from O3 phase in the R-3m space group to monoclinic structure, and then back to O3 phase, which involves the "order ⇆ disorder" transformation of crystalline phase. In this process, the change in crystal parameters caused by the spatial mismatch between lithium ion and lithium vacancy will lead to the change in particle volume for LCO. Finally, another phase transformation of LiCoO 2 from O3 phase to H1-3 phase occurs when charging to above 4.5 V. In these reversible phase transitions, the transformation of "O3 phase ⇆ monoclinic structure" will significantly reduce the Li + diffusion kinetics, and during the further transformation of "O3 phase → H1-3 phase," severe mechanical stress and cracks will appear in the bulk material, accompanied by the decrease in Li + diffusion rate, which leads to the last rapid capacity fading. Thus, overcoming these obstacles is significant for the development of H-LCO materials.Generally, many strategies have been developed to overcome the cycling stability fading of H-LCO. On the one hand, foreign element doping in bulk phase has been demonstrated to be promising and effective for the improvement of H-LCO LIB performance, [12,13] which can inhibit the irreversible phase transformation, improve the stability of the phase structure, and alleviate the stress and deformation caused by the structural transformation during the charge/discharge process. For example, Zhao et al. found that Sn 4+ doping can inhibit the conversion of LCO to spinel phase under high potential due to the decrease in the

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“…[17][18][19][20] Therefore, the operation voltage of LiCoO 2 is limited to 4.2 V to mitigate the capacity decay. 21 In order to solve this problem, LiCoO 2 synthesized by traditional methods requires doping with Mg, [22][23][24] Zr, 24,25 Al, 17,26,27 Ni, 28 Fe, 29 Cr, 30 Mn, 31 and Ti, 32 and coating with MgO, 33 Al 2 O 3 , 34 and TiO 34 to inhibit orderdisorder phase transitions and improve structural stability. However, these modications require delicate control over synthetic parameters.…”

Section: Introductionmentioning

confidence: 99%

From metal to cathode material: in situ formation of LiCoO₂ with enhanced cycling performance and suppressed phase transition

et al. 2023

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Constructing compatible interface between Li₇La₃Zr₂O₁₂ solid electrolyte and LiCoO₂ cathode for stable cycling performances at 4.5 V

Abstract: With high theoretical capacity and tap density, LiCoO2 (LCO) cathode has been extensively utilized in lithium-ion batteries (LIBs) for energy storage devices. However, the bottleneck of structural and interfacial instabilities...

Cited by 10 publications

References 84 publications

Intermediate‐Stage Sintered LLZO Scaffolds for Li‐Garnet Solid‐State Batteries

Intermediate‐Stage Sintered LLZO Scaffolds for Li‐Garnet Solid‐State Batteries

Easily Obtaining Excellent Performance High‐voltage LiCoO₂ via Pr₆O₁₁ Modification

From metal to cathode material: in situ formation of LiCoO₂ with enhanced cycling performance and suppressed phase transition

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Constructing compatible interface between Li7La3Zr2O12 solid electrolyte and LiCoO2 cathode for stable cycling performances at 4.5 V

Abstract: With high theoretical capacity and tap density, LiCoO2 (LCO) cathode has been extensively utilized in lithium-ion batteries (LIBs) for energy storage devices. However, the bottleneck of structural and interfacial instabilities...

Cited by 10 publications

References 84 publications

Intermediate‐Stage Sintered LLZO Scaffolds for Li‐Garnet Solid‐State Batteries

Intermediate‐Stage Sintered LLZO Scaffolds for Li‐Garnet Solid‐State Batteries

Easily Obtaining Excellent Performance High‐voltage LiCoO2 via Pr6O11 Modification

From metal to cathode material: in situ formation of LiCoO2 with enhanced cycling performance and suppressed phase transition

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Constructing compatible interface between Li₇La₃Zr₂O₁₂ solid electrolyte and LiCoO₂ cathode for stable cycling performances at 4.5 V

Easily Obtaining Excellent Performance High‐voltage LiCoO₂ via Pr₆O₁₁ Modification

From metal to cathode material: in situ formation of LiCoO₂ with enhanced cycling performance and suppressed phase transition