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Modification strategies of Li7La3Zr2O12 ceramic electrolyte for high-performance solid-state batteries

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A Correction to this article was published on 21 August 2021

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Abstract

Enormous research focusing on solid-state electrolyte promotes the development of solid-state batteries. Compared to lithium-ion batteries using liquid electrolyte, the solid-state batteries feature the high energy density and non-flammability, which accelerates the revolution in portable electronics and transportation. Garnet-type Li7La3Zr2O12 (LLZO) solid-state electrolyte is considered as the promising solid-state electrolyte due to high ionic conductivity, Li transference number and shear modulus. However, surface contaminant and poor contact with lithium inhibit its practical application in lithium metal batteries. The review provides a brief introduction about structure and properties of LLZO. Then, we conclude the modification strategies for increasing ionic conductivity, enhancing interfacial contact and inhibiting lithium dendrite. At last, the challenge and perspectives are discussed for development of LLZO in solid-state batteries.

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Fig. 1

Reproduced with permission from Ref. [16] Copyright 2012 American Physical Society

Fig. 2

a, b Reproduced with permission from Ref. [27] Copyright 2015 ACS. c Schematic model which illustrates the Li2CO3 formation process. Reproduced with permission from Ref. [26] Copyright 2017 The American Ceramic Society

Fig. 3

Reproduced with permission from Ref. [32] Copyright 2020 Wiley

Fig. 4

Reproduced with permission from Ref. [33] Copyright 2020 Springer Nature

Fig. 5

Reproduced with permission from Ref. [44] Copyright 2016 ACS. The mechanism of MCI-coated LLZO pellet for suppressing lithium dendrites: b LLZO/Li and c LLZO/T–LLZO/Li. Reproduced with permission from Ref. [45] Copyright 2020 Wiley

Fig. 6

Reproduced with permission from Ref. [62]. Copyright 2017 Wiley. b Illustration for synthesis of Li3N-coated LLZTO, and the SEM images of Li2CO3-coated LLZTO and Li3N-coated LLZTO. Reproduced with permission from Ref. [63]. Copyright 2018 ACS. c The mechanism of Li3OCl for better contact between Li metal and LLZTO. Reproduced with permission from Ref. [64]. Copyright 2018 Elsevier. d Schematic illustration for poor contact between LLZTO and Li and the formation of LiySn and Li3N at the interface to realize intimate contact. Right: magnified area. Reproduced with permission from Ref. [65]. Copyright 2020 Wiley

Fig. 7

Reproduced with permission from Ref. [66] Copyright 2021 Springer Nature

Fig. 8

Reproduced with permission from Ref. [67] Copyright 2020 ACS. b Illustration for poor contact between SSE and Li metal and stable contact between Li–Mg alloy and SSE. Reproduced with permission from Ref. [61] Copyright 2018 Wiley. c Mechanism of the formation of Li3N interlayer by reaction between molten Li and g-C3N4. Reproduced with permission from Ref. [68] Copyright 2019 Wiley

Fig. 9

Reproduced with permission from Ref. [70] Copyright 2016 ACS. b Schematic illustrations for microcrack caused within LBO layer during batteries cycling and the SEM images of the microcrack. Reproduced with permission from Ref. [73] Copyright 2019 ACS. c Schematics of the Li2.3C0.7B0.3O3 as solder to realize intact contact between LCO powder and LLZO powder, and between cathode layer and LLZO pellet and cycling performance of Li/LLZO/LCO batteries at 0.05 C at room temperature. Reproduced with permission from Ref. [69] Copyright 2018 Elsevier

Fig. 10

a, b Reproduced with permission from Ref. [80] Copyright 2020 RSC. c Schematic of the consolidating mechanism. d Cycling performance of the NCM811/LFP cathode for more than 100 cycles at 0.2  C by LLZTO/LBO electrolyte. c, d Reproduced with permission from Ref. [81] Copyright 2019 RSC

Fig. 11

a, b Reproduced with permission from Ref. [89] Copyright 2020 Wiley. c Schematics of fabrication procedures of the presented LLZO thin films. d Illustration of the migration barrier and Li vacancy concentration at the conventional grain boundary and the grain boundary with amorphous domains. c, d Reproduced with permission from Ref. [90] Copyright 2020 Springer Nature

Fig. 12

a, b Reproduced with permission from Ref. [95] Copyright 2021 Wiley. c Photo showing the flexibility of the hybrid electrolyte, which is associated with the fiber network and conformal structure between ceramic fibers and a polymer electrolyte. Reproduced with permission from Ref. [97] Copyright 2018 Wiley

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Acknowledgements

This work was financially supported by the National Natural Science Foundation of China (Grant No. 51672156), Local Innovative Research Teams Project of Guangdong Pearl River Talents Program (Grant No. 2017BT01N111), Shenzhen Technical Plan Project (Grant Nos. JCYJ20170412170706047, JCYJ20170307153806471 and GJHS20170314165324888).

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  1. Jian-Shuai Lv and Shao-Ke Guo contributed equally to this paper.

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  1. Tsinghua Shenzhen International Graduate School, Tsinghua University, Shenzhen, 518055, China

    Jian-Shuai Lv, Shao-Ke Guo & Yan-Bing He

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  1. Jian-Shuai Lv
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Lv, JS., Guo, SK. & He, YB. Modification strategies of Li7La3Zr2O12 ceramic electrolyte for high-performance solid-state batteries. Tungsten 3, 260–278 (2021). https://doi.org/10.1007/s42864-021-00102-9

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