Research Progress of Rare Earth Bromides Based Solid Electrolytes for All⁃Solid⁃State Batteries

doi:10.19894/j.issn.1000-0518.210448

Chinese Journal of Applied Chemistry ›› 2022, Vol. 39 ›› Issue (4): 585-598.DOI: 10.19894/j.issn.1000-0518.210448

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Research Progress of Rare Earth Bromides Based Solid Electrolytes for All⁃Solid⁃State Batteries

Qi ZHANG¹, Qian ZHANG¹(), Xiao-Meng SHI², Ya-Qi KONG¹, Ke-Xin GAO¹, Ya-Ping DU²()

^1.State Key Laboratory of Eco-Hydraulics in Northwest Arid Region，Department of Applied Chemistry，Xi'an University of Technology，Xi'an 710048，China
^2.Tianjin Key Lab for Rare Earth Materials and Applications，Center for Rare Earth and Inorganic Functional Materials，School of Materials Science and Engineering & National Institute for Advanced Materials，Nankai University，Tianjin 300350，China

Received:2021-09-01 Accepted:2021-11-22 Published:2022-04-01 Online:2022-04-19
Contact: Qian ZHANG,Ya-Ping DU
Supported by:
the “Water Saving and Reuse Innovation Team” Program of State Key Laboratory of Eco?Hydraulics in Northwest Arid Region(2019KJCXTD?8);from the National Natural Science Foundation of China(21971117);Functional Research Funds for the Central Universities, Nankai University(63186005);Tianjin Key Lab for Rare Earth Materials and Applications(ZB19500202);the Open Funds of the State Key Laboratory of Rare Earth Resource Utilization(RERU2019001);111 Project from China(B18030);Beijing?Tianjin?Hebei Collaborative Innovation Project(19YFSLQY00030);the Outstanding Youth Project of Tianjin Natural Science Foundation(20JCJQJC00130);the Key Project of Tianjin Natural Science Foundation(20JCZDJC00650)

Abstract

Abstract:

All-solid-state lithium-ion batteries possess excellent safety performance and high energy density， and are expected to be the next generation energy storage devices to replace traditional liquid batteries. Solid-state electrolytes are definitely the key materials to achieve the real all-solid-state batteries. In recent years， considerable progress has been made in halide electrolytes， especially rare earth-containing bromide based solid electrolytes （RE-BSEs）， which show good ionic conductivities （up to mS/cm order of magnitude）， electrochemical stability （1.5~3.4 V vs.Li⁺/Li） and so on. In this article， we review the research advances focusing on the possible applications and technical bottlenecks of RE-BSEs. Hopefully， it may be enlightening and spark some inspirations in terms of synthetic strategies， lithium ion transportation mechanism， and investigating methodologies in the study of RE-BSEs. Rare earth is one of the most important strategic resources of China and even for the world. The research and important achievements made on RE-BSEs show the high value potentials of rare earth elements， especially in fields of solid ionics and energy saving and conversions. It is of great significance for structural adjustment of energy economics， and will contribute to the emission peak and carbon neutrality.

Key words: Rare earth, Bromide, Solid electrolyte, All solid state battery

CLC Number:

O611.6

Qi ZHANG, Qian ZHANG, Xiao-Meng SHI, Ya-Qi KONG, Ke-Xin GAO, Ya-Ping DU. Research Progress of Rare Earth Bromides Based Solid Electrolytes for All⁃Solid⁃State Batteries[J]. Chinese Journal of Applied Chemistry, 2022, 39(4): 585-598.

Figures/Tables 7

Fig.1 A brief chronology of the development of RE-BSEs （modified according to reference ［16］）

Fig.2 （a） The Nyquist plots of the EIS measurement results of LYC and LYB. （b） Arrhenius conductivity plots of LYC and LYB. （c） Initial charge/discharge curves of all-solid-state cells （LYC， LYC/LYB， Li2S-P2S5 （LPS））. （d） The discharge capacity retention and coulombic efficiency of the LYC-cell and the LYC/LYB-cell for 100 cycles［35］

Fig. 3 （a， b） Proposed Li+ diffusion pathways along different orientations of LYBC-HP. （c） Arrhenius plots of conductivities of LYBC-BM samples. （d） LYBC-BM after hot-pressed at 170 ℃， 294 MPa. SEM images of （e） cold-pressed LYBC-BM and （f） hot-pressed LYBC-HP［43］

Fig. 4 Electrochemical performance of LCO/LYBC/In-Li battery（a） Charge-discharge curves at 0.1 C. （b） Cycling performance at 0.1 C. （c） Discharge curves at different rates. （d） Rate performances of ASSB cells with LYBC and LYC， respectively［43］

Fig. 5 The XRD Rietveld refinement results of （a） hc-LYC and （b） hc-LYB. （c，d） The crystal structures of LYC and LYB obtained from Rietveld refinement， superimposed with a calculated BVSE-based lithium-ion potential map. The yellow surface represents the ionic conduction path， and the regions enclosed with red surfaces represent the stable lithium-ion positions［35］

Fig.6 （a-d） DSC characterization of LYB and LYC in argon and oxygen. （e） DSC characterization of sulfide electrolyte in oxygen［35］

Fig. 7 Li-ion conductivities versus Li octahedral occupancy in （a） Li x M2/3Cl4，（b） Li x M1/2Cl4 and （c） Li x MCl4. （d） Li-ion conductivities as a function of M cation concentration y in hypothetical Li-ion conductors Li x M y Cl4， M = Sc3+， Zr4+， and Hf4+ at 600 K， substituted with reduced M cation concentration from original Li2MgCl4 materials. （e） Li-ion conductivities at 600 K of original Li2MgCl4， hypothetical Li-ion conductors derived from Li2MgCl4 with reduced cation concentrations， and original Li3MCl6 materials， along with their crystal structures （right） and （f-h） radial distribution function （RDF） g（r） of M cations［59］

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Research Progress of Rare Earth Bromides Based Solid Electrolytes for All⁃Solid⁃State Batteries

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