Research advance of lithium-rich cathode materials in all-solid-state lithium batteries

Yang Yuan; Hu Nai-Fang; Jin Yong-Cheng; Ma Jun; Cui Guang-Lei

doi:10.7498/aps.72.20230258

Abstract

The development of all-solid-state lithium batteries with high energy density, long cycle life, low cost and high safety is one of the important directions for the developing next-generation lithium-ion batteries. Lithium-rich cathode materials have been widely used in liquid lithium batteries for their higher discharge specific capacity (> 250 mAh/g) and energy density (> 900 Wh/kg), high thermal stability and low raw material cost. With the rapid development of high-performance lithium-rich cathode materials and solid-state electrolytes in all-solid-state lithium batteries, the application of lithium-rich cathode materials in all-solid-state lithium batteries is expected to make a breakthrough toward the target of 500 Wh/kg energy density of lithium-ion batteries. In this review, first, we elaborate the failure mechanism of lithium-rich cathode materials in all-solid-state lithium batteries. The poor electronic conductivity, irreversible redox reaction of anionic oxygen and structute transformation during the electrochemical cycling of lithium-rich cathode materials result in the low initial coulomb efficiency, poor cycling stability and voltage decay. In addition, the high operating voltage of lithium-rich cathode materials (> 4.5 V vs. Li/Li⁺) triggers off not only the conventional interfacial chemical reactions between anode and electrolyte, but also the release of oxygen, aggravating the interfacial electrochemical reactions, which reduces the stability of the cathode/electrolyte interface. Therefore, the intrinsic characteristics of lithium-rich cathode materials and the severe interfacial reaction of lithium-rich cathode/electrolyte greatly limit the application of lithium-rich cathode materials in all-solid-state lithium batteries. Then, we review the research progress of lithium-rich cathode materials in various solid-state electrolyte systems in recent years. The higher room temperature ionic conductivity and wider voltage window of inorganic solid-state electrolytes provide opportunities for the application of lithium-rich cathode materials in all-solid-state lithium batteries. At present, the application of lithium-rich cathode materials in all-solid-state lithium batteries is explored on the basis of sulfide, halide and oxide solid-state electrolyte systems, and important progress has been made in the studies of composite cathode preparation methods, interfacial reaction mechanisms and activation mechanisms. Finally, we summarize the current research hotspot of lithium-rich cathode all-solid-state lithium batteries and propose several strategies for their future studies, such as the regulation of cathode material components, the construction of lithium ion and electron transport pathways within the composite cathode, and the interfacial modification of cathode materials that have been shown to have significant effects in solving the failure problem.

Keywords:

Authors and contacts

1.
Institute of Materials Science and Engineering, Ocean University of China, Qingdao 266100, China
2.
Qingdao Industrial Energy Storage Research Institute, Qingdao Institute of Bioenergy and Bioprocess Technology, Chinese Academy of Sciences, Qingdao 266101, China

Corresponding author: Jin Yong-Cheng, jinyongcheng@ouc.edu.cn ; Ma Jun, majun@qibebt.ac.cn ; Cui Guang-Lei, cuigl@qibebt.ac.cn

Funds: Project supported by the National Natural Science Foundation of China (Grant Nos. 52172245, 21975274), the Natural Science Foundation of Shandong Province, China (Grant Nos. ZR2020KE032, ZR2022QB166), and the Foundation of Postdoctoral Application Program of Qingdao, China (Grant No. Y63302190F).

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References

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图 1 富锂正极材料在全固态锂电池中的发展历史概览^[18-30]

Figure 1. Development history of lithium-rich cathodes in all-solid-state lithium batteries^[18-30].

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图 2 富锂固态复合正极界面电子和离子迁移的示意图^[21]　(a) 传统的无碳富锂固态复合正极; (b) 含碳富锂固态复合正极; (c) 具有改性富锂正极的含碳固态复合电极

Figure 2. Schematic illustrations of the electronic and ionic migration at the interface of Li-rich composite cathode^[21]: (a) Conventional carbon-free Li-rich solid-state composite cathode; (b) carbon-containing Li-rich solid-state composite cathode; (c) carbon-containing solid-state composite cathode with modified Li-rich cathode materials.

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图 3 富锂硫化物全固态锂电池　(a) 原始和第11次充电状态下LRO的O-K mRIXs图谱(红色箭头和黄色圆圈表示阴离子氧氧化还原的特征), 在531 eV激发能量下提取的LRO在完全充电状态和相应放电状态(浅灰色图)下的RIXs图谱(红色箭头和蓝色线圈中的强度对应于在充电状态下由氧氧化还原反应触发的氧化氧)^[18]; (b) LRCox和LRCo10@yLN正极的电子电导率, 离子电导率和C2/m相含量^[20]; (c)(LPSCl+VGCF)|LPSCl|Li-In电池在2.0—4.8 V(vs. Li/Li⁺), 0.1 mV/s下初始4个循环期间的CV曲线; (d) Pt|LLO|LPSCl|Pt的原位加电装置图和原位电荷密度分布^[19]

Figure 3. Lithium-rich cathode sulfide ASSLB: (a) O-K mRIXS of LRO at the pristine and upon 11^th charge states (the red arrows and the yellow circle indicated the features of anionic oxygen redox), and RIXs spectra extracted at 531 eV excitation energy of LRO in the fully charged states and corresponding discharges states (light gray plot) (the intensity in the red arrow and the blue coil corresponds to the oxidized oxygen triggered by oxygen redox reaction at the charged state)^[18]; (b) electronic conductivity, ionic conductivity and C2/m phase content of LRCox and LRCo10@yLN cathodes^[20]; (c) CV curves of the (LPSCl+VGCF)|LPSCl|Li-In cell during the initial four cycles between 2.0 and 4.8 V vs. Li/Li⁺ at 0.1 mV/s; (d) in-situ power-up installation diagram and in-situ charge-density-distribution characterization of Pt|LLO|LPSCl|Pt^[19].

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图 4 富锂卤化物全固态锂电池　(a) 由碳添加剂和LPO包覆的LLO组成全固态锂电池示意图^[21]; (b) 采用LNO离子导电涂层材料对LRM进行表面化学修饰^[23]; (c) 通过S—O键以稳定LRMO/SE界面^[22]

Figure 4. Lithium-rich cathode halide ASSLB: (a) Schematic illustration of ASSLB consisting of carbon additives and coated-LPO LLO^[21]; (b) surface chemistry modification of LRM with an ionic conductive coating material of LNO^[23]; (c) stabilization of LRMO/SE interface by S—O bonding^[22].

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图 5 富锂氧化物全固态锂电池　(a) 第一次充放电期间Li_1+x+yAl_x(Ti, Ge)_2–xSi_yP_3–yO₁₂(LASGTP)基板上Li₂MnO₃原位HAXPES光谱的O 1s和Mn 3s峰值偏移^[26]; (b) 原位实验装置示意图和脱锂前后LNMO颗粒的HAADF-STEM图像^[27]; (c) 单晶富锂石榴石型氧化物全固态锂电池的结构示意图及其在0.05 C和80 °C条件下的初始充放电曲线以及相应的dQ/dV曲线^[28]

Figure 5. Lithium-rich cathode oxide ASSLB: (a) O 1s and Mn 3s peak shifts in the in situ hard X-ray photoelectron spectroscopy (HAXPES) spectra of Li₂MnO₃ on Li_1+x+yAl_x(Ti, Ge)_2–xSi_yP_3–yO₁₂ (LASGTP) substrates during the first charge/discharge^[26]; (b) schematic of the in situ experimental setup and HAADF-STEM images of other LNMO particle before and after delithiation^[27]; (c) structural schematic of a single-crystal lithium garnet-rich oxide all-solid-state lithium battery and its initial charge/discharge curves at 0.05 C, 80 ℃ and the corresponding dQ/dV curves ^[28].

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表 1 典型的富锂全固态锂电池电化学性能

Table 1. Representative of reported lithium-rich cathode all-solid-state lithium batteries.

类型	电池结构	测试条件	放电比容量/ (mAh·g^–1)	容量保持率	文献
硫化物	Li₂RuO₃-Li₆PS₅Cl-AB\| Li₇P₃S₁₁\| Li-In	60 ℃, 2.0—4.3 V (1 C = 200 mA/g)	220, 0.1 C 210, 1 C (after 10 activation cycles, 0.05 C)	90%–1 C, 1000 cycles	[18]
	Li_1.2Ni_0.13Co_0.13Mn_0.54O₂- Li₆PS₅Cl- conductive\| Li₆PS₅Cl\| Li-In	30 ℃, 2.0—4.7 V (1 C = 250 mA/g)	110.4, 0.1 C	—	[19]
	Li₆PS₅Cl\|LiNbO₃-coated Li_1.18Ni_0.21Co_0.15Mn_0.45O₂-Li₆PS₅Cl-VGCF\| Li₆PS₅Cl \| Li-In	27 ℃, 2.0—4.8 V (1 C = 200 mA/g)	~170, 0.1 C ~160, 0.5 C	83%–0.5 C, 1000 cycles	[20]
卤化物	Li₂SO₃-coated Li_1.2Mn_0.54Co_0.13Ni_0.13O₂-Li₃InCl_4.8F_1.2 -CN\|Li₃InCl_4.8F_1.2- Li₆PS₅Cl\|Li-In	30 ℃, 2.3—4.6 V (1 C = 200 mA/g)	248, 0.1 C 130, 1 C	81.2%–1 C, 300 cycles	[22]
	Li₃PO₄-coated Li_1.17Mn_0.55Ni_0.24Co_0.05O₂-Li₃InCl₆-AB\|Li₃InCl₆- Li₆PS₅Cl\|In	25 ℃, 2.0—4.8 V (1 C = 200 mA/g)	230.7, 0.1 C ~200, 0.2 C	87.9%–0.2 C, 100 cycles	[21]
	LiNbO₃-coated Li_1.15Mn_0.53Ni_0.265Co_0.055O₂-Li₃InCl₆\|Li₃InCl₆\|Li-In	25 ℃, 2—4.8 V (1 C = 200 mA/g)	221, 0.1 C	49%–0.1 C, 100 cycles	[23]
氧化物	Li₂RuO₃\|Li₃PO₄\|Li	30 ℃, 3—4.0 V (0.1 C=1.67 mA/cm²)	101.4, 0.1 C	99%–0.1 C, 30 cycles	[24]
	Li₂MnO₃\|Li₃PO₄\|Li	30 ℃, 2—4.8 V (0.2 C =1.17 µA/cm²)	180, 0.2 C	99%–0.2 C, 100 cycles	[25]
	Li_1.2Mn_0.567Ni_0.167Co_0.067O₂-Ta-doped Li₇La₃Zr₂O₁₂-Li₃BO₃\|Ta-doped Li₇La₃Zr₂O₁₂\|Li	80 ℃, 2—4.7 V (1 C = 200 mA/g)	226, 0.05 C	80%–0.05 C, 30 cycles	[28]

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[1]	Li M, Lu J, Chen Z W, Amine K 2017 Adv. Mater. 30 1063 Google Scholar
[2]	Manthiram A 2017 ACS Cent. Sci. 3 1063 Google Scholar
[3]	Tarascon J M, Armand M 2001 Nature 414 359 Google Scholar
[4]	Tan S J, Wang W P, Tian Y F, Xin S, Guo Y G 2021 Adv. Funct. Mater. 31 2105253 Google Scholar
[5]	Chen J, Wu J W, Wang X D, Zhou A A, Yang Z L 2021 Energy Stor. Mater. 35 70 Google Scholar
[6]	Chen L K, Huang Y F, Ma J B, Ling H J, Kang F Y, He Y B 2020 Energy Fuels 34 13456 Google Scholar
[7]	Xu J J, Cai X Y, Cai S M, Shao Y X, Hu C, Lu S R, Ding S J 2022 Energy Environ. Mater. 0 e12450 Google Scholar
[8]	Li W D, Song B H, Manthiram A 2017 Chem. Soc. Rev. 46 3006 Google Scholar
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[12]	Hodeau J L, Marezio M, Santoro A, Roth R S 1982 J. Solid State Chem. 45 170 Google Scholar
[13]	Pearce P E, Perez A J, Rousse G, Saubanere M, Batuk D, Foix D, McCalla E, Abakumov A M, Van Tendeloo G, Doublet M L, Tarascon J M 2017 Nat. Mater. 16 580 Google Scholar
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[18]	Wu Y Q, Zhou K, Ren F C, Ha Y, Liang Z T, Zheng X F, Wang Z Y, Yang W, Zhang M J, Luo M Z, Battaglia C, Yang W L, Zhu L Y, Gong Z L, Yang Y 2022 Energy Environ. Sci. 15 3470 Google Scholar
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[22]	Sun S, Zhao C Z, Yuan H, Fu Z H, Chen X, Lu Y, Li Y F, Hu J K, Dong J, Huang J Q, Ouyang M, Zhang Q 2022 Sci. Adv. 8 eadd5189 Google Scholar
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[25]	Sugawara Y, Taminato S, Hirayama T, Hirayama M, Kanno R, Ukyo Y, Ikuhara Y 2018 J. Electrochem. Soc. 165 A55 Google Scholar
[26]	Hikima K, Shimizu K, Kiuchi H, Hinuma Y, Suzuki K, Hirayama M, Matsubara E, Kanno R 2022 J. Am. Chem. Soc. 144 236 Google Scholar
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[31]	Gao M X, Yan C H, Shao Q N, Chen J, Zhang C Y, Chen G R, Jiang Y Z, Zhu T J, Sun W P, Liu Y F, Gao M X, Pan H G 2021 Small 17 2008132 Google Scholar
[32]	Xue J P, Jiang C H, Pan B X, Zou Z M 2019 J. Electroanal. Chem. 850 113419 Google Scholar
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