Research progress of interface problems and optimization of garnet-type solid electrolyte

Zhang Nian; Ren Guo-Xi; Zhang Hui; Zhou Deng; Liu Xiao-Song

doi:10.7498/aps.69.20201533

Abstract

With the increasing demand for storage devices with higher energy output and better safety performance, all-solid-state batteries show their potential to replace the traditional liquid-based Li-ion batteries in the future storage market. Garnet-type Li₇La₃Zr₂O₁₂ is one of the most attractive solid electrolyte materials because of its high ionic conductivity and stability to lithium metal. However, the large interfacial resistance originating from the insufficient solid-solid contact and the penetration of the lithium dendrite due to the inhomogeneous dissolution and deposition of lithium, hinder the all-solid-state batteries from developing. Focusing on the main interfacial problems in garnet-type all-solid battery, this review provides a fundamental understanding of the Li₂CO₃ issues in Li₇La₃Zr₂O₁₂ solid electrolyte and addresses the key factors influencing Li/ Li₇La₃Zr₂O₁₂/cathode interfacial wettability and the growth of Li dendrite, thus giving the key factors of constructing ideal interfaces. Finally, the possible research direction of garnet-type all-solid-state battery in the future is also prospected, which provides a guidance for developing and using all-solid-state batteries.

Keywords:

Authors and contacts

1.
State Key Laboratory of Functional Materials for Informatics, Shanghai Institute of Microsystem and Information Technology, Chinese Academy of Sciences, Shanghai 200050, China
2.
Tianmu Lake Institute of Advanced Energy Storage Technologies, Liyang 213300, China
3.
School of Physical Science and Technology, Shanghai Tech University, Shanghai 201210, China

Corresponding author: Liu Xiao-Song, xliu3@mail.sim.ac.cn

Funds: Project supported by the National Natural Science Foundation of China (Grant Nos. 11905283, U1632269, 11227902) and the National Key R&D Program of China (Grant No. 2019YFA0405600)

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Cited By

图 1 (a) 熔融的金属锂在各种界面上的浸润角; (b) 计算得到的Li–Li₂CO₃和Li–LLZO界面的附着功(W_ad)、接触角(θ)以及原子结构^[32]

Figure 1. (a) The contact angle of molten metallic Li on different surfaces; (b) calculated work of adhesion (W_ad), contact angle (θ), and atomic structure for the Li–Li₂CO₃ and Li–LLZO interfaces^[32].

DownLoad: Full-Size Img PowerPoint

图 2 (a) 利用铂金坩埚代替传统Al₂O₃坩埚可以有效减少暴露空气后LLZO表面碳酸锂的形成^[34]; (b) 利用快速热脉冲的处理方法可以有效去除碳酸锂, 并且使得锂损失最小化^[48]; (c) 通过添加LiF, Li₃PO₄等疏水添加剂, 或者在表面制造缺锂层, 都可以有效抑制碳酸锂的形成^[33,51]; (d) 通过快速酸处理可以除去表面碳酸锂, 得到稳定接触的界面^[52]

Figure 2. (a) Using Pt crucible instead of alumina crucible can effectively reduce the Li₂CO₃formation on LLZO after exposed to air^[34]; (b) the rapid thermal pulsing treatment can effectively remove the Li₂CO₃ impurity and minimize Li loss^[48]; (c) adding inorganic additives such as LiF and Li₃PO₄, or creating Li-deficient compounds on the surface can eliminate Li₂CO₃ contaminants^[33,51]; (d) improving Li/LLZO interface contact by removing Li₂CO₃ via rapid acid treatment^[52].

DownLoad: Full-Size Img PowerPoint

图 3 (a) 利用Ge作为界面缓冲材料优化Li/LLZO界面^[5]; (b) 中子深度分析装置示意图及LLZO原位探测结果^[58]; (c) 利用MoS₂作为界面缓冲材料优化Li/LLZO界面, 和界面转化反应及极化原理示意图^[61]

Figure 3. (a) Using Ge as buffer layer to modify Li/LLZO interface^[5]; (b) schematic of the experimental set-up for operando Neutron depth profiling and the results for LLZO cell^[58]; (c) schematic diagram of the conversion reaction and the chemical evolution of the MoS₂-coating layer in the polarization process^[61].

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图 4 (a) 利用添加Nb缓冲层可以有效改善激光脉冲沉积过程中LiCoO₂/LLZO界面稳定性^[70]; (b) 利用快速热退火的方法将V₂O₅电极材料制备到LLZO片上^[72]; (c) 利用Li_2.3-_xC_0.7+_xB_0.3-_xO₃与碳酸锂反应生成LCBO改善LiCoO₂/LLZO界面示意图以及全固态电池在常温下的循环特性^[73]

Figure 4. (a) Using Nb as buffer layer can modify the stability of LiCoO₂/LLZO interface during Pulsed Laser Deposition (PLD) process^[70]; (b) using rapid thermal annealing to melt V₂O₅ cathode onto LLZO pellet^[72]; (c) schematics of the interphase-engineered all-ceramic cathode/electrolyte by using the reaction of Li_2.3-_xC_0.7+_xB_0.3-_xO₃ with Li₂CO₃. The all sold battery can cycle well over 100 times at room temperature^[73].

DownLoad: Full-Size Img PowerPoint

图 5 石榴石型全固态电池未来可能的研究方向^[63,78,82]

Figure 5. Possible research directions for garnet-based all solid battery in the future^[63,78,82].

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表 1 计算得到的在298.15 K下LLZO发生水合以及碳酸化反应所需的吉布斯自由能, 其中, 前4项是反应过程中有Li⁺/H⁺交换作用对应的能量, 后2项为直接反应对应的能量^[37]

Table 1. Calculated Gibbs free energy for the hydration and carbonation of LLZO at 298.15 K. The first 4 reactions involve Li⁺/H⁺ ion exchange and the last 2 reactions assume direct hydration and carbonation of LLZO^[37].

LLZO与空气中的水和二氧化碳可能的反应过程	吉布斯自由能 ΔG/kJ·mol^–1
Li₅₆La₂₄Zr₁₆O₉₆+H₂O(g) → Li₅₅HLa₂₄Zr₁₆O₉₆+LiOH	–33
LiOH+1/2 CO₂(g) → 1/2 Li₂CO₃+1/2 H₂O(g)	–33.6
Li₅₆La₂₄Zr₁₆O₉₆+CO₂(g) → Li₅₄La₂₄Zr₁₆O₉₅+Li₂CO₃	+21.5
Li₂O+CO₂(g)→Li₂CO₃	–147.6
Li₅₆La₂₄Zr₁₆O₉₆+H₂O(g) → Li₅₄La₂₄Zr₁₆O₉₅+2 LiOH	+82.8
Li₅₆La₂₄Zr₁₆O₉₆+CO₂(g) → Li₅₄La₂₄Zr₁₆O₉₅+Li₂CO₃	+15.6

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[12]	Chang H J, Ilott A J, Trease N M, Mohammadi M, Jerschow A, Grey C P 2015 J. Am. Chem. Soc. 137 15209 Google Scholar
[13]	Xu R C, Xia X H, Zhang S Z, Xie D, Wang X L, Tu J P 2018 Electrochim. Acta 284 177 Google Scholar
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[15]	Kobayashi T, Imade Y, Shishihara D, Homma K, Nagao M, Watanabe R, Yokoi T, Yamada A, Kanno R, Tatsumi T 2008 J. Power Sources 182 621 Google Scholar
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[18]	Bonanos N, Knight K, Ellis B 1995 Solid State Ionics 79 161 Google Scholar
[19]	Kanno R, Murayama M 2001 J. Electrochem. Soc. 148 A742 Google Scholar
[20]	Zhang Z, Zhang L, Liu Y, Yu C, Yan X, Xu B, Wang L M 2018 J. Alloys Compd. 747 227 Google Scholar
[21]	Senevirathne K, Day C S, Gross M D, Lachgar A, Holzwarth N 2013 Solid State Ionics 233 95 Google Scholar
[22]	Mizuno F, Hayashi A, Tadanaga K, Tatsumisago M 2005 Adv. Mater. 17 918 Google Scholar
[23]	Ferraresi G, El Kazzi M, Czornomaz L, Tsai C L, Uhlenbruck S, Villevieille C 2018 ACS Energy Lett. 3 1006 Google Scholar
[24]	Murugan R, Thangadurai V, Weppner W 2007 Angew. Chem. Int. Ed. Engl. 46 7778 Google Scholar
[25]	Awaka J, Kijima N, Hayakawa H, Akimoto J 2009 J. Solid State Chem. 182 2046 Google Scholar
[26]	Zhou W, Wang S, Li Y, Xin S, Manthiram A, Goodenough J B 2016 J. Am. Chem. Soc. 138 9385 Google Scholar
[27]	Haruyama J, Sodeyama K, Tateyama Y 2017 ACS Appl. Mater. Interfaces 9 286 Google Scholar
[28]	Han X, Gong Y, Fu K K, He X, Hitz G T, Dai J, Pearse A, Liu B, Wang H, Rubloff G, Mo Y, Thangadurai V, Wachsman E D, Hu L 2017 Nat. Mater. 16 572 Google Scholar
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[31]	Cheng L, Crumlin E J, Chen W, Qiao R, Hou H, Franz Lux S, Zorba V, Russo R, Kostecki R, Liu Z, Persson K, Yang W, Cabana J, Richardson T, Chen G, Doeff M 2014 Phys. Chem. Chem. Phys. 16 18294 Google Scholar
[32]	Sharafi A, Kazyak E, Davis A L, Yu S, Thompson T, Siegel D J, Dasgupta N P, Sakamoto J 2017 Chem. Mater. 29 7961 Google Scholar
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[35]	Wagner R, Rettenwander D, Redhammer G J, Tippelt G, Sabathi G, Musso M E, Stanje B, Wilkening M, Suard E, Amthauer G 2016 Inorg. Chem. 55 12211 Google Scholar
[36]	Cheng L, Wu C H, Jarry A, Chen W, Ye Y, Zhu J, Kostecki R, Persson K, Guo J, Salmeron M, Chen G, Doeff M 2015 ACS Appl. Mater. Interfaces 7 17649 Google Scholar
[37]	Sharafi A, Yu S, Naguib M, Lee M, Ma C, Meyer H M, Nanda J, Chi M, Siegel D J, Sakamoto J 2017 J. Mater. Chem. A 5 13475 Google Scholar
[38]	Ma C, Rangasamy E, Liang C, Sakamoto J, More K L, Chi M 2015 Angew. Chem. Int. Ed. Engl. 54 129 Google Scholar
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[40]	Truong L, Thangadurai V 2012 Inorg. Chem. 51 1222 Google Scholar
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[42]	Liu X, Chen Y, Hood Z D, Ma C, Yu S, Sharafi A, Wang H, An K, Sakamoto J, Siegel D J, Cheng Y, Jalarvo N H, Chi M 2019 Energy Environ. Sci. 12 945 Google Scholar
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