Abstract
By modifying the preparation process of Pechini method, we can improve the structure of Li0.33La0.55TiO3 (LLTO) crystalline powder, so as to obtain high-density LLTO solid electrolyte. Through optimizing the sintering process, LLTO powder with good dispersion and uniform particle size was calcined at 800 °C; afterwards, the LLTO solid electrolyte samples with excellent properties were prepared by sintering at 1250 °C. The LLTO samples showed a low activation energy of 0.32 eV, a high relative density of 91.2%, and a high ionic conductivity of 2.7 × 10−5 S/cm. By adding three different aluminum salts, the ionic conductivity of Al3+-doped LLTO (A-LLTO) was further improved significantly. Especially in this case, with 30-nm Al2O3 doped, the conductivity of A-LLTO was increased to 4.7 × 10−5 S/cm, the activation energy was reduced to 0.30 eV, and the relative density was increased to 92.8%.
Similar content being viewed by others
References
Sun C, Liu J, Gong Y, Wilkinson DP, Zhang J (2017) Recent advances in all-solid-state rechargeable lithium batteries. Nano Energy 33:363. https://doi.org/10.1016/j.nanoen.2017.01.028
Mao W, Ai G, Dai Y et al (2016) In-situ synthesis of MnO2@CNT microsphere composites with enhanced electrochemical performances for lithium-ion batteries. J Power Sources 310:54. https://doi.org/10.1016/j.jpowsour.2016.02.002
Tang H, Zho Y, Zan L, Zhao N, Tang Z (2016) Long cycle life of carbon coated lithium zinc titanate using copper as conductive additive for lithium ion batteries. Electrochim Acta 191:887. https://doi.org/10.1016/j.electacta.2016.01.141
Xie J, Zhang Q (2016) Recent progress in rechargeable lithium batteries with organic materials as promising electrodes. Journal of Materials Chemistry A 4:7091. https://doi.org/10.1039/c6ta01069e
Wang H-G, Yuan S, Ma D-L, Zhang X-B, Yan J-M (2015) Electrospun materials for lithium and sodium rechargeable batteries: from structure evolution to electrochemical performance. Energy Environ Sci 8:1660. https://doi.org/10.1039/c4ee03912b
Ulissi U, Agostini M, Ito S, Aihara Y, Hassoun J (2016) All solid-state battery using layered oxide cathode, lithium-carbon composite anode and thio-LISICON electrolyte. Solid State Ionics 296:13. https://doi.org/10.1016/j.ssi.2016.08.014
Hayashi A, Nishio Y, Kitaura H, Tatsumisago M (2008) Novel technique to form electrode-electrolyte nanointerface in all-solid-state rechargeable lithium batteries. Electrochem Commun 10:1860. https://doi.org/10.1016/j.elecom.2008.09.026
Li J, Daniel C, Wood D (2011) Materials processing for lithium-ion batteries. J Power Sources 196:2452. https://doi.org/10.1016/j.jpowsour.2010.11.001
Ritchie A, Howard W (2006) Recent developments and likely advances in lithium-ion batteries. J Power Sources 162:809. https://doi.org/10.1016/j.jpowsour.2005.07.014
AKM Ahasan Habib, SMA Motakabber, MI Ibrahimy (2019) A comparative study of electrochemical battery for electric vehicles applications. https://doi.org/10.1109/PEEIACON48840.2019.9071955
Gong Y, Zhang J, Jiang L et al (2017) In situ atomic-scale observation of electrochemical delithiation induced structure evolution of LiCoO2 cathode in a working all-solid-state battery. J Am Chem Soc 139:4274. https://doi.org/10.1021/jacs.6b13344
L Wang, J Su, S Liu, et al. (2018) Interfacial issues of all solid state lithium batteries. Transactions of Nanjing University of Aeronautics & Astronautics 35: 578. https://doi.org/10.16356/j.1005-1120.2018.04.578
Wang C, Yang Y, Liu X et al (2017) Suppression of lithium dendrite formation by using LAGP-PEO (LiTFSI) composite solid electrolyte and lithium metal anode modified by PEO (LiTFSI) in all-solid-state lithium batteries. ACS Appl Mater Interfaces 9:13694. https://doi.org/10.1021/acsami.7b00336
Adachi GY, Imanaka N, Tamura S (2002) Ionic conducting lanthanide oxides. Chem Rev 102:2405. https://doi.org/10.1021/cr0103064
Gao X, Fisher CAJ, Kimura T et al (2014) Domain boundary structures in lanthanum lithium titanates. Journal of Materials Chemistry A 2:843. https://doi.org/10.1039/c3ta13726k
Moriwake H, Gao X, Kuwabara A et al (2015) Domain boundaries and their influence on Li migration in solid-state electrolyte (La, Li)TiO3. J Power Sources 276:203. https://doi.org/10.1016/j.jpowsour.2014.11.139
Gao X, Fisher CAJ, Kimura T et al (2013) Lithium atom and A-site vacancy distributions in lanthanum lithium titanate. Chem Mater 25:1607. https://doi.org/10.1021/cm3041357
T Teranishi, Y Ishii, H Hayashi, A Kishimoto (2016) Lithium ion conductivity of oriented Li0.33La0.56TiO3 solid electrolyte films prepared by a sol–gel process. Solid State Ionics 284: 1. https://doi.org/10.1016/j.ssi.2015.11.029
P Zhu, C Yan, M Dirican, et al. (2018) Li0.33La0.557TiO3 ceramic nanofiber-enhanced polyethylene oxide-based composite polymer electrolytes for all-solid-state lithium batteries. Journal of Materials Chemistry A 6: 4279. https://doi.org/10.1039/c7ta10517g
S Sasano, R Ishikawa, K Kawahara, et al. (2020) Grain boundary Li-ion conductivity in (Li0.33La0.56)TiO3 polycrystal. Applied Physics Letters 116. https://doi.org/10.1063/1.5141396
Lu DL, Zhao RR, Wu JL et al (2020) Investigations on the properties of Li3xLa2/3-xTiO3 based all-solid-state supercapacitor: relationships between the capacitance, ionic conductivity, and temperature. J Eur Ceram Soc 40:2396. https://doi.org/10.1016/j.jeurceramsoc.2020.02.006
Braun P, Uhlmann C, Weber A, Störmer H, Gerthsen D, Ivers-Tiffée E (2017) Separation of the bulk and grain boundary contributions to the total conductivity of solid lithium-ion conducting electrolytes. J Electroceram 38:157. https://doi.org/10.1007/s10832-016-0061-y
Du C-h Chen J (2015) Lithium ion diffusion mechanism in lithium lanthanum titanate solid-state electrolytes from atomistic simulations. J Am Ceram Soc 98:534. https://doi.org/10.1111/jace.13307
Thangadurai V, Weppner W (2000) Effect of B-site substitution of (Li, La)TiO3 perovskites by di-, tri-, tetra- and hexavalent metal ions on the lithium ion conductivity. Ionics 6:70. https://doi.org/10.1007/bf02375549
Le HTT, Kalubarme RS, Duc Tung N et al (2015) Citrate gel synthesis of aluminum-doped lithium lanthanum titanate solid electrolyte for application in organic-type lithium-oxygen batteries. J Power Sources 274:1188. https://doi.org/10.1016/j.jpowsour.2014.10.146
S Ulusoy, S Gulen, G Aygun, L Ozyuzer, M Ozdemir (2018) Characterization of thin film Li0.5La0.5Ti1-xAlxO3 electrolyte for all-solid-state Li-ion batteries. Solid State Ionics 324: 226. https://doi.org/10.1016/j.ssi.2018.07.005
Q Wang, J Zhang, X He, et al. (2019) Synergistic effect of cation ordered structure and grain boundary engineering on long-term cycling of Li0.35La0.55TiO3-based solid batteries. J. Eur. Ceram. Soc. 39: 3332. https://doi.org/10.1016/j.jeurceramsoc.2019.04.045
Morata-Orrantia A, Garcia-Martin S, Moran E, Alario-Franco MA (2002) A new La2/3LixTi1-xAlxO3 solid solution: structure, microstructure, and Li+ conductivity. Chem Mater 14:2871. https://doi.org/10.1021/cm011149s
Y Huang, Y Jiang, Y Zhou, X Liu, X Zeng, X Zhu (2021) One-step low-temperature synthesis of Li0.33La0.55TiO3 solid electrolytes by tape casting method. Ionics 27: 145. https://doi.org/10.1007/s11581-020-03823-y
Y Huang, X Liu, Y Jiang, X Zhu (2021) Synthesis of textured Li0.33La0.55TiO3 solid electrolytes by molten salt method. Ceramics International. https://doi.org/10.1016/j.ceramint.2021.01.003
M Chen, C Huang, Y Li, et al. (2019) Perovskite-type La0.56Li0.33TiO3 as an effective polysulfide promoter for stable lithium–sulfur batteries in lean electrolyte conditions. Journal of Materials Chemistry A 7: 10293. https://doi.org/10.1039/c9ta01500k
MW Khalid, YI Kim, MA Haq, et al. (2021) Densification behavior of microwave hybrid sintered Al2O3 bimodal powder mixtures and comparison with 3D modeling and simulation. International Journal of Refractory Metals and Hard Materials 99. https://doi.org/10.1016/j.ijrmhm.2021.105586
Zhang Z, Shao Y, Lotsch B et al (2018) New horizons for inorganic solid state ion conductors. Energy Environ Sci 11:1945. https://doi.org/10.1039/c8ee01053f
Y Harada, T Ishigaki, H Kawai, J Kuwano (1998) Lithium ion conductivity of polycrystalline perovskite La0.67-xLi3xTiO3 with ordered and disordered arrangements of the A-site ions. Solid State Ionics 108: 407. https://doi.org/10.1016/s0167-2738(98)00070-8
Morata-Orrantia A, Garcia-Martin S, Alario-Franco MA (2003) Optimization of lithium conductivity in La/Li titanates. Chem Mater 15:3991. https://doi.org/10.1021/cm0300563
Ban CW, Choi GM (2001) The effect of sintering on the grain boundary conductivity of lithium lanthanum titanates. Solid State Ionics 140:285. https://doi.org/10.1016/s0167-2738(01)00821-9
Zhong WL, Jiang B, Zhang PL et al (1993) Phase-transition in PbTiO3 ultrafine particles of different sizes. Journal of Physics-Condensed Matter 5:2619. https://doi.org/10.1088/0953-8984/5/16/018
Wu Y-J, Tanaka T, Komori T et al (2020) Essential structural and experimental descriptors for bulk and grain boundary conductivities of Li solid electrolytes. Sci Technol Adv Mater 21:712. https://doi.org/10.1080/14686996.2020.1824985
Cho SY, Park KS, Shim JE et al (2002) An integrated proteome database for two-dimensional electrophoresis data analysis and laboratory information management system. Proteomics 2:1104. https://doi.org/10.1002/1615-9861(200209)2:9%3c1104::Aid-prot1104%3e3.0.Co;2-q
L Cheng, W Chen, M Kunz, et al. (2015) Effect of surface microstructure on electrochemical performance of garnet solid electrolytes.Acs Applied Materials & Interfaces 7: 2073. https://doi.org/10.1021/am508111r
Ma C, Chen K, Liang CD et al (2014) Atomic-scale origin of the large grain-boundary resistance in perovskite Li-ion-conducting solid electrolytes. Energy Environ Sci 7:1638. https://doi.org/10.1039/c4ee00382a
NRL Bin Feng, Akihito Kumamoto, Yuichi Ikuhara, and Naoya Shibata (2017) Direct observation of oxygen vacancy distribution across yttria-stabilized zirconia grain boundaries. ASC nano 11. https://doi.org/10.1021/acsnano.7b05943
Feng B, Yokoi T, Kumamoto A, Yoshiya M, Ikuhara Y, Shibata N (2016) Atomically ordered solute segregation behaviour in an oxide grain boundary. Nat Commun 7:11079. https://doi.org/10.1038/ncomms11079
Guo X, Waser R (2006) Electrical properties of the grain boundaries of oxygen ion conductors: acceptor-doped zirconia and ceria. Prog Mater Sci 51:151. https://doi.org/10.1016/j.pmatsci.2005.07.001
S Qin, X Zhu, Y Jiang, Me Ling, Z Hu, J Zhu (2018) Growth of self-textured Ga3+-substituted Li7La3Zr2O12 ceramics by solid state reaction and their significant enhancement in ionic conductivity. Applied Physics Letters 112. https://doi.org/10.1063/1.5019179
M Ling, X Zhu, Y Jiang, J Zhu (2016) Comparative study of solid-state reaction and sol-gel process for synthesis of Zr-doped Li0.5La0.5TiO3 solid electrolytes. Ionics 22: 2151. https://doi.org/10.1007/s11581-016-1744-8
Kim KM, Shin DO, Lee Y-G (2015) Effects of preparation conditions on the ionic conductivity of hydrothermally synthesized Li1+xAlxTi2-x(PO4)(3) solid electrolytes. Electrochim Acta 176:1364. https://doi.org/10.1016/j.electacta.2015.07.170
Takatori K, Saura K, Orum A, Kadoura H, Tani T (2016) Textured lithium lanthanum titanate polycrystals prepared by a reactive-templated grain growth method. J Eur Ceram Soc 36:551. https://doi.org/10.1016/j.jeurceramsoc.2015.10.012
Funding
This work was financially supported by the Ministry of Science and Technology of China (MOST) (Grant No. 2013CB934700), Sichuan Science and Technology Program (Grant No. 2020YFH0047), and the Fundamental Research Funds for Central Universities.
Author information
Authors and Affiliations
Corresponding author
Ethics declarations
Conflict of interest
The authors declare no competing interests.
Additional information
Publisher's Note
Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.
Supplementary Information
Below is the link to the electronic supplementary material.
Rights and permissions
About this article
Cite this article
Huang, Y., He, L. & Zhu, X. Low temperature synthesis of Li0.33La0.55TiO3 solid electrolyte with Al3+ doping by a modified Pechini method. Ionics 28, 1739–1751 (2022). https://doi.org/10.1007/s11581-021-04422-1
Received:
Revised:
Accepted:
Published:
Issue Date:
DOI: https://doi.org/10.1007/s11581-021-04422-1