Garnet-Based Electrolytes for Advanced All-Solid-State Lithium Battery

Abstract

All-solid-state lithium batteries are emerging as one of the key energy storage technologies due to their high theoretical energy density compared to conventional lithium- and sodium-ion-based batteries [1]. The present lithium batteries such as Li-S batteries suffer from Li dendrite formation and capacity decay due to polysulfide dissolution effect – a typical problem with liquid organic electrolytes [2]. Solid-state (ceramic) electrolytes are promising to prevent Li dendrite growth and polysulfide dissolution. Among the different ceramic electrolytes, garnet-type structure solid inorganic electrolytes are very promising because of their high lithium-ion conductivity and stability with elemental Li and humidity [3,4]. However, high interfacial resistance with the electrode is the major bottleneck for practical use of ceramic electrolytes [1]. In this talk, we will present strategies to solve the interfacial resistance issue in garnet-based electrolytes. Elemental doping [5], solution-based interface engineering [6], and hybrid polymer-ceramic electrolyte approach [7] will be discussed. Methods to improve lithium battery electrodes such as sulfur with minimal polysulfide shuttle effect will also be introduced [2]. References J. Samson, K. Hofstetter, S. Bag, and V Thangadurai,* “A bird's-eye view of Li-stuffed garnet-type Li7La3Zr2O12 ceramic electrolytes for advanced all-solid-state Li batteries,” Energy Environ. Sci., 12, 2957-2975 (2019).M. Abraham, S. P. Kammampata, S. Ponnurangam, and V. Thangadurai,* “Efficient Synthesis and Characterization of Robust MoS2 and S Cathode for Advanced Li-S Battery: Combined Experimental and Theoretical Studies,” ACS Appl. Mater. Interfaces 11, 35729-35737 (2019).Hofstetter, A. J. Samson, J. Dai, J. E. Gritton, L. Hu, E. D. Wachsman, and V. Thangadurai,* “Eelectrochemical stability of garnet-type Li7La2.75Ca0.25Zr1.75Nb0.25O12 with and without atomic layer deposited-Al2O3 under CO2 and humidity,” J. Electrochem. Soc., 166, A1844-A1852 (2019).Hofstetter, A. J. Samson, S. Narayanan, and V. Thangadurai,*“Present understanding of the stability of Li-stuffed garnets with moisture, carbon dioxide, and metallic lithium,” J. Power Sources, 390, 297–312 (2018).J. Samson, K. Hofstetter, E. Wachsman, and V. Thangadurai,*“Towards Mixed Ionic and Electronic Conducting Li-Stuffed Garnets,” J. Electrochem. Soc., 165, A1-A9 (2018).Zhou, A. J. Samson, K. Hofstetter, and V. Thangadurai,*Surfactant-Assisted Strategy to Tailor Li-ion Charge Transfer Interfacial Resistance for Scalable All-Solid-State Li Batteries, Sustainable Energy Fuels, 2, 2165 – 2170 (2018).Bag, C. Zhou, P.J. Kim, V.G. Pol, and V Thangadurai,* “LiF modified stable flexible PVDF-garnet hybrid electrolyte for high performance all-solid-state Li-S batteries,” Energy Storage Mater., 24, 198-207 (2020).