Journal
ACS APPLIED MATERIALS & INTERFACES
Volume 13, Issue 47, Pages 56054-56063Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsami.1c15115
Keywords
solid electrolyte; garnet-type Li7La3Zr2O12; Li+ conductivity; Li2O atmosphere; air ambient sintering; solid-state lithium battery
Funding
- National Natural Science Foundation of China [51272221]
- Innovation Foundation for Postgraduate of Hunan Province [CX2018B369]
- Key Project of Strategic New Industry of Hunan Province, China [2019GK2032]
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The MCLL method proposed in this study effectively controls the Li2O atmosphere during the sintering process of highly conductive LLZO ceramics, resulting in high conductivity and potential applications.
Garnet-type Li7La3Zr2O12 (LLZO) is a promising solid-state electrolyte (SSE) due to its high Li+ conductivity and stability against lithium metal. However, wide research and application of LLZO are hampered by the difficulty in sintering highly conductive LLZO ceramics, which is mainly attributed to its poor sinterability and the hardship of controlling the Li2O atmosphere at a high sintering temperature (similar to 1200 degrees C). Herein, an efficient mutual-compensating Li-loss (MCLL) method is proposed to effectively control the Li2O atmosphere during the sintering process for highly conductive LLZO ceramics. The Li6.5La3Zr1.5Ta0.5O12 (LLZTO) ceramic SSEs sintered by the MCLL method own high relative density (96%), high Li content (5.54%), high conductivity (7.19 x 10(-4) S cm(-1)), and large critical current density (0.85 mA cm(-2)), equating those sintered by a hot-pressing technique. The assembled Li-Li symmetric battery and a Li-metal solid-state battery (LMSSB) show that the as-prepared LLZTO can achieve a small interfacial resistance (17 Omega cm(2)) with Li metal, exhibits high electrochemical stability against Li metal, and has broad potential in the application of LMSSBs. In addition, this method can also improve the sintering efficiency, avoid the use of mother powder, and reduce raw-material cost, and thus it may promote the large-scale preparation and wide application of LLZO ceramic SSE.
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