Crack‐Free Single‐Crystalline LiNiO 2 for High Energy Density All‐Solid‐State Batteries (in EN)
Abstract Single‐crystalline layered oxide (LiNi1‐x‐yMnxCoyO2) cathodes have been found to exhibit exceptional electrochemical properties when coupled with various inorganic solid electrolytes (ISEs) in all‐solid‐state batteries (ASSBs). Their advantages stem from the robust morphological integrity with the absence of grain boundaries and the high electrochemical oxidative stability. Here, ASSBs featuring single‐crystalline LiNiO2(LNO) with the highest Ni content are reported, offering a high theoretical specific capacity of 275 mAh g‐1alongside a high average discharge voltage (3.7 V vs Li+/Li). Through a careful investigation, it is demonstrated that micron‐sized single‐crystalline LNO (µSC‐LNO) composite cathodes with a halide ISE exhibit a high initial discharge capacity of 205 mAh g‐1with an outstanding cycle performance over 200 cycles in room‐temperature ASSBs. The significance of engineering parameters is emphasized, such as particle size and specific density, in promoting a homogeneous and fast Li+transport within the composite cathodes. Furthermore, the formation of undesirable interphase between the halide ISE in the cathode and sulfide ISE separator is elucidated, which may be a critical factor impeding long‐term cyclability of ASSBs. This work provides insights into the design of composite cathodes for high‐energy‐density ASSBs.
- Research Organization:
- Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)
- Sponsoring Organization:
- USDOE
- Grant/Contract Number:
- AC05-76RL01830; AC06-76RL01830
- OSTI ID:
- 2580546
- Journal Information:
- Advanced Energy Materials, Journal Name: Advanced Energy Materials Journal Issue: 19 Vol. 14; ISSN 1614-6832
- Publisher:
- WileyCopyright Statement
- Country of Publication:
- United States
- Language:
- EN
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