Coupling chloride solid electrolytes (SEs) with ultrahigh-nickel oxide cathodes (LiNiCoMnO, > 0.9) exhibits higher interfacial stability and better safety than traditional sulfide SE-based cathodes. However, the inevitable ∼30 wt% addition of inactive chloride SEs for sufficient Li percolation sacrifices the electrode-level energy density.
View Article and Find Full Text PDFNano Lett
December 2024
Despite competitive compatibility with high-nickel cathodes, chloride solid electrolytes (SEs) still experience inevitable side reactions at the cathode/SE interface, causing capacity decay in all-solid-state lithium batteries (ASSLBs) during cycling. Herein, a three-electrode ASSLB testing device is developed to comprehensively reveal the interface failure mechanisms of the ultrahigh-nickel LiNiCoMnO (NCM92) cathode paired with LaCl-based chloride SE LiLaZrTaCl (LLZTC). Distribution of relaxation time (DRT) analysis clearly shows the ASSLB degradation accompanied by a significant NCM92/LLZTC interface impedance increase, which becomes more pronounced at the higher cutoff charging voltage of 4.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
April 2024
Halide superionic conductors (SICs) are drawing significant research attention for their potential applications in all-solid-state batteries. A key challenge in developing such SICs is to explore and design halide structural frameworks that enable rapid ion movement. In this work, we show that the close-packed anion frameworks shared by traditional halide ionic conductors face intrinsic limitations in fast ion conduction, regardless of structural regulation.
View Article and Find Full Text PDFSolid electrolytes (SEs) are central components that enable high-performance, all-solid-state lithium batteries (ASSLBs). Amorphous SEs hold great potential for ASSLBs because their grain-boundary-free characteristics facilitate intact solid-solid contact and uniform Li-ion conduction for high-performance cathodes. However, amorphous oxide SEs with limited ionic conductivities and glassy sulfide SEs with narrow electrochemical windows cannot sustain high-nickel cathodes.
View Article and Find Full Text PDFLead halide perovskite nanocrystals (LHP NCs) are regarded as promising emitters for next-generation ultrahigh-definition displays due to their high color purity and wide color gamut. Recently, the external quantum efficiency (EQE) of LHP NC based light-emitting diodes (PNC LEDs) has been rapidly improved to a level required by practical applications. However, the poor operational stability of the device, caused by halide ion migration at the grain boundary of LHP NC thin films, remains a great challenge.
View Article and Find Full Text PDFInorganic superionic conductors possess high ionic conductivity and excellent thermal stability but their poor interfacial compatibility with lithium metal electrodes precludes application in all-solid-state lithium metal batteries. Here we report a LaCl-based lithium superionic conductor possessing excellent interfacial compatibility with lithium metal electrodes. In contrast to a LiMCl (M = Y, In, Sc and Ho) electrolyte lattice, the UCl-type LaCl lattice has large, one-dimensional channels for rapid Li conduction, interconnected by La vacancies via Ta doping and resulting in a three-dimensional Li migration network.
View Article and Find Full Text PDFACS Appl Mater Interfaces
April 2022
Exploring new solid electrolytes (SEs) for lithium-ion conduction is significant for the development of rechargeable all-solid-state lithium batteries. Here, a lead-free organic-inorganic halide perovskite, MASrLiCl (MA = methylammonium, CHNH in formula), is reported as a new SE for Li-ion conduction due to its highly symmetric crystal structure, inherent soft lattice, and good tolerance for composition tunability. Via density functional theory calculations, we demonstrate that the hybrid perovskite framework can allow fast Li-ion migration without the collapse of the crystal structure.
View Article and Find Full Text PDFSolid electrolytes (SEs) with superionic conductivity and interfacial stability are highly desirable for stable all-solid-state Li-metal batteries (ASSLMBs). Here, we employ neural network potential to simulate materials composed of Li, Zr/Hf, and Cl using stochastic surface walking method and identify two potential unique layered halide SEs, named LiZrCl and LiHfCl, for stable ASSLMBs. The predicted halide SEs possess high Li conductivity and outstanding compatibility with Li metal anodes.
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