Abstract:All‐solid‐state batteries with an alkali metal anode have the potential to achieve high energy density. However, the onset of dendrite formation limits the maximum plating current density across the solid electrolyte and prevents fast charging. It is shown that the maximum plating current density is related to the interfacial resistance between the solid electrolyte and the metal anode. Due to their high ionic conductivity, low electronic conductivity, and stability against sodium metal, Na‐β″‐alumina ceramics… Show more
“…It is interesting to note that this value is ~10× lower than reported values of the critical current density (CCD) in symmetric Li/LLZO/Li cells 18 . This may support recent hypotheses, which suggest that the combination of inhomogeneous Li plating and slow diffusivity, and deformation of electroplated Li, can result in regions of high pressure and act as nucleation sites for Li filaments 18 , 19 , 26 , 27 . Fig.…”
The coupling of solid-state electrolytes with a Li-metal anode and state-of-the-art (SOA) cathode materials is a promising path to develop inherently safe batteries with high energy density (>1000 Wh L−1). However, integrating metallic Li with solid-electrolytes using scalable processes is not only challenging, but also adds extraneous volume since SOA cathodes are fully lithiated. Here we show the potential for “Li-free” battery manufacturing using the Li7La3Zr2O12 (LLZO) electrolyte. We demonstrate that Li-metal anodes >20 μm can be electroplated onto a current collector in situ without LLZO degradation and we propose a model to relate electrochemical and nucleation behavior. A full cell consisting of in situ formed Li, LLZO, and NCA is demonstrated, which exhibits stable cycling over 50 cycles with high Coulombic efficiencies. These findings demonstrate the viability of “Li-free” configurations using LLZO which may guide the design and manufacturing of high energy density solid-state batteries.
“…It is interesting to note that this value is ~10× lower than reported values of the critical current density (CCD) in symmetric Li/LLZO/Li cells 18 . This may support recent hypotheses, which suggest that the combination of inhomogeneous Li plating and slow diffusivity, and deformation of electroplated Li, can result in regions of high pressure and act as nucleation sites for Li filaments 18 , 19 , 26 , 27 . Fig.…”
The coupling of solid-state electrolytes with a Li-metal anode and state-of-the-art (SOA) cathode materials is a promising path to develop inherently safe batteries with high energy density (>1000 Wh L−1). However, integrating metallic Li with solid-electrolytes using scalable processes is not only challenging, but also adds extraneous volume since SOA cathodes are fully lithiated. Here we show the potential for “Li-free” battery manufacturing using the Li7La3Zr2O12 (LLZO) electrolyte. We demonstrate that Li-metal anodes >20 μm can be electroplated onto a current collector in situ without LLZO degradation and we propose a model to relate electrochemical and nucleation behavior. A full cell consisting of in situ formed Li, LLZO, and NCA is demonstrated, which exhibits stable cycling over 50 cycles with high Coulombic efficiencies. These findings demonstrate the viability of “Li-free” configurations using LLZO which may guide the design and manufacturing of high energy density solid-state batteries.
“…6 Comparisons to traditional sodium ion conducting solid state electrolytes are also made with the NASICON family of materials (with the general formula Na1+xZr2SixP3−xO12) and sodium beta alumina as these are both promising and extensively studied candidate for sodium ion batteries. [48][49][50][51][52][53] Incremental improvements over the last 40 years have led to the increase in room temperature ionic conductivities from 10 -4 S cm -1 in undoped Na3Zr2Si2PO12, to 10 -3 S cm -1 with various structural substitution and optimisation of the microstructure e.g. by using nanoparticle precursors.…”
IL@MOF (IL: ionic liquid; MOF: metal-organic framework) materials have been proposed as a candidate for solid-state electrolytes, combining the inherent non-flammability and high thermal and chemical stability of the ionic...
“…[7,8] However, in view of the traditional solid-liquid contact has turned into solid-solid contact in SSSBs, how to maintain the physical contact and stabilize the interfacial structure between electrodes and SSEs have left substantial room to be investigated. [40][41][42][43][44] In this review, we summarize the key challenges in solidsolid interfaces versus liquid-solid interfaces, and discuss the interfacial stability, interfacial compatibility, interfacial characterization, as well as the approaches to effectively address dendrite issues. Then, various solid-solid interfaces and a few major advances within the field of SSSBs are listed in detail.…”
although some promising solutions have been proposed in battery design, traditional NIBs with organic liquid electrolytes are plagued by safety issues and limited energy density. [9] For instance, the high reactivity of metallic Na with organic liquid electrolytes and dendrite formation in the process of Na metal deposition can result in inferior electrochemical performance of cells. [10-14] Moreover, the low melting point of Na at 97.7 °C have been demonstrated to be a safety hazard, which may impede further applications of sodium metal-based batteries. [4] Therefore, fabricating cells with solid-state electrolytes (SSEs) rather than organic liquid electrolytes will constitute a significant step toward novel batteries, and solid-state sodium batteries (SSSBs) will also be an innovative approach to fully inherit the merits of both metallic Na and SSEs. [15-18] With the introduction of SSEs, safety issues originating from leakage and flammability of organic liquid electrolytes will no longer impede the development of sodium metal-based batteries and thus make them to be safer battery systems. [19-22] In addition, due to the slower reactivity of SSEs against electrodes, SSSBs can deliver a long cycle life and show great merit for successful operation of cells. [23,24] Versatile geometries originating from the nature of SSEs are also of prime significance to tailor battery properties. [25,26] To note, the solid polymer electrolytes (SPEs), gel polymer electrolytes (GPEs), and many derivatives of the abovementioned materials, which inherit the merits of both liquid-like solvating environments and the dimension stability, in a deeper perspective, belong to an intermediate class between the liquid-state and true solid-state. [27,28] In principle, exemplary cases of inorganic SSEs mainly include Na-β/β″-Al 2 O 3 , Na superionic conductor (NASICON), and sulfide electrolytes. [16,29-32] The introduction of such electrolytes will not only help effectively improving the safety of battery systems, but also open up the possibility of assembling a SSSB with high-voltage positive electrode at room temperature. [33] Nonetheless, the development of SSSBs is hindered by some severe challenges, and plenty of possibilities are waiting to be explored to reach the full potential of them. [34-36] Gas evolution issues, which originates from cathode materials and will result in safety concern and aging issues to cells, still exist in SSSBs. [37,38] Moreover, based on initial conjectures, the properties of SSSBs are expected to without being hampered by dendrite penetration, but recent studies have demonstrated the contrary belief. [39] Aside from the aforementioned obstacles, Solid-state sodium batteries (SSSBs) are considered as promising candidates for next-generation energy storage applications due to the probability to achieve safer and higher energy density characteristics. However, though SSSBs can avoid using combustible organic liquid electrolytes, the development of such novel batteries is hindered by some critical challenges. P...
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