The use of solid electrolytes is a promising direction to improve the energy density of lithium‐ion batteries. However, the low ionic conductivity of many solid electrolytes currently hinders the performance of solid‐state batteries. Sulfide solid electrolytes can be processed in a number of forms (glass, glass‐ceramic, and crystalline) and have a wide range of available chemistries. Crystalline sulfide materials demonstrate ionic conductivity on par with those of liquid electrolytes through the utilization of near ideal conduction pathways. Low‐temperature processing is also possible for these materials due to their favorable mechanical properties. The main drawback of sulfide solid electrolytes remains their electrochemical stability, but this can be addressed through compositional tuning or the use of artificial solid electrolyte interphase (SEI). Implementation of sulfide solid electrolytes, with proper treatment for stability, can lead to substantial improvements in solid‐state battery performance leading to significant advancement in electric vehicle technology.
Identifying positive
electrode materials capable of reversible
multivalent electrochemistry in electrolytes containing divalent ions
such as Mg2+, Ca2+, and Zn2+ at high
operating potentials remains an ongoing challenge in “beyond
lithium-ion” research. Herein, we explore the Zn2+ charge-storage mechanism of a vanadium-based Na+ superionic
conductor (NASICON), Na3V2(PO4)3. By using X-ray synchrotron techniques to unravel potential-dependent
structure–property relationships, we ascribe the reversible
electrochemical behavior of Na3V2(PO4)3 to a quasi-two-stage intercalation process that involves
both Na+ and Zn2+. Initial charging of Na3V2(PO4)3 leads to a Na+-extracted phase corresponding to NaV2(PO4)3, whereas subsequent discharge results predominantly
in Na+ intercalation followed by Zn2+ intercalation.
Operando X-ray diffraction of Na3V2(PO4)3 was used to study the phase changes associated with
the first charge/discharge process, and ex situ measurements were
used to precisely link the changes in the crystal structure to a quasi-two-stage
intercalation of Na+ and Zn2+. The corresponding
changes in the V-oxidation state, V-O coordination, and the presence
of Zn2+ were confirmed by X-ray absorption spectroscopy.
The results of this work present a comprehensive understanding of
the charge-storage properties for a well-established NASICON structure
that confers both the high capacity (∼100 mA h g–1) and high potential (1.35 and 1.1 V vs Zn/Zn2+).
Solid electrolytes have the potential to be safer alternatives to liquid electrolytes for lithium-ion batteries while being effectively configurable for powering small electronics. However, solid electrolytes typically exhibit poor interfaces and low ionic conductivity. Ionogel electrolytes, consisting of ionic liquid trapped inside a mesoporous solid, mitigate these limitations by maintaining a nanoscale fluidic state while behaving macroscopically solid. Adapting the synthesis process to achieve photo-patterning enables ionogels to be utilized in a variety of device architectures.
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