Abstract
NASICON- (Na superionic conductor-) based solid-state electrolytes (SSEs) are believed to be attracting candidates for solid-state sodium batteries due to their high ionic conductivity and prospectively reliable stability. However, the poor interface compatibility and the formation of Na dendrites inhibit their practical application. Herein, we directly observed the propagation of Na dendrites through NASICON-based Na 3.1 Zr 2 Si 2.1 P 0.9 O 12 SSE for the first time. Moreover, a fluorinated amorphous carbon (FAC) interfacial layer on the ceramic surface was simply developed by in situ carbonization of PVDF to improve the compatibility between Na metal and SSEs. Surprisingly, Na dendrites were effectively suppressed due to the formation of NaF in the interface when molten Na metal contacts with the FAC layer. Benefiting from the optimized interface, both the Na||Na symmetric cells and Na 3 V 2 (PO 4 ) 3 ||Na solid-state sodium batteries deliver remarkably electrochemical stability. These results offer benign reference to the maturation of NASICON-based solid-state sodium batteries.
Highlights
Na-ion batteries (NIBs) have been investigated broadly for the potential application in large-scale electrical energy storage due to the infinite sodium resources and relatively low cost [1,2,3,4,5,6]
The X-ray powder diffraction (XRD) pattern of the as-synthesized NZSP pellet matches the structure of monoclinic C2/c NASICON, as confirmed by the standard diffraction peaks located at around 19.2° and 27.5° (Supplementary Figure S1(a))
Little ZrO2 impurity appears, which is common during the synthesis of NASICON-based solid-state electrolytes (SSEs) using a ceramic method [34, 35]
Summary
Na-ion batteries (NIBs) have been investigated broadly for the potential application in large-scale electrical energy storage due to the infinite sodium resources and relatively low cost [1,2,3,4,5,6]. Owning to its low electrochemical potential of -2.71 V (vs standard hydrogen electrode) and high specific capacity of 1166 mAh g-1, Na metal becomes the most attractive anode for NIBs [4, 5, 7,8,9]. Failures arising from the formation of Na dendrites and severe side reactions hinder the extensive application of NIBs adopting a Na metal anode coupled with organic liquid electrolytes [10]. Developing solid-state sodium batteries (SSSBs) is regarded as an effective approach to physically stabilize the. Na anode/solid-state electrolyte (SSE) interface, suppressing the Na dendrites and side reactions due to the high mechanical strength and wide electrochemical window of SSEs [11, 12]. The NASICON-based SSSBs are considered to not Energy Material Advances
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