Abstract

Sodium-ion batteries (SIBs) are regarded as one of the most promising candidates for next-generation energy storage devices and have been gradually grasping market share for their low cost and similar reaction mechanism and production process as compared to lithium-ion batteries. However, the low energy density of SIBs restricts their practical applications. For example, regular full cells of a Prussian blue cathode and NASICON anode have only a low discharge capacity (about 77 mA h/g at 1 C). Taking into account the compatibility of the electrolyte and electrode materials, a novel strategy for a viable aqueous dual-electrolyte sodium-ion battery (ADESIB) has been proposed using Na2SO4 solution as the anolyte and redox-active sodium hexacyanoferrate Na4Fe(CN)6 solution as the catholyte to accommodate a NASICON NaTi2(PO4)3 anode and Prussian blue Na2NiFe(CN)6 cathode. The capacity of Na+ ion deinsertion/insertion electrodes combined with the redox chemistry of the Na4Fe(CN)6 catholyte thus enhances overall charge storage and energy density. The ADESIB delivers a capacity of about 113 mA h/g at 1 C, showing a 43% improvement over batteries with a regular single Na2SO4 electrolyte. Additionally, the dual-electrolyte full-cell system is proved to reach a 84.7% capacity retention after 1000 cycles, mainly due to the synergy of the electrolytes in both sides. This pioneering research proposes an aqueous dual-electrolyte sodium-ion full cell, showing potential applications in a new sodium-ion full battery system.

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