Aqueous Dual-Electrolyte Full-Cell System for Improving Energy Density of Sodium-Ion Batteries.

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.

Defect-Rich Amorphous Iron-Based Oxide/Graphene Hybrid-Modified Separator toward the Efficient Capture and Catalysis of Polysulfides.

The sluggish sulfur reduction reaction, severe shuttle effect, and poor conductivity of sulfur species are three main problems in lithium-sulfur (Li-S) batteries. Functional materials with a strong affinity and catalytic effect toward polysulfides play a key role in addressing these issues. Herein, we report a defect-rich amorphous a-Fe3O4-x/GO material with a nanocube-interlocked structure as an adsorber as well as an electrocatalyst for the Li-S battery. The composition and defect structure of the material are determined by X-ray diffraction, high-resolution transmission electron microscopy, Raman spectroscopy, and X-ray photoelectron spectroscopy measurements. The distinctive open framework architecture of the as-engineered composite inherited from the metal-organic framework precursor ensures the stability and activity of the catalyst during extended cycles. The oxygen defects in the amorphous structure are capable of absorbing polysulfides and similarly work as catalytic centers to boost polysulfide conversion. Taking advantage of a-Fe3O4-x/GO on the separator surface, the Li-S battery shows a capacity over 610 mA h g-1 at 1 C and a low decay rate of 0.12% per cycle over 500 cycles and superior rate capability. The functional material made via the low-cost synthesis process provides a potential solution for advanced Li-S batteries.

Structure Recovery and Recycling of Used LiCoO2 Cathode Material.

A large number of lithium batteries have been retiring from the market of energy storage. Thus, recycling of the used electrode materials is becoming urgent. In this study, an industrial machinery processing was used to recover the crystal structure of the waste LiCoO2 materials with the combination of small-scale equipment repair technology. The results show that the crystal parameters of the repaired LiCoO2 material become small, the unit cell volume is reduced, and the crystal structure tends to be stable. The Co-O bond length of 1.9134 nm, O-Co-O bond angle of 94.72°, the (003) interplanar spacing of 0.467 nm indicate the excellent recovery level of the repaired LiCoO2 . In addition, the electrochemical performance of the repaired LiCoO2 material is greatly improved, compared with the waste material. The capacity of the repaired electrode material can be maintained at 120 mAh g-1 after 100 cycles at the current density of 0.2C. The promising rate performance of the repaired electrode material demonstrates the stable structure. This research work provides a large-scale method for the direct recovery of LiCoO2 with the reduction of unnecessary energy and reagent consumption, which will be beneficial to the environmental protection.

Regulate Phosphorus Configuration in High P-Doped Hard Carbon as a Superanode for Sodium Storage.

Heteroatom-doped hard carbon is a popular method to optimize the electrochemical performance of anode electrodes for sodium-ion batteries. Herein, phosphorus-doped hollow carbon nanorods (P-HCNs) are obtained by a one-step synthesis with a high phosphorus content of 7.5 atom %. By controlling the P configuration, the P-HCNs03 exhibits reversible capacity as high as 260 mA h g-1 at the current density of 1.0 A g-1 after 500 cycles with an initial Coulombic efficiency (ICE) of 73%. When the amount of phosphorus in the as-prepared materials is changed, the different structures of the P-doped carbon lattices are analyzed by X-ray diffraction, Raman spectroscopy, and X-ray photoelectron spectroscopy. Based on the first-principles calculation, although the P-O bond has the most configurations, the excellent reversible capacity of the electrode is attributed to the strong Na-absorption ability of P═O and P-C bonds. The sodium-based dual-ion batteries (NDIBs) assembled with P-HCNs03 as an anode and expanded graphite as a cathode (P-HCNs03//EG) exhibited a high energy density of 138 W h kg-1 at a power density of 159 W kg-1. The results provide an important angle to optimize the performance of hard carbons with other functionalized heteroatoms.