Simple magnesium salts with high electrochemical and chemical stability and adequate ionic conductivity represent a new-generation electrolyte for magnesium (Mg) batteries. Similar to other Mg electrolytes, the simple-salt electrolyte also suffers from high charge-transfer resistance on the Mg surface due to the adsorbed species in the solution. In the current study, we built a model Mg cell system with the Mg[B(hfip) 4 ] 2 /DME electrolyte and Chevrel phase Mo 6 S 8 cathode, to demonstrate the effect of such anode−electrolyte interfacial properties on the full-cell performance. It was found that the cell required additional activation cycles to achieve its maximal capacity. The activation process is mainly attributed to the conditioning of the anode−electrolyte interface, which could be boosted by introducing an additive amount of Mg(BH 4 ) 2 to the Mg[B(hfip) 4 ] 2 /DME electrolyte. Electrochemical and spectroscopic analyses revealed that the Mg(BH 4 ) 2 additive helps to remove the native oxide layer and promotes the formation of a solid electrolyte interphase layer on Mg. As a result, the full cell with the additive-containing electrolyte delivered a stable capacity from the second cycle onward. Further battery tests showed a reversible cycling for 600 cycles and an excellent rate capability, indicating good compatibility of the Mg(BH 4 ) 2 additive. The current study not only provides fundamental insights into the interfacial phenomena in Mg batteries but also highlights the facile tunability of the simple-salt Mg electrolytes.
Rechargeable calcium batteries possess attractive features for sustainable energy-storage solutions owing to their high theoretical energy densities, safety aspects and abundant natural resources. However, divalent Ca-ions and reactive Ca metal strongly interact with cathode materials and non-aqueous electrolyte solutions, leading to high charge-transfer barriers at the electrode-electrolyte interface and consequently low electrochemical performance. Here, we demonstrate the feasibility and elucidate the electrochemical properties of calcium-tin (Ca–Sn) alloy anodes for Ca-ion chemistries. Crystallographic and microstructural characterizations reveal that Sn formed from electrochemically dealloying the Ca–Sn alloy possesses unique properties, and that this in-situ formed Sn undergoes subsequent reversible calciation/decalciation as CaSn3. As demonstration of the suitability of Ca–Sn alloys as anodes for Ca-ion batteries, we assemble coin cells with an organic cathode (1,4-polyanthraquinone) in an electrolyte of 0.25 M calcium tetrakis(hexafluoroisopropyloxy)borate in dimethoxyethane. These electrochemical cells are charged/discharged for 5000 cycles at 260 mA g−1, retaining a capacity of 78 mAh g−1 with respect to the organic cathode. The discovery of new class of Ca–Sn alloy anodes opens a promising avenue towards viable high-performance Ca-ion batteries.
Rechargeable magnesium batteries are gaining attention as promising candidates for large-scale energy storage applications because of their potentially high energy, safety and sustainability. However, the development of Mg batteries is impeded by the lack of efficient cathode materials and compatible electrode-electrolyte combinations. Herein, we demonstrate a new poly(1,4-anthraquinone)/Ketjenblack composite (14PAQ@KB) in combination with non-corrosive magne-sium tetrakis(hexafluoroisopropyloxy) borate Mg[B(hfip) 4 ] 2 (hfip = OC(H)(CF 3 ) 2 ) electrolyte towards high-energy and longlifespan Mg batteries. This combination exhibits prominent electrochemical performance including a maximum discharge capacity of 242 mA h g À 1 (approximately 93 % of the theoretical capacity), superior cycling stability (81 mA h g À 1 after 1000 cycles), and excellent rate capability (120 mA h g À 1 at 5 C).
Calcium (Ca) batteries represent an attractive option for electrochemical energy storage due to physicochemical and economic reasons. The standard reduction potential of Ca (−2.87 V) is close to Li and promises a wide voltage window for Ca full batteries, while the high abundance of Ca in the earth's crust implicates low material costs. However, the development of Ca batteries is currently hindered by technical issues such as the lack of compatible electrolytes for reversible Ca 2+ plating/stripping and high-capacity cathodes with fast kinetics. Herein, we employed FeS 2 as a conversion cathode material and combined it with a Li + /Ca 2+ hybrid electrolyte for Ca batteries. We demonstrate that Li + ions ensured reversible Ca 2+ plating/ stripping on the Ca metal anode with a small overpotential. At the same time, they enable the conversion of FeS 2 , offering high discharge capacity. As a result, the Ca/FeS 2 cell demonstrated an excellent long-term cycling performance with a high discharge capacity of 303 mAh g −1 over 200 cycles. Even though the practical application of such an approach is questionable due to the high quantity of electrolytes, we believe that our scientific findings still provide new directions for studying Ca batteries with long-term cycling.
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