The abundance of Ca, its low redox potential and high specific capacity make Ca metal batteries an attractive energy storage system for the future. A recent demonstration of room temperature calcium plating/stripping opened a new avenue of the development, but the performance of cathode materials is lagging far behind. Due to the nature of divalent cations, conversion and coordination electrochemical reactions show better performance compared to insertion. Herein, we demonstrate the use of the anthraquinone‐based polymer as a cathode material for the Ca metal‐organic battery. Electrochemical mechanism investigation confirms the reversible reduction of the carbonyl bond and coordination with Ca2+ cations in the discharged state, opening a pathway toward high energy density battery. Continued performance of a 2‐electrode cell is strongly hampered by the overpotential increase caused by the Ca stripping process on the Ca metal anode stating the need for further development of Ca electrolytes. Ca metal‐organic battery promises to achieve cells with gravimetric energy density on the practical level compared to the state‐of‐the‐art Li‐ion batteries.
Calcium batteries represent a promising alternative to lithium metal batteries. The combination of the low redox potential and low-cost and energy-dense calcium anode (2073 mAh/cm 3 , similar to 2044 mAh/cm 3 for Li) with appropriate low-cost cathode materials such as sulfur, could produce a game-changing technology in several fields of applications. In this work, we present the reversible activity of a proof-of-concept Ca/S battery at room temperature, characterized by a surprising medium-term cycling stability with low polarization, promoted by the use of a simple positive electrode made of sulfur supported on an activated carbon cloth scaffold, and a state-of-the-art fluorinated alkoxyborate-based electrolyte. Insights on the electrochemical mechanism governing the chemistry of the Ca/S system were obtained for the first time by combining X-ray photoelectron spectroscopy and X-ray absorption spectroscopy. The mechanism implies the formation of different types of soluble polysulfides species during both charge and discharge at room temperature, and the formation of solid CaS at the end of discharge. The reversible electrochemical activity is proven by the reformation of elemental sulfur at the end of the following charge. These promising results open the way to the comprehension of emerging Ca/S systems which may represent a valid alternative to Mg/S and Li/S batteries.
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