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Published August 2013 | Supplemental Material
Journal Article Open

A High Capacity Calcium Primary Cell Based on the Ca–S System

Abstract

Conversion reaction cells afford the ability to explore new energy storage paradigms that transcend the dogma of small, low‐charge cations essential to intercalative processes. Here we report the use of earth‐abundant and green calcium and sulfur in unprecedented conversion reaction Ca–S primary cells. Using S‐infiltrated mesoporous carbon (abbreviated S@meso‐C) cathodes, we achieve discharge capacities as high as 600 mAh g^(−1) (S basis) within the geometry Ca|Ca(ClO_4)_2/CH_3CN|S@meso‐C, at a discharge rate of C/3.5. The electrolyte system in the Ca–S battery is of paramount importance as the solid electrolyte interface (SEI) formed on the Ca anode limits the capacity and stability of the cell. We determine that 0.5 M Ca(ClO_4)_2 in CH_3CN forms an SEI that advantageously breaks down under anodic bias to allow oxidation of the anode. This same SEI, however, exhibits high impedance which increases over time at open circuit limiting the shelf life of the cell.

Additional Information

© 2013 WILEY‐VCH. Received: February 12, 2013. Published online: April 5, 2013. We thank Dr. Makoto Ue and Dr. Tomohiro Kawai of Mitsubishi Chemical for helpful discussions on electrochemical methods. Fellowship support to KAS from the ConvEne IGERT Program of the National Science Foundation (DGE 0801627) is gratefully acknowledged. This research made extensive use of the shared experimental facilities of the Materials Research Laboratory, supported by the MRSEC Program of the NSF (DMR 1121053). We also thank Dr. James Pavlovich for assistance with mass spectrometry.

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