期刊
ADVANCED ENERGY MATERIALS
卷 9, 期 14, 页码 -出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/aenm.201803794
关键词
calcium-sulfur chemistry; electrochemical mechanism; electrochemical performance; lithium-ion mediation; rechargeable batteries
类别
资金
- U.S. Department of Energy, Office of Basic Energy Sciences, Division of Materials Sciences and Engineering [DE-SC0005397]
- Robert A. Welch Foundation [F-1535]
Calcium represents a promising anode for the development of high-energy-density, low-cost batteries. However, a lack of suitable electrolytes has restricted the development of rechargeable batteries with a Ca anode. Furthermore, to achieve a high energy density system, sulfur would be an ideal cathode to couple with the Ca anode. Unfortunately, a reversible calcium-sulfur (Ca-S) battery has not yet been reported. Herein, a basic study of a reversible nonaqueous room-temperature Ca-S battery is presented. The reversibility of the Ca-S chemistry and high utilization of the sulfur cathode are enabled by employing a Li+-ion-mediated calcium-based electrolyte. Mechanistic insights pursued by spectroscopic, electrochemical, microscopic, and theoretical simulation (density functional theory) investigations imply that the Li+-ions in the Ca-electrolyte stimulate the reactivation of polysulfide/sulfide species. The coordination of lithium to sulfur reduces the formation of sturdy Ca-S ionic bonds, thus boosting the reversibility of the Ca-S chemistry. In addition, the presence of Li+-ions facilitates the ionic charge transfer both in the electrolyte and across the solid electrolyte interphase layer, consequently reducing the interfacial and bulk impedance of Ca-S batteries. As a result, both the utilization of active sulfur in the cathode and the discharge voltage of Ca-S batteries are significantly improved.
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