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Toward a Reversible Calcium‐Sulfur Battery with a Lithium‐Ion Mediation Approach
Author(s) -
Yu Xingwen,
Boyer Mathew J.,
Hwang Gyeong S.,
Manthiram Arumugam
Publication year - 2019
Publication title -
advanced energy materials
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 10.08
H-Index - 220
eISSN - 1614-6840
pISSN - 1614-6832
DOI - 10.1002/aenm.201803794
Subject(s) - polysulfide , electrolyte , anode , cathode , materials science , electrochemistry , inorganic chemistry , ionic bonding , sulfur , battery (electricity) , ion , chemical engineering , chemistry , electrode , organic chemistry , metallurgy , power (physics) , physics , quantum mechanics , engineering
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.