Toward a Reversible Calcium-Sulfur Battery with a Lithium-Ion Mediation Approach

Yu, Xingwen; Boyer, Mathew J.; Hwang, Gyeong S.; Manthiram, Arumugam

doi:10.1002/aenm.201803794

Toward a Reversible Calcium-Sulfur Battery with a Lithium-Ion Mediation Approach

Journal Article · Fri Feb 15 00:00:00 EST 2019 · Advanced Energy Materials

DOI:https://doi.org/10.1002/aenm.201803794· OSTI ID:1598280

Yu, Xingwen ^[1]; Boyer, Mathew J. ^[2]; Hwang, Gyeong S. ^[2]; ^[3]

Univ. of Texas, Austin, TX (United States). Materials Science and Engineering Program; Univ. of Texas, Austin, TX (United States). Texas Materials Inst. (TMI); University of Texas at Austin
Univ. of Texas, Austin, TX (United States). McKetta Dept. of Chemical Engineering
Univ. of Texas, Austin, TX (United States). Materials Science and Engineering Program; Univ. of Texas, Austin, TX (United States). Texas Materials Inst. (TMI)

Calcium represents a promising anode for the development of high-energy-density, low-cost batteries. Yet, 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. Furthermore, 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.

View Accepted Manuscript (DOE)

Research Organization:: Univ. of Texas, Austin, TX (United States)

Sponsoring Organization:: Robert A. Welch Foundation; USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division

Grant/Contract Number:: SC0005397

OSTI ID:: 1598280

Alternate ID(s):: OSTI ID: 1494846

Journal Information:: Advanced Energy Materials, Journal Name: Advanced Energy Materials Journal Issue: 14 Vol. 9; ISSN 1614-6832

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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