Toward a Reversible Calcium-Sulfur Battery with a Lithium-Ion Mediation Approach
Abstract
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.
- Authors:
-
- Univ. of Texas, Austin, TX (United States). Materials Science and Engineering Program; Univ. of Texas, Austin, TX (United States). Texas Materials Inst. (TMI)
- Univ. of Texas, Austin, TX (United States). McKetta Dept. of Chemical Engineering
- Publication Date:
- Research Org.:
- Univ. of Texas, Austin, TX (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division; Robert A. Welch Foundation
- OSTI Identifier:
- 1598280
- Alternate Identifier(s):
- OSTI ID: 1494846
- Grant/Contract Number:
- SC0005397
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Advanced Energy Materials
- Additional Journal Information:
- Journal Volume: 9; Journal Issue: 14; Journal ID: ISSN 1614-6832
- Publisher:
- Wiley
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 25 ENERGY STORAGE; calcium‐sulfur chemistry; electrochemical mechanism; electrochemical performance; lithium‐ion mediation; rechargeable batteries
Citation Formats
Yu, Xingwen, Boyer, Mathew J., Hwang, Gyeong S., and Manthiram, Arumugam. Toward a Reversible Calcium-Sulfur Battery with a Lithium-Ion Mediation Approach. United States: N. p., 2019.
Web. doi:10.1002/aenm.201803794.
Yu, Xingwen, Boyer, Mathew J., Hwang, Gyeong S., & Manthiram, Arumugam. Toward a Reversible Calcium-Sulfur Battery with a Lithium-Ion Mediation Approach. United States. https://doi.org/10.1002/aenm.201803794
Yu, Xingwen, Boyer, Mathew J., Hwang, Gyeong S., and Manthiram, Arumugam. Fri .
"Toward a Reversible Calcium-Sulfur Battery with a Lithium-Ion Mediation Approach". United States. https://doi.org/10.1002/aenm.201803794. https://www.osti.gov/servlets/purl/1598280.
@article{osti_1598280,
title = {Toward a Reversible Calcium-Sulfur Battery with a Lithium-Ion Mediation Approach},
author = {Yu, Xingwen and Boyer, Mathew J. and Hwang, Gyeong S. and Manthiram, Arumugam},
abstractNote = {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.},
doi = {10.1002/aenm.201803794},
journal = {Advanced Energy Materials},
number = 14,
volume = 9,
place = {United States},
year = {Fri Feb 15 00:00:00 EST 2019},
month = {Fri Feb 15 00:00:00 EST 2019}
}
Web of Science
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