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Evaluation of sulfur spinel compounds for multivalent battery cathode applications

Journal Article · · Energy & Environmental Science
DOI:https://doi.org/10.1039/c6ee01731b· OSTI ID:1474969
 [1];  [1];  [2];  [1];  [3];  [2];  [4];  [5]
  1. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Electrochemical Technologies Group
  2. Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States). Dept. of Materials Science and Engineering
  3. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Materials Sciences Division
  4. Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States). Dept. of Materials Science and Engineering; Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Materials Sciences Division; Univ. of California, Berkeley, CA (United States). Dept. of Materials Science and Engineering
  5. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Electrochemical Technologies Group; Univ. of California, Berkeley, CA (United States). Dept. of Materials Science and Engineering
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The rapid growth of portable consumer electronics and electric vehicles demands new battery technologies with greater energy stored at a reduced cost. Energy storage solutions based on multivalent metals, such as Mg, could significantly increase the energy density as compared to lithium-ion based technology. Here, we employ density functional theory calculations to systematically evaluate the performance, such as thermodynamic stability, ion diffusivity and voltage, of a group of 3d transition-metal sulfur-spinel compounds (21 in total) for multivalent cathode applications. Based on our calculations, Cr2S4, Ti2S4 and Mn2S4 spinel compounds exhibit improved Mg2+ mobility (diffusion activation energy <650 meV) relative to their oxide counterparts, however the improved mobility comes at the expense of lower voltage and thereby lower theoretical specific energy. Ca2+ intercalating into Cr2S4 spinel exhibits a low diffusion activation barrier of 500 meV and a voltage of ~2 V, revealing a potential cathode for use in Ca rechargeable batteries.
Research Organization:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Sponsoring Organization:
USDOE Office of Energy Efficiency and Renewable Energy (EERE); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Scientific User Facilities Division
Grant/Contract Number:
AC02-05CH11231; AC02-06CH11357
OSTI ID:
1474969
Journal Information:
Energy & Environmental Science, Journal Name: Energy & Environmental Science Journal Issue: 10 Vol. 9; ISSN EESNBY; ISSN 1754-5692
Publisher:
Royal Society of ChemistryCopyright Statement
Country of Publication:
United States
Language:
English

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Cited By (16)

Paving the Path toward Reliable Cathode Materials for Aluminum-Ion Batteries journal February 2019
Fervent Hype behind Magnesium Batteries: An Open Call to Synthetic Chemists-Electrolytes and Cathodes Needed journal August 2017
Sulfur‐ and Selenium‐Containing Compounds Potentially Exhibiting Al Ion Conductivity journal May 2019
Microstructure Characteristics of Cathode Materials for Rechargeable Magnesium Batteries journal March 2019
Magnesium Storage Performance and Mechanism of 2D‐Ultrathin Nanosheet‐Assembled Spinel MgIn 2 S 4 Cathode for High‐Temperature Mg Batteries journal July 2019
High magnesium mobility in ternary spinel chalcogenides journal November 2017
Analysis of Minerals as Electrode Materials for Ca-based Rechargeable Batteries journal July 2019
Ab initio study of Li, Mg and Al insertion into rutile VO 2 : fast diffusion and enhanced voltages for multivalent batteries journal January 2017
A critical review of cathodes for rechargeable Mg batteries journal January 2018
Exploring the sodium ion storage mechanism of gallium sulfide (Ga 2 S 3 ): a combined experimental and theoretical approach journal January 2019
Towards Al 3+ Mobility in Crystalline Solids: Critical Review and Analysis journal April 2019
On the Reliability of Half-Cell Tests for Monovalent (Li + , Na + ) and Divalent (Mg 2+ , Ca 2+ ) Cation Based Batteries journal January 2017
Insertion of Mono- vs. Bi- vs. Trivalent Atoms in Prospective Active Electrode Materials for Electrochemical Batteries: An ab Initio Perspective journal December 2017
Mg6MnO8 as a Magnesium-Ion Battery Material: Defects, Dopants and Mg-Ion Transport journal August 2019
Copper sulfide nanoparticles as high-performance cathode materials for Mg-ion batteries text January 2019
On the Balance of Intercalation and Conversion Reactions in Battery Cathodes text January 2018

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