Evaluation of sulfur spinel compounds for multivalent battery cathode applications
Abstract
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.
- Authors:
-
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Electrochemical Technologies Group
- 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
- 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
- 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
- Publication Date:
- Research Org.:
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities Division; USDOE Office of Energy Efficiency and Renewable Energy (EERE)
- OSTI Identifier:
- 1474969
- Grant/Contract Number:
- AC02-05CH11231; AC02-06CH11357; EDCBEE
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Energy & Environmental Science
- Additional Journal Information:
- Journal Volume: 9; Journal Issue: 10; Related Information: © 2016 The Royal Society of Chemistry.; Journal ID: ISSN 1754-5692
- Publisher:
- Royal Society of Chemistry
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 25 ENERGY STORAGE; 36 MATERIALS SCIENCE
Citation Formats
Liu, Miao, Jain, Anubhav, Rong, Ziqin, Qu, Xiaohui, Canepa, Pieremanuele, Malik, Rahul, Ceder, Gerbrand, and Persson, Kristin A. Evaluation of sulfur spinel compounds for multivalent battery cathode applications. United States: N. p., 2016.
Web. doi:10.1039/c6ee01731b.
Liu, Miao, Jain, Anubhav, Rong, Ziqin, Qu, Xiaohui, Canepa, Pieremanuele, Malik, Rahul, Ceder, Gerbrand, & Persson, Kristin A. Evaluation of sulfur spinel compounds for multivalent battery cathode applications. United States. https://doi.org/10.1039/c6ee01731b
Liu, Miao, Jain, Anubhav, Rong, Ziqin, Qu, Xiaohui, Canepa, Pieremanuele, Malik, Rahul, Ceder, Gerbrand, and Persson, Kristin A. Wed .
"Evaluation of sulfur spinel compounds for multivalent battery cathode applications". United States. https://doi.org/10.1039/c6ee01731b. https://www.osti.gov/servlets/purl/1474969.
@article{osti_1474969,
title = {Evaluation of sulfur spinel compounds for multivalent battery cathode applications},
author = {Liu, Miao and Jain, Anubhav and Rong, Ziqin and Qu, Xiaohui and Canepa, Pieremanuele and Malik, Rahul and Ceder, Gerbrand and Persson, Kristin A.},
abstractNote = {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.},
doi = {10.1039/c6ee01731b},
journal = {Energy & Environmental Science},
number = 10,
volume = 9,
place = {United States},
year = {Wed Aug 17 00:00:00 EDT 2016},
month = {Wed Aug 17 00:00:00 EDT 2016}
}
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