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Title: On the Balance of Intercalation and Conversion Reactions in Battery Cathodes

Abstract

A thermodynamic analysis of the driving forces is presented for intercalation and conversion reactions in battery cathodes across a range of possible working ion, transition metal, and anion chemistries. Using this body of results, the importance of polymorph selection as well as chemical composition on the ability of a host cathode to support intercalation reactions is analyzed. It is found that the accessibility of high energy charged polymorphs in oxides generally leads to larger intercalation voltages favoring intercalation reactions, whereas sulfides and selenides tend to favor conversion reactions. Furthermore, it is observed that Cr‐containing cathodes favor intercalation more strongly than those with other transition metals. Finally, it is concluded that two‐electron reduction of transition metals (as is possible with the intercalation of a 2 + ion) will favor conversion reactions in the compositions studied.

Authors:
 [1]; ORCiD logo [2]; ORCiD logo [1]; ORCiD logo [3]
  1. Materials Science Division, Lawrence Berkeley National Laboratory, Berkeley CA 94720 USA
  2. Materials Science Division, Lawrence Berkeley National Laboratory, Berkeley CA 94720 USA; Department of Materials Science and Engineering, Massachusetts Institute of Technology, Cambridge MA 02139 USA; Department of Materials Science and Engineering, University of California, Berkeley CA 94720 USA
  3. Materials Science Division, Lawrence Berkeley National Laboratory, Berkeley CA 94720 USA; Department of Materials Science and Engineering, University of California, Berkeley CA 94720 USA
Publication Date:
Research Org.:
Lawrence Berkeley National Laboratory-National Energy Research Scientific Computing Center (NERSC)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1543466
Resource Type:
Journal Article
Journal Name:
Advanced Energy Materials
Additional Journal Information:
Journal Volume: 8; Journal Issue: 20; Journal ID: ISSN 1614-6832
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
Chemistry; Energy & Fuels; Materials Science; Physics

Citation Formats

Hannah, Daniel C., Sai Gautam, Gopalakrishnan, Canepa, Pieremanuele, and Ceder, Gerbrand. On the Balance of Intercalation and Conversion Reactions in Battery Cathodes. United States: N. p., 2018. Web. doi:10.1002/aenm.201800379.
Hannah, Daniel C., Sai Gautam, Gopalakrishnan, Canepa, Pieremanuele, & Ceder, Gerbrand. On the Balance of Intercalation and Conversion Reactions in Battery Cathodes. United States. doi:10.1002/aenm.201800379.
Hannah, Daniel C., Sai Gautam, Gopalakrishnan, Canepa, Pieremanuele, and Ceder, Gerbrand. Mon . "On the Balance of Intercalation and Conversion Reactions in Battery Cathodes". United States. doi:10.1002/aenm.201800379.
@article{osti_1543466,
title = {On the Balance of Intercalation and Conversion Reactions in Battery Cathodes},
author = {Hannah, Daniel C. and Sai Gautam, Gopalakrishnan and Canepa, Pieremanuele and Ceder, Gerbrand},
abstractNote = {A thermodynamic analysis of the driving forces is presented for intercalation and conversion reactions in battery cathodes across a range of possible working ion, transition metal, and anion chemistries. Using this body of results, the importance of polymorph selection as well as chemical composition on the ability of a host cathode to support intercalation reactions is analyzed. It is found that the accessibility of high energy charged polymorphs in oxides generally leads to larger intercalation voltages favoring intercalation reactions, whereas sulfides and selenides tend to favor conversion reactions. Furthermore, it is observed that Cr‐containing cathodes favor intercalation more strongly than those with other transition metals. Finally, it is concluded that two‐electron reduction of transition metals (as is possible with the intercalation of a 2 + ion) will favor conversion reactions in the compositions studied.},
doi = {10.1002/aenm.201800379},
journal = {Advanced Energy Materials},
issn = {1614-6832},
number = 20,
volume = 8,
place = {United States},
year = {2018},
month = {4}
}

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