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Title: Odyssey of Multivalent Cathode Materials: Open Questions and Future Challenges

We report that the rapidly expanding field of nonaqueous multivalent intercalation batteries offers a promising way to overcome safety, cost, and energy density limitations of state-of-the-art Li-ion battery technology. We present a critical and rigorous analysis of the increasing volume of multivalent battery research, focusing on a wide range of intercalation cathode materials and the mechanisms of multivalent ion insertion and migration within those frameworks. The present analysis covers a wide variety of material chemistries, including chalcogenides, oxides, and polyanions, highlighting merits and challenges of each class of materials as multivalent cathodes. The review underscores the overlap of experiments and theory, ranging from charting the design metrics useful for developing the next generation of MV-cathodes to targeted in-depth studies rationalizing complex experimental results. In conclusion, on the basis of our critical review of the literature, we provide suggestions for future multivalent cathode studies, including a strong emphasis on the unambiguous characterization of the intercalation mechanisms.
Authors:
ORCiD logo [1] ; ORCiD logo [2] ;  [3] ;  [4] ;  [5] ;  [6] ;  [5] ;  [2]
  1. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Materials Science Division; Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States). Department of Materials Science and Engineering
  2. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Materials Science Division; Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States). Department of Materials Science and Engineering; Univ. of California, Berkeley, CA (United States). Department of Materials Science and Engineering
  3. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Materials Science Division
  4. Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States). Department of Materials Science and Engineering
  5. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Energy and Environmental Science Division
  6. Argonne National Lab. (ANL), Argonne, IL (United States). Chemical Sciences and Engineering
Publication Date:
Grant/Contract Number:
AC02-05CH11231; 3F-31144
Type:
Published Article
Journal Name:
Chemical Reviews
Additional Journal Information:
Journal Volume: 117; Journal Issue: 5; Related Information: © 2017 American Chemical Society.; Journal ID: ISSN 0009-2665
Publisher:
American Chemical Society
Research Org:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 25 ENERGY STORAGE
OSTI Identifier:
1343461
Alternate Identifier(s):
OSTI ID: 1476467

Canepa, Pieremanuele, Sai Gautam, Gopalakrishnan, Hannah, Daniel C., Malik, Rahul, Liu, Miao, Gallagher, Kevin G., Persson, Kristin A., and Ceder, Gerbrand. Odyssey of Multivalent Cathode Materials: Open Questions and Future Challenges. United States: N. p., Web. doi:10.1021/acs.chemrev.6b00614.
Canepa, Pieremanuele, Sai Gautam, Gopalakrishnan, Hannah, Daniel C., Malik, Rahul, Liu, Miao, Gallagher, Kevin G., Persson, Kristin A., & Ceder, Gerbrand. Odyssey of Multivalent Cathode Materials: Open Questions and Future Challenges. United States. doi:10.1021/acs.chemrev.6b00614.
Canepa, Pieremanuele, Sai Gautam, Gopalakrishnan, Hannah, Daniel C., Malik, Rahul, Liu, Miao, Gallagher, Kevin G., Persson, Kristin A., and Ceder, Gerbrand. 2017. "Odyssey of Multivalent Cathode Materials: Open Questions and Future Challenges". United States. doi:10.1021/acs.chemrev.6b00614.
@article{osti_1343461,
title = {Odyssey of Multivalent Cathode Materials: Open Questions and Future Challenges},
author = {Canepa, Pieremanuele and Sai Gautam, Gopalakrishnan and Hannah, Daniel C. and Malik, Rahul and Liu, Miao and Gallagher, Kevin G. and Persson, Kristin A. and Ceder, Gerbrand},
abstractNote = {We report that the rapidly expanding field of nonaqueous multivalent intercalation batteries offers a promising way to overcome safety, cost, and energy density limitations of state-of-the-art Li-ion battery technology. We present a critical and rigorous analysis of the increasing volume of multivalent battery research, focusing on a wide range of intercalation cathode materials and the mechanisms of multivalent ion insertion and migration within those frameworks. The present analysis covers a wide variety of material chemistries, including chalcogenides, oxides, and polyanions, highlighting merits and challenges of each class of materials as multivalent cathodes. The review underscores the overlap of experiments and theory, ranging from charting the design metrics useful for developing the next generation of MV-cathodes to targeted in-depth studies rationalizing complex experimental results. In conclusion, on the basis of our critical review of the literature, we provide suggestions for future multivalent cathode studies, including a strong emphasis on the unambiguous characterization of the intercalation mechanisms.},
doi = {10.1021/acs.chemrev.6b00614},
journal = {Chemical Reviews},
number = 5,
volume = 117,
place = {United States},
year = {2017},
month = {2}
}