DataVXACS Energy LettersPaper
journal article·2018-10-12Open access

Correlated Polyhedral Rotations in the Absence of Polarons during Electrochemical Insertion of Lithium in ReO3

Nicholas H. Bashian, Shiliang Zhou, Mateusz Zuba, Alex M. Ganose, Joseph W. Stiles, Allyson Ee, David S. Ashby, David O. Scanlon, Louis F. J. Piper, Bruce Dunn, Brent C. Melot

ACS Energy Letters· Volume 3· Issue 10
Publisher pageOpen full text
Source abstract

Abstract

Understanding the structural transformations that materials undergo during (de)insertion of Li ions is crucial for designing high-performance intercalation hosts as these deformations can lead to significant capacity fade. Herein, we present a study of the metallic defect perovskite ReO3 to determine whether these distortions are driven by polaronic charge transport (i.e., the electrons and ions moving through the lattice in a coupled way) due to the semiconducting nature of most oxide hosts. Employing numerous techniques, including electrochemical probes, operando X-ray diffraction, X-ray photoelectron spectroscopy, and density functional theory calculations, we find that the cubic structure of ReO3 experiences multiple phase changes involving the correlated twisting of rigid octahedral subunits upon lithiation. This results in exceptionally poor long-term cyclability due to large strains upon lithiation, even though metallic character is maintained throughout. This suggests that phase transformations during alkali ion intercalation are the result of local strains in the lattice and not exclusively due to polaron migration.
Source: openalex_inverted_index · Quality: baseline

Research context

Electronic materials

OpenAlex topics: Advancements in Battery Materials · Advanced Battery Materials and Technologies · Ferroelectric and Piezoelectric Materials

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

Department of Chemistry, University of Southern California, Los Angeles, California 90089, United States

Department of Physics, Applied Physics and Astronomy, Binghamton University, Binghamton, New York 13902, United States

Department of Chemistry, University College London, 20 Gordon Street, London WC1H 0AJ, U.K.

Diamond Light Source Ltd., Diamond House, Harwell Science and Innovation Campus, Didcot, Oxfordshire OX11 0DE, U.K.

Thomas Young Centre, University College London, Gower Street, London WC1E 6BT, U.K.

Department of Materials Science and Engineering, University of California, Los Angeles, California 90095, United States

The Faraday Institution, Quad One, Harwell Science and Innovation Campus, Didcot OX11 0RA, U.K.

Materials Science & Engineering, Binghamton University, Binghamton, New York 13902, United States

Funding

Engineering and Physical Sciences Research Council · Basic Energy Sciences · Research Corporation for Science Advancement · U.S. Department of Education · Division of Materials Research · Faraday Institution

References (22)

Show source-provided references
1. 10.1021/acs.chemmater.6b0180610.1021/acs.chemmater.6b01806 ↗
2. 10.1021/acsami.6b1621610.1021/acsami.6b16216 ↗
3. 10.1021/acs.jpcc.7b0611810.1021/acs.jpcc.7b06118 ↗
4. 10.1021/acsomega.7b0146210.1021/acsomega.7b01462 ↗
5. 10.1038/ncomms1202210.1038/ncomms12022 ↗
6. 10.1016/0022-4596(82)90004-410.1016/0022-4596(82)90004-4 ↗
7. 10.1016/0022-4596(83)90239-610.1016/0022-4596(83)90239-6 ↗
8. 10.1063/1.312078310.1063/1.3120783 ↗
9. 10.1103/PhysRevB.78.13410510.1103/PhysRevB.78.134105 ↗
10. 10.1021/am405579h10.1021/am405579h ↗
11. 10.1021/jp055670b10.1021/jp055670b ↗
12. 10.1021/ja01150a11710.1021/ja01150a117 ↗
13. 10.1016/j.jcis.2013.01.03010.1016/j.jcis.2013.01.030 ↗
14. 10.1021/acs.chemmater.5b0214510.1021/acs.chemmater.5b02145 ↗
15. 10.1149/1.139163110.1149/1.1391631 ↗
16. 10.1149/1.139097710.1149/1.1390977 ↗
17. 10.1149/1.139169310.1149/1.1391693 ↗
18. 10.1149/2.0141505jes10.1149/2.0141505jes ↗
19. 10.1103/PhysRev.181.98710.1103/PhysRev.181.987 ↗
20. 10.1021/jp963724z10.1021/jp963724z ↗
21. 10.1515/zpch-2014-000210.1515/zpch-2014-0002 ↗
22. Scofield, J. H. T. Theoretical Photoionization Cross Sections from 1 to 1500 keV; UCRL-51326; Lawrence Livermore Laboratory, 1973.10.2172/4545040 ↗