Strongly correlated perovskite lithium ion shuttles

Yifei Sun, Michele Kotiuga, Dawgen Lim, Badri Narayanan, Mathew Cherukara, Zhen Zhang, Yongqi Dong, Ronghui Kou, Cheng Jun Sun, Qiyang Lu, Iradwikanari Waluyo, Adrian Hunt, Hidekazu Tanaka, Azusa N. Hattori, Sampath Gamage, Yohannes Abate, Vilas G. Pol, Hua Zhou, Subramanian K.R.S. Sankaranarayanan, Bilge YildizKarin Rabe, Shriram Ramanathan

Research output: Contribution to journalArticle

8 Citations (Scopus)

Abstract

Solid-state ion shuttles are of broad interest in electrochemical devices, nonvolatile memory, neuromorphic computing, and bio-mimicry utilizing synthetic membranes. Traditional design approaches are primarily based on substitutional doping of dissimilar valent cations in a solid lattice, which has inherent limits on dopant concentration and thereby ionic conductivity. Here, we demonstrate perovskite nickelates as Li-ion shuttles with simultaneous suppression of electronic transport via Mott transition. Electrochemically lithiated SmNiO3 (Li-SNO) contains a large amount of mobile Li+ located in interstitial sites of the perovskite approaching one dopant ion per unit cell. A significant lattice expansion associated with interstitial doping allows for fast Li+ conduction with reduced activation energy. We further present a generalization of this approach with results on other rare-earth perovskite nickelates as well as dopants such as Na+. The results highlight the potential of quantum materials and emergent physics in design of ion conductors.

Original languageEnglish (US)
Pages (from-to)9672-9677
Number of pages6
JournalProceedings of the National Academy of Sciences of the United States of America
Volume115
Issue number39
DOIs
StatePublished - Sep 25 2018

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Lithium
Ions
Physics
Cations
Equipment and Supplies
Membranes
perovskite

All Science Journal Classification (ASJC) codes

  • General

Keywords

  • Emergent phenomena
  • Ionic conductivity
  • Mott transition
  • Neuromorphic
  • Perovskite nickelate

Cite this

Sun, Y., Kotiuga, M., Lim, D., Narayanan, B., Cherukara, M., Zhang, Z., ... Ramanathan, S. (2018). Strongly correlated perovskite lithium ion shuttles. Proceedings of the National Academy of Sciences of the United States of America, 115(39), 9672-9677. https://doi.org/10.1073/pnas.1805029115
Sun, Yifei ; Kotiuga, Michele ; Lim, Dawgen ; Narayanan, Badri ; Cherukara, Mathew ; Zhang, Zhen ; Dong, Yongqi ; Kou, Ronghui ; Sun, Cheng Jun ; Lu, Qiyang ; Waluyo, Iradwikanari ; Hunt, Adrian ; Tanaka, Hidekazu ; Hattori, Azusa N. ; Gamage, Sampath ; Abate, Yohannes ; Pol, Vilas G. ; Zhou, Hua ; Sankaranarayanan, Subramanian K.R.S. ; Yildiz, Bilge ; Rabe, Karin ; Ramanathan, Shriram. / Strongly correlated perovskite lithium ion shuttles. In: Proceedings of the National Academy of Sciences of the United States of America. 2018 ; Vol. 115, No. 39. pp. 9672-9677.
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abstract = "Solid-state ion shuttles are of broad interest in electrochemical devices, nonvolatile memory, neuromorphic computing, and bio-mimicry utilizing synthetic membranes. Traditional design approaches are primarily based on substitutional doping of dissimilar valent cations in a solid lattice, which has inherent limits on dopant concentration and thereby ionic conductivity. Here, we demonstrate perovskite nickelates as Li-ion shuttles with simultaneous suppression of electronic transport via Mott transition. Electrochemically lithiated SmNiO3 (Li-SNO) contains a large amount of mobile Li+ located in interstitial sites of the perovskite approaching one dopant ion per unit cell. A significant lattice expansion associated with interstitial doping allows for fast Li+ conduction with reduced activation energy. We further present a generalization of this approach with results on other rare-earth perovskite nickelates as well as dopants such as Na+. The results highlight the potential of quantum materials and emergent physics in design of ion conductors.",
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Sun, Y, Kotiuga, M, Lim, D, Narayanan, B, Cherukara, M, Zhang, Z, Dong, Y, Kou, R, Sun, CJ, Lu, Q, Waluyo, I, Hunt, A, Tanaka, H, Hattori, AN, Gamage, S, Abate, Y, Pol, VG, Zhou, H, Sankaranarayanan, SKRS, Yildiz, B, Rabe, K & Ramanathan, S 2018, 'Strongly correlated perovskite lithium ion shuttles', Proceedings of the National Academy of Sciences of the United States of America, vol. 115, no. 39, pp. 9672-9677. https://doi.org/10.1073/pnas.1805029115

Strongly correlated perovskite lithium ion shuttles. / Sun, Yifei; Kotiuga, Michele; Lim, Dawgen; Narayanan, Badri; Cherukara, Mathew; Zhang, Zhen; Dong, Yongqi; Kou, Ronghui; Sun, Cheng Jun; Lu, Qiyang; Waluyo, Iradwikanari; Hunt, Adrian; Tanaka, Hidekazu; Hattori, Azusa N.; Gamage, Sampath; Abate, Yohannes; Pol, Vilas G.; Zhou, Hua; Sankaranarayanan, Subramanian K.R.S.; Yildiz, Bilge; Rabe, Karin; Ramanathan, Shriram.

In: Proceedings of the National Academy of Sciences of the United States of America, Vol. 115, No. 39, 25.09.2018, p. 9672-9677.

Research output: Contribution to journalArticle

TY - JOUR

T1 - Strongly correlated perovskite lithium ion shuttles

AU - Sun, Yifei

AU - Kotiuga, Michele

AU - Lim, Dawgen

AU - Narayanan, Badri

AU - Cherukara, Mathew

AU - Zhang, Zhen

AU - Dong, Yongqi

AU - Kou, Ronghui

AU - Sun, Cheng Jun

AU - Lu, Qiyang

AU - Waluyo, Iradwikanari

AU - Hunt, Adrian

AU - Tanaka, Hidekazu

AU - Hattori, Azusa N.

AU - Gamage, Sampath

AU - Abate, Yohannes

AU - Pol, Vilas G.

AU - Zhou, Hua

AU - Sankaranarayanan, Subramanian K.R.S.

AU - Yildiz, Bilge

AU - Rabe, Karin

AU - Ramanathan, Shriram

PY - 2018/9/25

Y1 - 2018/9/25

N2 - Solid-state ion shuttles are of broad interest in electrochemical devices, nonvolatile memory, neuromorphic computing, and bio-mimicry utilizing synthetic membranes. Traditional design approaches are primarily based on substitutional doping of dissimilar valent cations in a solid lattice, which has inherent limits on dopant concentration and thereby ionic conductivity. Here, we demonstrate perovskite nickelates as Li-ion shuttles with simultaneous suppression of electronic transport via Mott transition. Electrochemically lithiated SmNiO3 (Li-SNO) contains a large amount of mobile Li+ located in interstitial sites of the perovskite approaching one dopant ion per unit cell. A significant lattice expansion associated with interstitial doping allows for fast Li+ conduction with reduced activation energy. We further present a generalization of this approach with results on other rare-earth perovskite nickelates as well as dopants such as Na+. The results highlight the potential of quantum materials and emergent physics in design of ion conductors.

AB - Solid-state ion shuttles are of broad interest in electrochemical devices, nonvolatile memory, neuromorphic computing, and bio-mimicry utilizing synthetic membranes. Traditional design approaches are primarily based on substitutional doping of dissimilar valent cations in a solid lattice, which has inherent limits on dopant concentration and thereby ionic conductivity. Here, we demonstrate perovskite nickelates as Li-ion shuttles with simultaneous suppression of electronic transport via Mott transition. Electrochemically lithiated SmNiO3 (Li-SNO) contains a large amount of mobile Li+ located in interstitial sites of the perovskite approaching one dopant ion per unit cell. A significant lattice expansion associated with interstitial doping allows for fast Li+ conduction with reduced activation energy. We further present a generalization of this approach with results on other rare-earth perovskite nickelates as well as dopants such as Na+. The results highlight the potential of quantum materials and emergent physics in design of ion conductors.

KW - Emergent phenomena

KW - Ionic conductivity

KW - Mott transition

KW - Neuromorphic

KW - Perovskite nickelate

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U2 - 10.1073/pnas.1805029115

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AN - SCOPUS:85053894094

VL - 115

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JO - Proceedings of the National Academy of Sciences of the United States of America

JF - Proceedings of the National Academy of Sciences of the United States of America

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