Fluid-enhanced surface diffusion controls intraparticle phase transformations

Yiyang Li, Hungru Chen, Kipil Lim, Haitao D. Deng, Jongwoo Lim, Dimitrios Fraggedakis, Peter M. Attia, Sang Chul Lee, Norman Jin, Jože Moškon, Zixuan Guan, William E. Gent, Jihyun Hong, Young Sang Yu, Miran Gaberšček, M. Saiful Islam, Martin Z. Bazant, William C. Chueh

Research output: Contribution to journalArticle

8 Citations (Scopus)

Abstract

Phase transformations driven by compositional change require mass flux across a phase boundary. In some anisotropic solids, however, the phase boundary moves along a non-conductive crystallographic direction. One such material is LiXFePO4, an electrode for lithium-ion batteries. With poor bulk ionic transport along the direction of phase separation, it is unclear how lithium migrates during phase transformations. Here, we show that lithium migrates along the solid/liquid interface without leaving the particle, whereby charge carriers do not cross the double layer. X-ray diffraction and microscopy experiments as well as ab initio molecular dynamics simulations show that organic solvent and water molecules promote this surface ion diffusion, effectively rendering LiXFePO4 a three-dimensional lithium-ion conductor. Phase-field simulations capture the effects of surface diffusion on phase transformation. Lowering surface diffusivity is crucial towards supressing phase separation. This work establishes fluid-enhanced surface diffusion as a key dial for tuning phase transformation in anisotropic solids.

Original languageEnglish
Pages (from-to)915-922
Number of pages8
JournalNature Materials
Volume17
Issue number10
DOIs
Publication statusPublished - 17 Sep 2018

ASJC Scopus subject areas

  • Chemistry(all)
  • Materials Science(all)
  • Condensed Matter Physics
  • Mechanics of Materials
  • Mechanical Engineering

Cite this

Li, Y., Chen, H., Lim, K., Deng, H. D., Lim, J., Fraggedakis, D., ... Chueh, W. C. (2018). Fluid-enhanced surface diffusion controls intraparticle phase transformations. Nature Materials, 17(10), 915-922. https://doi.org/10.1038/s41563-018-0168-4

Fluid-enhanced surface diffusion controls intraparticle phase transformations. / Li, Yiyang; Chen, Hungru; Lim, Kipil; Deng, Haitao D.; Lim, Jongwoo; Fraggedakis, Dimitrios; Attia, Peter M.; Lee, Sang Chul; Jin, Norman; Moškon, Jože; Guan, Zixuan; Gent, William E.; Hong, Jihyun; Yu, Young Sang; Gaberšček, Miran; Islam, M. Saiful; Bazant, Martin Z.; Chueh, William C.

In: Nature Materials, Vol. 17, No. 10, 17.09.2018, p. 915-922.

Research output: Contribution to journalArticle

Li, Y, Chen, H, Lim, K, Deng, HD, Lim, J, Fraggedakis, D, Attia, PM, Lee, SC, Jin, N, Moškon, J, Guan, Z, Gent, WE, Hong, J, Yu, YS, Gaberšček, M, Islam, MS, Bazant, MZ & Chueh, WC 2018, 'Fluid-enhanced surface diffusion controls intraparticle phase transformations', Nature Materials, vol. 17, no. 10, pp. 915-922. https://doi.org/10.1038/s41563-018-0168-4
Li Y, Chen H, Lim K, Deng HD, Lim J, Fraggedakis D et al. Fluid-enhanced surface diffusion controls intraparticle phase transformations. Nature Materials. 2018 Sep 17;17(10):915-922. https://doi.org/10.1038/s41563-018-0168-4
Li, Yiyang ; Chen, Hungru ; Lim, Kipil ; Deng, Haitao D. ; Lim, Jongwoo ; Fraggedakis, Dimitrios ; Attia, Peter M. ; Lee, Sang Chul ; Jin, Norman ; Moškon, Jože ; Guan, Zixuan ; Gent, William E. ; Hong, Jihyun ; Yu, Young Sang ; Gaberšček, Miran ; Islam, M. Saiful ; Bazant, Martin Z. ; Chueh, William C. / Fluid-enhanced surface diffusion controls intraparticle phase transformations. In: Nature Materials. 2018 ; Vol. 17, No. 10. pp. 915-922.
@article{c2a6336af9034a268c91999dc5e58949,
title = "Fluid-enhanced surface diffusion controls intraparticle phase transformations",
abstract = "Phase transformations driven by compositional change require mass flux across a phase boundary. In some anisotropic solids, however, the phase boundary moves along a non-conductive crystallographic direction. One such material is LiXFePO4, an electrode for lithium-ion batteries. With poor bulk ionic transport along the direction of phase separation, it is unclear how lithium migrates during phase transformations. Here, we show that lithium migrates along the solid/liquid interface without leaving the particle, whereby charge carriers do not cross the double layer. X-ray diffraction and microscopy experiments as well as ab initio molecular dynamics simulations show that organic solvent and water molecules promote this surface ion diffusion, effectively rendering LiXFePO4 a three-dimensional lithium-ion conductor. Phase-field simulations capture the effects of surface diffusion on phase transformation. Lowering surface diffusivity is crucial towards supressing phase separation. This work establishes fluid-enhanced surface diffusion as a key dial for tuning phase transformation in anisotropic solids.",
author = "Yiyang Li and Hungru Chen and Kipil Lim and Deng, {Haitao D.} and Jongwoo Lim and Dimitrios Fraggedakis and Attia, {Peter M.} and Lee, {Sang Chul} and Norman Jin and Jože Moškon and Zixuan Guan and Gent, {William E.} and Jihyun Hong and Yu, {Young Sang} and Miran Gaberšček and Islam, {M. Saiful} and Bazant, {Martin Z.} and Chueh, {William C.}",
year = "2018",
month = "9",
day = "17",
doi = "10.1038/s41563-018-0168-4",
language = "English",
volume = "17",
pages = "915--922",
journal = "Nature Materials",
issn = "1476-1122",
publisher = "Nature Research",
number = "10",

}

TY - JOUR

T1 - Fluid-enhanced surface diffusion controls intraparticle phase transformations

AU - Li, Yiyang

AU - Chen, Hungru

AU - Lim, Kipil

AU - Deng, Haitao D.

AU - Lim, Jongwoo

AU - Fraggedakis, Dimitrios

AU - Attia, Peter M.

AU - Lee, Sang Chul

AU - Jin, Norman

AU - Moškon, Jože

AU - Guan, Zixuan

AU - Gent, William E.

AU - Hong, Jihyun

AU - Yu, Young Sang

AU - Gaberšček, Miran

AU - Islam, M. Saiful

AU - Bazant, Martin Z.

AU - Chueh, William C.

PY - 2018/9/17

Y1 - 2018/9/17

N2 - Phase transformations driven by compositional change require mass flux across a phase boundary. In some anisotropic solids, however, the phase boundary moves along a non-conductive crystallographic direction. One such material is LiXFePO4, an electrode for lithium-ion batteries. With poor bulk ionic transport along the direction of phase separation, it is unclear how lithium migrates during phase transformations. Here, we show that lithium migrates along the solid/liquid interface without leaving the particle, whereby charge carriers do not cross the double layer. X-ray diffraction and microscopy experiments as well as ab initio molecular dynamics simulations show that organic solvent and water molecules promote this surface ion diffusion, effectively rendering LiXFePO4 a three-dimensional lithium-ion conductor. Phase-field simulations capture the effects of surface diffusion on phase transformation. Lowering surface diffusivity is crucial towards supressing phase separation. This work establishes fluid-enhanced surface diffusion as a key dial for tuning phase transformation in anisotropic solids.

AB - Phase transformations driven by compositional change require mass flux across a phase boundary. In some anisotropic solids, however, the phase boundary moves along a non-conductive crystallographic direction. One such material is LiXFePO4, an electrode for lithium-ion batteries. With poor bulk ionic transport along the direction of phase separation, it is unclear how lithium migrates during phase transformations. Here, we show that lithium migrates along the solid/liquid interface without leaving the particle, whereby charge carriers do not cross the double layer. X-ray diffraction and microscopy experiments as well as ab initio molecular dynamics simulations show that organic solvent and water molecules promote this surface ion diffusion, effectively rendering LiXFePO4 a three-dimensional lithium-ion conductor. Phase-field simulations capture the effects of surface diffusion on phase transformation. Lowering surface diffusivity is crucial towards supressing phase separation. This work establishes fluid-enhanced surface diffusion as a key dial for tuning phase transformation in anisotropic solids.

UR - http://www.scopus.com/inward/record.url?scp=85053558886&partnerID=8YFLogxK

U2 - 10.1038/s41563-018-0168-4

DO - 10.1038/s41563-018-0168-4

M3 - Article

VL - 17

SP - 915

EP - 922

JO - Nature Materials

JF - Nature Materials

SN - 1476-1122

IS - 10

ER -