TY - JOUR
T1 - Hidden structural and chemical order controls lithium transport in cation-disordered oxides for rechargeable batteries
AU - Ji, Huiwen
AU - Urban, Alexander
AU - Kitchaev, Daniil A.
AU - Kwon, Deok Hwang
AU - Artrith, Nongnuch
AU - Ophus, Colin
AU - Huang, Wenxuan
AU - Cai, Zijian
AU - Shi, Tan
AU - Kim, Jae Chul
AU - Kim, Haegyeom
AU - Ceder, Gerbrand
N1 - Publisher Copyright:
© 2019, The Author(s).
PY - 2019/12/1
Y1 - 2019/12/1
N2 - Structure plays a vital role in determining materials properties. In lithium ion cathode materials, the crystal structure defines the dimensionality and connectivity of interstitial sites, thus determining lithium ion diffusion kinetics. In most conventional cathode materials that are well-ordered, the average structure as seen in diffraction dictates the lithium ion diffusion pathways. Here, we show that this is not the case in a class of recently discovered high-capacity lithium-excess rocksalts. An average structure picture is no longer satisfactory to understand the performance of such disordered materials. Cation short-range order, hidden in diffraction, is not only ubiquitous in these long-range disordered materials, but fully controls the local and macroscopic environments for lithium ion transport. Our discovery identifies a crucial property that has previously been overlooked and provides guidelines for designing and engineering cation-disordered cathode materials.
AB - Structure plays a vital role in determining materials properties. In lithium ion cathode materials, the crystal structure defines the dimensionality and connectivity of interstitial sites, thus determining lithium ion diffusion kinetics. In most conventional cathode materials that are well-ordered, the average structure as seen in diffraction dictates the lithium ion diffusion pathways. Here, we show that this is not the case in a class of recently discovered high-capacity lithium-excess rocksalts. An average structure picture is no longer satisfactory to understand the performance of such disordered materials. Cation short-range order, hidden in diffraction, is not only ubiquitous in these long-range disordered materials, but fully controls the local and macroscopic environments for lithium ion transport. Our discovery identifies a crucial property that has previously been overlooked and provides guidelines for designing and engineering cation-disordered cathode materials.
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U2 - 10.1038/s41467-019-08490-w
DO - 10.1038/s41467-019-08490-w
M3 - Article
C2 - 30723202
AN - SCOPUS:85061122255
VL - 10
JO - Nature Communications
JF - Nature Communications
IS - 1
M1 - 592
ER -