TY - JOUR
T1 - A two-dimensional type I superionic conductor
AU - Rettie, Alexander J.E.
AU - Ding, Jingxuan
AU - Zhou, Xiuquan
AU - Johnson, Michael J.
AU - Malliakas, Christos D.
AU - Osti, Naresh C.
AU - Chung, Duck Young
AU - Osborn, Raymond
AU - Delaire, Olivier
AU - Rosenkranz, Stephan
AU - Kanatzidis, Mercouri G.
N1 - Funding Information:
We are indebted to W. Xu for assistance in the acquisition and analysis of X-ray total scattering data and to E. Mamontov for valuable discussions concerning the QENS data analysis. M.J.J. acknowledges HORIBA-Motor Industry Research Association (MIRA), University College London (UCL) and the Engineering and Physical Sciences Research Council (EPSRC) (EP/R513143/1) for a Collaborative Awards in Science and Engineering (CASE) studentship. This work was performed primarily at the Materials Science Division at Argonne National Laboratory, supported by the US Department of Energy, Office of Science, Office of Basic Energy Sciences, Materials Sciences and Engineering Division. We gratefully acknowledge the computing resources provided on Bebop, the high-performance computing clusters operated by the Laboratory Computing Resource Center at Argonne National Laboratory. First-principles modelling at Duke University (J.D., O.D.) was supported by the US Department of Energy, Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division, under award no. DE-SC0019299. Work at Oak Ridge National Laboratory’s Spallation Neutron Source is supported by the US Department of Energy, Office of Basic Energy Sciences. The Oak Ridge National Laboratory is managed by UT–Battelle for the US Department of Energy under contract no. DEAC05-00OR22725. This work made use of the Integrated Molecular Structure Education and Research Center (IMSERC) facility at Northwestern University, which has received support from the Soft and Hybrid Nanotechnology Experimental (SHyNE) Resource (NSF ECCS-2025633) and Northwestern University. A.J.E.R. and M.J.J. gratefully acknowledge the Faraday Institution Lithium-Sulfur Technology Accelerator (LiSTAR) programme (FIRG014, EP/S003053/1) for funding.
Publisher Copyright:
© 2021, The Author(s), under exclusive licence to Springer Nature Limited.
PY - 2021/12
Y1 - 2021/12
N2 - Superionic conductors possess liquid-like ionic diffusivity in the solid state, finding wide applicability from electrolytes in energy storage to materials for thermoelectric energy conversion. Type I superionic conductors (for example, AgI, Ag2Se and so on) are defined by a first-order transition to the superionic state and have so far been found exclusively in three-dimensional crystal structures. Here, we reveal a two-dimensional type I superionic conductor, α-KAg3Se2, by scattering techniques and complementary simulations. Quasi-elastic neutron scattering and ab initio molecular dynamics simulations confirm that the superionic Ag+ ions are confined to subnanometre sheets, with the simulated local structure validated by experimental X-ray powder pair-distribution-function analysis. Finally, we demonstrate that the phase transition temperature can be controlled by chemical substitution of the alkali metal ions that compose the immobile charge-balancing layers. Our work thus extends the known classes of superionic conductors and will facilitate the design of new materials with tailored ionic conductivities and phase transitions.
AB - Superionic conductors possess liquid-like ionic diffusivity in the solid state, finding wide applicability from electrolytes in energy storage to materials for thermoelectric energy conversion. Type I superionic conductors (for example, AgI, Ag2Se and so on) are defined by a first-order transition to the superionic state and have so far been found exclusively in three-dimensional crystal structures. Here, we reveal a two-dimensional type I superionic conductor, α-KAg3Se2, by scattering techniques and complementary simulations. Quasi-elastic neutron scattering and ab initio molecular dynamics simulations confirm that the superionic Ag+ ions are confined to subnanometre sheets, with the simulated local structure validated by experimental X-ray powder pair-distribution-function analysis. Finally, we demonstrate that the phase transition temperature can be controlled by chemical substitution of the alkali metal ions that compose the immobile charge-balancing layers. Our work thus extends the known classes of superionic conductors and will facilitate the design of new materials with tailored ionic conductivities and phase transitions.
UR - http://www.scopus.com/inward/record.url?scp=85111122359&partnerID=8YFLogxK
UR - http://www.scopus.com/inward/citedby.url?scp=85111122359&partnerID=8YFLogxK
U2 - 10.1038/s41563-021-01053-9
DO - 10.1038/s41563-021-01053-9
M3 - Article
C2 - 34294884
AN - SCOPUS:85111122359
SN - 1476-1122
VL - 20
SP - 1683
EP - 1688
JO - Nature materials
JF - Nature materials
IS - 12
ER -