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A two-dimensional type I superionic conductor
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DOI：10.1038/s41563-021-01053-9.png)
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Abstract
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Superionic conductors present liquid-like ionic diffusivity with applications ranging from energy storage to thermoelectrics. A two-dimensional type I superionic conductor alpha-KAg3Se2 is now reported and should help to design other materials with tailored ionic conductivities and phase transitions. 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, alpha-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.
Keywords:
TOTAL-ENERGY CALCULATIONS
ELECTRICAL-CONDUCTIVITY
NEUTRON-SCATTERING
CRYSTAL-STRUCTURES
DIFFUSION
SILVER
LIQUID
TRANSITION
DYNAMICS
TEMPERATURE
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