%0 Generic
%A Bo, Shou-Hang
%A Wang, Yan
%A Kim, Jae Chul
%A Richards, William
Davidson
%A Ceder, Gerbrand
%D 2016
%T Computational and Experimental Investigations of Na-Ion
Conduction in Cubic Na3PSe4
%U https://acs.figshare.com/articles/dataset/Computational_and_Experimental_Investigations_of_Na_Ion_Conduction_in_Cubic_Na_sub_3_sub_PSe_sub_4_sub_/2090005
%R 10.1021/acs.chemmater.5b04013.s002
%2 https://acs.figshare.com/ndownloader/files/3723220
%K Na 3PSe
%K conductivity
%K grain boundary resistance
%X All-solid-state Na-ion batteries
that operate at or close to room
temperature are a promising next-generation battery technology with
enhanced safety and reduced manufacturing cost. An indispensable component
of this technology is the solid-state electrolyte that allows rapid
shuttling of the mobile cation (i.e., Na+) between the
cathode and anode. However, there are very few fast Na-ion conductors
with ionic conductivity approaching that of the liquid counterparts
(i.e., 1 mS cm–1). In this work, we present the
synthesis and characterization of a fast Na-ion conductor, cubic Na3PSe4. This material possesses a room-temperature
ionic conductivity exceeding 0.1 mS cm–1 and does
not require high-temperature sintering to minimize grain boundary
resistance, making it a promising solid-state electrolyte candidate
for all-solid-state Na-ion battery applications. On the basis of density
functional theory, nudged elastic band, and molecular dynamics investigations,
we demonstrate that the framework of cubic Na3PSe4 only permits rapid Na+ diffusion with the presence of
defects, and that the formation of the Na vacancy (charge-balanced
by slight Se2– oxidation) is more energetically
favorable among the various defects considered. This finding provides
important guidelines to further improve Na-ion conductivity in this
class of materials.
%I ACS Publications