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Title: Computational and Experimental Investigations of Na-Ion Conduction in Cubic Na 3PSe 4

Abstract

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 Na 3PSe 4. 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 Na 3PSe 4 only permits rapid Na + diffusion with the presence of defects, and that the formation of the Na vacancy (charge-balanced by slight Se 2– 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.

Authors:
 [1];  [2];  [1];  [2];  [3]
  1. Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  2. Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)
  3. Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Univ. of California, Berkeley, CA (United States)
Publication Date:
Research Org.:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1393010
Grant/Contract Number:  
AC02-05CH11231
Resource Type:
Accepted Manuscript
Journal Name:
Chemistry of Materials
Additional Journal Information:
Journal Volume: 28; Journal Issue: 1; Journal ID: ISSN 0897-4756
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 36 MATERIALS SCIENCE

Citation Formats

Bo, Shou -Hang, Wang, Yan, Kim, Jae Chul, Richards, William Davidson, and Ceder, Gerbrand. Computational and Experimental Investigations of Na-Ion Conduction in Cubic Na3PSe4. United States: N. p., 2015. Web. doi:10.1021/acs.chemmater.5b04013.
Bo, Shou -Hang, Wang, Yan, Kim, Jae Chul, Richards, William Davidson, & Ceder, Gerbrand. Computational and Experimental Investigations of Na-Ion Conduction in Cubic Na3PSe4. United States. doi:10.1021/acs.chemmater.5b04013.
Bo, Shou -Hang, Wang, Yan, Kim, Jae Chul, Richards, William Davidson, and Ceder, Gerbrand. Tue . "Computational and Experimental Investigations of Na-Ion Conduction in Cubic Na3PSe4". United States. doi:10.1021/acs.chemmater.5b04013. https://www.osti.gov/servlets/purl/1393010.
@article{osti_1393010,
title = {Computational and Experimental Investigations of Na-Ion Conduction in Cubic Na3PSe4},
author = {Bo, Shou -Hang and Wang, Yan and Kim, Jae Chul and Richards, William Davidson and Ceder, Gerbrand},
abstractNote = {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.},
doi = {10.1021/acs.chemmater.5b04013},
journal = {Chemistry of Materials},
number = 1,
volume = 28,
place = {United States},
year = {2015},
month = {11}
}

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