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Title: Deconvolution of Composition and Crystallite Size of Silver Hollandite Nanorods: Influence on Electrochemistry

In this paper, silver hollandite (Ag 1.4Mn 8O 16) has been synthesized by an aqueous, low-temperature co-precipitation technique to afford silver hollandite with distinct crystallite sizes (10 and 15 nm, identified as S-Ag 1.4Mn 8O 16 and L-Ag 1.4Mn 8O 16, respectively) and equivalent silver content (x), allowing for the deconvolution of electrochemical effects related to crystallite size and silver content. The as-prepared silver hollandite materials were confirmed to be structurally analogous. Notably, TEM imaging reveals a high degree of bundling of S-Ag 1.4Mn 8O 16 nanorods compared to L-Ag 1.4Mn 8O 16 which facilitates more intimate connection of the S-Ag 1.4Mn 8O 16 material with enhanced interparticle contact. The electrochemical behavior and lithium diffusion properties were investigated by galvanostatic cycling, CV, electrochemical impedance, pulsed-discharge experiments, and ex-situ XAS analysis of cycled cathodes. Lithium based electrochemical cells containing S-Ag 1.4Mn 8O 16 delivered a capacity 15X higher than L-Ag 1.4Mn 8O 16 on cycle 1. Ex-situ XAS demonstrated structural change for S-Ag 1.4Mn 8O 16 and formation of Ag 0 on insertion of 3.8 Li + intercalation. However, the samples of L-Ag 1.4Mn 8O 16 were lithiated by a more limited 0.25 molar equivalents, where no significant structural changes weremore » observed. Finally, the findings affirm crystallite size significantly impacts electrochemistry independent of cation occupancy of the α-MnO 2 type structure.« less
Authors:
 [1] ; ORCiD logo [1] ;  [1] ;  [2] ;  [2] ;  [2] ;  [2] ;  [3] ;  [4] ;  [4]
  1. Stony Brook Univ., NY (United States). Dept. of Chemistry
  2. Brookhaven National Lab. (BNL), Upton, NY (United States). Energy Sciences Directorate
  3. Stony Brook Univ., NY (United States). Dept. of Chemistry. Dept. of Materials Science and Chemical Engineering; Brookhaven National Lab. (BNL), Upton, NY (United States). Energy Sciences Directorate
  4. Stony Brook Univ., NY (United States). Dept. of Chemistry. Dept. of Materials Science and Chemical Engineering
Publication Date:
Report Number(s):
BNL-203324-2018-JAAM
Journal ID: ISSN 0013-4651
Grant/Contract Number:
SC0012704; SC0012673; AC02-06CH11357
Type:
Accepted Manuscript
Journal Name:
Journal of the Electrochemical Society
Additional Journal Information:
Journal Volume: 164; Journal Issue: 14; Journal ID: ISSN 0013-4651
Publisher:
The Electrochemical Society
Research Org:
Brookhaven National Lab. (BNL), Upton, NY (United States); Stony Brook Univ., NY (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
OSTI Identifier:
1425104