Journal
CHEMISTRY OF MATERIALS
Volume 29, Issue 10, Pages 4401-4410Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.chemmater.7b00879
Keywords
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Funding
- Fundamental Research Program of the Korea Institute of Materials Science (KIMS)
- Basic Science Research Program through the National Research Foundation of Korea (NRF) - Ministry of Education [2016R1D1A1B03932055]
- National Research Foundation of Korea [2016R1D1A1B03932055] Funding Source: Korea Institute of Science & Technology Information (KISTI), National Science & Technology Information Service (NTIS)
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A novel mesoporous silica-based single-ion conductor for lithium-ion batteries was prepared via two-step selective functionalization of designated silica precursors into the inner pore wall of mesoporous silica. 2-[(Trifluoromethanesulfonylimido)-N-4-sulfonylphenyl]ethyl (TFSISPE) group was first incorporated as a silica precursor having an anionic weak-binding imide group, and a dense brush of oligo-poly(ethylene glycol) (oligo-PEG) moieties, solvating Li, was cografted to produce functionalized mesoporous silica (FMS-TFSISPE) nanoparticles. FMS-TFSISPE showed a 2D hexagonal nanopore structure and a regular spherical shape with an average diameter of 50 nm. Poly(ethylene oxide) (PEO) was used to form a dispersion of the mesoporous silica nanoparticles into the polymer matrix. This new polymer-mesoporous silica nanohybrid solid electrolyte with the sole mobile Li ions (FMS-TFSISPE-PEO) exhibits attractive electrical, mechanical, and electrochemical properties. The ionic conductivity and storage modulus both increase simultaneously upon addition of FMS-TFSISPE nanoparticles. A 30 wt % amount of FMS-TFSISPE nanop articles leads to the highest ionic conductivity (sigma(DC) similar to 10(-3) S/cm at 25 degrees C) and storage modulus (G' similar to 10(4) Pa at 30 degrees C) with a high lithium ion transference number (t(Li)(+) similar to 0.9). Compared to conventional nonporous silica nanoparticles-incorporated PEO matrix (SiO2-TFSISPE-PEO), FMS-TFSISPE-PEO exhibits 2 orders of magnitude higher ionic conductivity with lower activation energy, suggesting that the facile transportation of lithium ions is achieved through the continuous weak-binding and solvating nanopore channel of the mesoporous silica retaining a high surface area and pore volume.
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