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  1. 2LiX-GaF3(X = Cl, Br, I) electrolytes offer favorable features for solid-state batteries: mechanical pliability and high conductivities. However, understanding the origin of fast ion transport in 2LiX-GaF3has been challenging. The ionic conductivity order of 2LiCl-GaF3(3.20 mS/cm) > 2LiBr-GaF3(0.84 mS/cm) > 2LiI-GaF3(0.03 mS/cm) contradicts binary LiCl (10−12S/cm) < LiBr (10−10S/cm) < LiI (10−7S/cm). Using multinuclear7Li,71Ga,19F solid-state nuclear magnetic resonance and density functional theory simulations, we found that Ga(F,X)npolyanions boost Li+-ion transport by weakening Li+-Xinteractions via charge clustering. In 2LiBr-GaF3and 2LiI-GaF3, Ga-X coordination is reduced with decreased F participation, compared to 2LiCl-GaF3. These insights will inform electrolyte design based on charge clustering, applicable to various ion conductors. This strategy could prove effective for producing highly conductive multivalent cation conductors such as Ca2+and Mg2+, as charge clustering of carboxylates in proteins is found to decrease their binding to Ca2+and Mg2+.

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    Free, publicly-accessible full text available November 24, 2024
  2. Free, publicly-accessible full text available June 1, 2024
  3. Boron oxide/hydroxide supported on oxidized activated carbon (B/OAC) was shown to be an inexpensive catalyst for the oxidative dehydrogenation (ODH) of propane that offers activity and selectivity comparable to boron nitride. Here, we obtain an atomistic picture of the boron oxide/hydroxide layer in B/OAC by using 35.2 T 11B and 17O solid-state NMR experiments. NMR spectra measured at 35.2 T resolve the boron and oxygen sites due to narrowing of the central-transition powder patterns. A 35.2 T 2D 11B{17O} dipolar heteronuclear correlation NMR spectrum revealed the structural connectivity between boron and oxygen atoms. The approach outlined here should be generally applicable to determine atomistic structures of heterogeneous catalysts containing quadrupolar nuclei. 
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