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A New Solid-State Proton Conductor: The Salt Hydrate Based on Imidazolium and 12-Tungstophosphate

Martinelli, Anna, 1978 (author)
Chalmers tekniska högskola,Chalmers University of Technology
Otero-Mato, José M. (author)
Universidade de Santiagode Compostela
Garaga Nagendrachar, Mounesha, 1985 (author)
Dalhousie University
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Elamin, Khalid, 1977 (author)
Chalmers tekniska högskola,Chalmers University of Technology
Rahman, Habibur Seikh Mohammad, 1976 (author)
Chalmers tekniska högskola,Chalmers University of Technology
Zwanziger, Josef W. (author)
Dalhousie University
Werner-Zwanziger, Ulrike (author)
Dalhousie University
Varela, Luis M. (author)
Universidade de Santiagode Compostela
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 (creator_code:org_t)
2021-08-18
2021
English.
In: Journal of the American Chemical Society. - : American Chemical Society (ACS). - 1520-5126 .- 0002-7863. ; 143:34, s. 13895-13907
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  • Journal article (peer-reviewed)
Abstract Subject headings
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  • We report the structure and charge transport properties of a novel solid-state proton conductor obtained by acid-base chemistry via proton transfer from 12-tungstophosphoric acid to imidazole. The resulting material (henceforth named Imid3WP) is a solid salt hydrate that, at room temperature, includes four water molecules per structural unit. To our knowledge, this is the first attempt to tune the properties of a heteropolyacid-based solid-state proton conductor by means of a mixture of water and imidazole, interpolating between water-based and ionic liquid-based proton conductors of high thermal and electrochemical stability. The proton conductivity of Imid3WP·4H2O measured at truly anhydrous conditions reads 0.8 × 10-6 S cm-1 at 322 K, which is higher than the conductivity reported for any other related salt hydrate, despite the lower hydration. In the pseudoanhydrous state, that is, for Imid3WP·2H2O, the proton conductivity is still remarkable and, judging from the low activation energy (Ea = 0.26 eV), attributed to structural diffusion of protons. From complementary X-ray diffraction data, vibrational spectroscopy, and solid-state NMR experiments, the local structure of this salt hydrate was resolved, with imidazolium cations preferably orienting flat on the surface of the tungstophosphate anions, thus achieving a densely packed solid material, and water molecules of hydration that establish extremely strong hydrogen bonds. Computational results confirm these structural details and also evidence that the path of lowest energy for the proton transfer involves primarily imidazole and water molecules, while the proximate Keggin anion contributes with reducing the energy barrier for this particular pathway.

Subject headings

NATURVETENSKAP  -- Kemi -- Oorganisk kemi (hsv//swe)
NATURAL SCIENCES  -- Chemical Sciences -- Inorganic Chemistry (hsv//eng)
NATURVETENSKAP  -- Kemi -- Fysikalisk kemi (hsv//swe)
NATURAL SCIENCES  -- Chemical Sciences -- Physical Chemistry (hsv//eng)
NATURVETENSKAP  -- Kemi -- Materialkemi (hsv//swe)
NATURAL SCIENCES  -- Chemical Sciences -- Materials Chemistry (hsv//eng)

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