Facile Proton Transport in Ammonium Borosulfate—An Unhumidified Solid Acid Polyelectrolyte for Intermediate Temperatures |
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Authors: | Matthew D Ward Brian L Chaloux Michelle D Johannes Albert Epshteyn |
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Affiliation: | 1. Chemistry Division, US Naval Research Laboratory, Washington, DC, 20375 USA;2. Center for Computational Materials Science, US Naval Research Laboratory, Washington, DC, 20375 USA |
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Abstract: | High proton conductivity is reported for unhumidified ammonium borosulfate, NH4B(SO4)2], a solid acid coordination polymer that contains 1D, hydrogen-bonded NH4+···1∞B(SO4)4/2]? chains. NH4B(SO4)2] is thermally stable to 320 °C and is amenable to sintering into monolithic, polycrystalline discs at 200 °C and about 300 MPa of uniaxial pressure. Impedance spectroscopy measurements reveal ionic conductivities for sintered ammonium borosulfate of 0.1 mS cm?1 at 25 °C and up to 10 mS cm?1 at 180 °C in ambient air. No superprotonic transition is observed in the temperature range of 25–180 °C. Ab initio molecular dynamics simulations show these high conductivities are aided by free rotation of the NH4+ units and significant gyrational mobility of the SO4 tetrahedra, which, in turn, provide facile pathways for proton locomotion. High conductivities, a wide operational temperature window, and tolerance to both ambient and anhydrous conditions make NH4B(SO4)]2 an attractive candidate electrolyte for intermediate-temperature hydrogen fuel cells that may enable operation at temperatures as high as 300 °C without active humidification. |
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Keywords: | intermediate-temperature hydrogen fuel cells proton conductors solid electrolytes |
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