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Hydrogen transport property of polymer-derived cobalt cation-doped amorphous silica

Abstract : The effect of the local structure of Co-doped amorphous silica on the hydrogen transport property was studied with the aim to improve the high-temperature hydrogen-permselectivity of microporous amorphous silica-based membranes. Co-Doped silica materials with measured Co/Si atomic ratios ranging from 0.01 to 0.18 were successfully synthesized through the polymer-derived ceramic (PDC) route. X-ray diffraction (XRD) and high-resolution transmission electron microscopy (HRTEM) analyses confirmed the amorphous state of the polymer-derived Co-doped silica, while both X-ray photoelectron and Fourier transform infrared (FT-IR) spectroscopy analyses revealed that the divalent Co cation (Co 2+) modified the matrix amorphous silica network to form hydrogen-bonded silanol. After dehydration treatment at 500°C in argon, hydrogen (H)/deuterium (D) isotope exchange behavior on the surface silanol groups (Si-OH/OD conversion) of the polymer-derived non-doped and Co-doped amorphous silica was in situ monitored by measuring diffuse reflectance infrared Fourier transform (DRIFT) spectra at 500°C. The self-diffusion coefficient for OH/OD conversion of free silanol groups of non-doped silica was 6.1 × 10 −15 m 2 s −1 , while that on the hydrogen bonded Si-OH was found to reach 15.6 × 10 −15 m 2 s −1 by Co-doping at the measured Co/Si atomic ratio of 0.05.The effect of the amount of Co 2+ doping on the hydrogen transport property was further studied by scanning transmission electron microscopy and electron energy loss spectroscopy (STEM-EELS) analyses, and it was suggested that a rather small amount of Co-doping, i.e. Co/Si atomic ratio of 0.05 was effective for enhancing high-temperature hydrogen permeance through microporous amorphous silica-based membranes.
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Submitted on : Friday, December 18, 2020 - 3:28:12 PM
Last modification on : Friday, April 1, 2022 - 3:54:58 AM
Long-term archiving on: : Friday, March 19, 2021 - 6:10:17 PM

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Shotaro Tada, Shiori Ando, Toru Asaka, Yusuke Daiko, Sawao Honda, et al.. Hydrogen transport property of polymer-derived cobalt cation-doped amorphous silica. Inorganic Chemistry Frontiers, Royal Society of Chemistry, 2021, 8, pp.90-99. ⟨10.1039/d0qi01035a⟩. ⟨hal-03053425⟩

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