24.02.2009
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24.02.2009

Incorporation of hydrogen in barium-doped α-alumina






Yuji OkuyamaCorresponding Author Contact Information, a, E-mail The Corresponding Author, Noriaki Kuritaa and Norihiko Fukatsua






aDepartment of Materials Science and Engineering, Graduate School of Engineering, Omohi College, Nagoya Institute of Technology, Gokiso-cho, Showa-ku, Nagoya 466-8555, Japan






Received 2 March 2007; 


revised 2 December 2008; 


accepted 25 December 2008. 


Available online 4 February 2009.






Abstract


The phenomenon of the incorporation of hydrogen into a single crystal of 0.1 mol% barium-doped α-alumina grown by the Verneuil method was studied using infrared absorption and conductivity measurements. A wide band of infrared absorption was observed in the range of 2500–3500 cm− 1 for the sample annealed in H2/H2O atmosphere and in the range of 2150–2300 cm− 1 for that annealed in D2/D2O atmosphere. These absorption bands were found to be attributed to the stretching vibration of the OH and OD bonds, respectively. The solubility of hydrogen was dependent only on hydrogen partial pressure under an oxidizing atmosphere. The IR absorbance measurement using polarized light was carried out to examine the crystal orientation dependence of the integral absorbance. The maximum intensity of integral absorbance was observed when the direction of the electric field was parallel to the direction of the c-axis. The H+/D+-isotope effect on the electrical conductivity was observed under a hydrogen atmosphere, and the chemical diffusion coefficient of the H+/D+ diffusion pair was determined by the relaxation time of the ohmic resistance change upon exchanging the atmosphere from H2 to D2. The temperature dependence of the self-diffusion coefficient of a proton was expressed as View the MathML source in the temperature range 1073–1373 K. The amount of dissolved hydrogen was estimated to be (1.0 ± 0.3) × 10− 6 mol cm− 3 using the self-diffusion coefficient and the value of conductivity.





Keywords: Proton conductor; Corundum; Diffusion coefficient; Conductivity; IR absorption; Solid electrolyte





Article Outline



1. Introduction
2. Theoretical background

2.1. Chemical diffusion coefficient of the D+/H+ diffusion pair from absorption intensity
2.2. Chemical diffusion coefficient of the D+/H+ diffusion pair from ohmic resistance
2.3. Estimation of self-diffusion coefficient of a proton from the chemical diffusion coefficient of the D+/H+ diffusion pair
2.4. Determination of mobility and concentration of charge carriers

3. Experimental

3.1. Sample preparation
3.2. Measurement of IR absorption
3.3. Measurement of electrical properties

4. Results

4.1. Dissolution of protons into the crystal
4.2. Anisotropy of infrared absorption
4.3. Determination of chemical diffusion coefficient of the D+/H+ diffusion pair

5. Discussion

5.1. Location of protons in the crystal lattice
5.2. Diffusion of protons in the crystal
5.3. Amount of hydrogen incorporated into the crystal

6. Conclusions
Acknowledgements
References





































































Corresponding Author Contact InformationCorresponding author. Tel.: +81 52 735 5315; fax: +81 52 735 5571.










Solid State Ionics
Volume 180, Issues 2-3, 9 March 2009, Pages 175-182


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  • Harton Vladislav Vadim  honorary member of ISSC science council

  • Lichtenstain Alexandr Iosif  honorary member of ISSC science council

  • Novikov Dimirtii Leonid  honorary member of ISSC science council

  • Yakushev Mikhail Vasilii  honorary member of ISSC science council

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