Carbon dioxide reduction on gadolinia-doped ceria cathodes

被引:100
作者
Green, Robert D. [1 ]
Liu, Chung-Chiun [2 ]
Adler, Stuart B. [3 ]
机构
[1] NASA, Glenn Res Ctr, Cleveland, OH 44135 USA
[2] Case Western Reserve Univ, Dept Chem Engn, Cleveland, OH 44106 USA
[3] Univ Washington, Dept Chem Engn, Seattle, WA 98195 USA
基金
美国国家航空航天局;
关键词
carbon dioxide electrolysis; impedance spectroscopy; porous electrode model; exchange rate; vacancy diffusion coefficient; thermodynamic factor;
D O I
10.1016/j.ssi.2008.04.024
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
AC impedance spectroscopy has been performed on 40 mol% gadolinia-doped ceria electrodes on yttria stabilized zirconia (YSZ) at 700-950 degrees C in reducing CO/CO2 atmospheres. Area-specific-resistance (ASR) values for this electrode were in the range of 0.8-37 Omega-cm(2), about two orders of magnitude lower than measurements on Pt electrodes and slightly lower than data on Ni-YSZ electrodes in the literature under similar temperature and partial pressure of oxygen (P-O2) conditions. A continuum-based model of this electrode is described and ail analysis performed to extract the vacancy diffusion coefficient (D-nu) and surface exchange rate coefficient (R-0) as a function of temperature and P-O2, from the impedance results. The D-nu data agree reasonably well with published measurements of the tracer diffusion coefficient (D*) based on isotope profiling by secondary ion mass spectroscopy (SIMS) and conductivity measurements on 40 mol% GDC. The R-0 values are a factor of 3 lower than the published measurements of the surface reaction rate (k) obtained from isothermal thermogravimetric relaxation, and decrease with increasing P-O2. Values of the thermodynamic factor (A) calculated from the fitted model parameters matched well with those calculated from oxygen non-stoichiometry data in the literature. Published by Elsevier B.V.
引用
收藏
页码:647 / 660
页数:14
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