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
相关论文
共 74 条
[1]   Mechanisms and rate laws for oxygen exchange on mixed-conducting oxide surfaces [J].
Adler, S. B. ;
Chen, X. Y. ;
Wilson, J. R. .
JOURNAL OF CATALYSIS, 2007, 245 (01) :91-109
[2]   Fundamental issues in modeling of mixed-conductors (A rebuttal to comments on ''electrode kinetics of porous mixed-conducting oxygen electrodes'') [J].
Adler, SB ;
Lane, JA ;
Steele, BCH .
JOURNAL OF THE ELECTROCHEMICAL SOCIETY, 1997, 144 (05) :1884-1890
[3]   Mechanism and kinetics of oxygen reduction on porous La1-xSrxCoO3-δ electrodes [J].
Adler, SB .
SOLID STATE IONICS, 1998, 111 (1-2) :125-134
[4]   Electrode kinetics of porous mixed-conducting oxygen electrodes [J].
Adler, SB ;
Lane, JA ;
Steele, BCH .
JOURNAL OF THE ELECTROCHEMICAL SOCIETY, 1996, 143 (11) :3554-3564
[5]   Factors governing oxygen reduction in solid oxide fuel cell cathodes [J].
Adler, SB .
CHEMICAL REVIEWS, 2004, 104 (10) :4791-4843
[6]  
ADLER SB, UNPUB
[7]   Surface-structure sensitivity of CO oxidation over polycrystalline ceria powders [J].
Aneggi, E ;
Llorca, J ;
Boaro, M ;
Trovarelli, A .
JOURNAL OF CATALYSIS, 2005, 234 (01) :88-95
[8]   FEASIBILITY OF ROCKET PROPELLANT PRODUCTION ON MARS [J].
ASH, RL ;
DOWLER, WL ;
VARSI, G .
ACTA ASTRONAUTICA, 1978, 5 (09) :705-724
[9]   Advanced anodes for high-temperature fuel cells [J].
Atkinson, A ;
Barnett, S ;
Gorte, RJ ;
Irvine, JTS ;
Mcevoy, AJ ;
Mogensen, M ;
Singhal, SC ;
Vohs, J .
NATURE MATERIALS, 2004, 3 (01) :17-27
[10]   Properties of La0.6Sr0.4Co0.2Fe0.8O3-δ (LSCF) double layer cathodes on gadolinium-doped cerium oxide (CGO) electrolytes -: I.: Role of SiO2 [J].
Bae, JM ;
Steele, BCH .
SOLID STATE IONICS, 1998, 106 (3-4) :247-253