Experimental and Computational Investigation of Effect of Sr on NO Oxidation and Oxygen Exchange for La1-xSrxCoO3 Perovskite Catalysts

被引:74
作者
Choi, Sang Ok [1 ,2 ]
Penninger, Michael [3 ]
Kim, Chang Hwan [5 ]
Schneider, William F. [3 ,4 ]
Thompson, Levi T. [1 ,2 ]
机构
[1] Univ Michigan, Dept Chem Engn, Ann Arbor, MI 48109 USA
[2] Univ Michigan, Hydrogen Energy Technol Lab, Ann Arbor, MI 48109 USA
[3] Univ Notre Dame, Dept Chem & Biomol Engn, Notre Dame, IN 46556 USA
[4] Univ Notre Dame, Dept Chem & Biochem, Notre Dame, IN 46556 USA
[5] Gen Motors Global R&D, Warren, MI 48090 USA
基金
美国国家科学基金会;
关键词
NO oxidation; perovskites; Sr substitution; oxygen mobility; isotope exchange; NO2; inhibition;
D O I
10.1021/cs400522r
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
NO oxidation rates over La1-xSrxCoO3 (x = 0-0.3) perovskite catalysts are reported as a function of Sr doping in the absence and presence of NO2 in the feed. Sr substitution is found to increase the rate of oxidation and to diminish the inhibitory influence of NO2. Temperature programmed desorption and isotopic exchange (TPIE) experiments were used to identify surface species and oxygen exchange processes expected to correlate with NO oxidation activity. Oxygen exchange in the LaCoO3 perovskites occurred primarily through a heteroexchange process that was enhanced by doping with Sr. Density functional theory (DFT) calculations were used to further investigate the oxygen exchange processes on (100) facets of undoped and doped LaCoO3. Vacancy formation is predicted to be more facile on CoO2-terminated than LaO-terminated surfaces. The Sr dopant segregates to the LaO-terminated surface and diminishes oxygen bonding consistent with the TPIE results. The results suggest a model in which multiple oxygen species contribute to low- and high-temperature oxygen exchange.
引用
收藏
页码:2719 / 2728
页数:10
相关论文
共 56 条
[1]   Synthesis and characterisation of La1-xSrxCoO3 with large surface area [J].
Berger, D ;
Fruth, V ;
Jitaru, I ;
Schoonman, J .
MATERIALS LETTERS, 2004, 58 (19) :2418-2422
[2]   Experimental and kinetic study of NO oxidation on model Pt catalysts [J].
Bhatia, Divesh ;
McCabe, Robert W. ;
Harold, Michael P. ;
Balakotaiah, Vemuri .
JOURNAL OF CATALYSIS, 2009, 266 (01) :106-119
[3]   Ethanol combustion over strontium- and cerium-doped LaCoO3 catalysts [J].
Bialobok, Beata ;
Trawczynski, Janusz ;
Mista, Wlodzimierz ;
Zawadzki, Miroslaw .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2007, 72 (3-4) :395-403
[4]  
BORESKOV GK, 1964, ADV CATAL, V15, P285
[5]  
Bourges P, 1998, STUD SURF SCI CATAL, V116, P213
[6]   Effect of oxygen vacancy on CO-NO-O-2 reaction over yttria-stabilized zirconia-supported copper oxide catalyst [J].
Chien, CC ;
Shi, JZ ;
Huang, TJ .
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH, 1997, 36 (05) :1544-1551
[7]   Computational study on the catalytic mechanism of oxygen reduction on La0.5Sr0.5MnO3 in solid oxide fuel cells [J].
Choi, YongMan ;
Lin, M. C. ;
Liu, Meilin .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2007, 46 (38) :7214-7219
[8]   Surface strontium enrichment on highly active perovskites for oxygen electrocatalysis in solid oxide fuel cells [J].
Crumlin, Ethan J. ;
Mutoro, Eva ;
Liu, Zhi ;
Grass, Michael E. ;
Biegalski, Michael D. ;
Lee, Yueh-Lin ;
Morgan, Dane ;
Christen, Hans M. ;
Bluhm, Hendrik ;
Shao-Horn, Yang .
ENERGY & ENVIRONMENTAL SCIENCE, 2012, 5 (03) :6081-6088
[9]   THERMAL-DESORPTION ANALYSIS - COMPARATIVE TEST OF 10 COMMONLY APPLIED PROCEDURES [J].
DEJONG, AM ;
NIEMANTSVERDRIET, JW .
SURFACE SCIENCE, 1990, 233 (03) :355-365
[10]   Catalytic oxidation of nitrogen monoxide over Pt/SiO2 [J].
Després, J ;
Elsener, M ;
Koebel, M ;
Kröcher, O ;
Schnyder, B ;
Wokaun, A .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2004, 50 (02) :73-82