CHARACTERIZATION OF MIXED COPPER-MANGANESE OXIDES SUPPORTED ON TITANIA CATALYSTS FOR SELECTIVE OXIDATION OF AMMONIA

被引:196
作者
WOLLNER, A
LANGE, F
SCHMELZ, H
KNOZINGER, H
机构
[1] UNIV MUNICH,INST PHYS CHEM,SOPHIENSTR 11,W-8000 MUNICH 2,GERMANY
[2] SIEMENS AG,W-8627 REDWITZ,GERMANY
关键词
COPPER-MANGANESE OXIDES; TITANIA SUPPORT; AMMONIA OXIDATION; X-RAY DIFFRACTION; X-RAY PHOTOELECTRON SPECTROSCOPY; TEMPERATURE PROGRAMMED REDUCTION; STRUCTURE DETERMINATION;
D O I
10.1016/0926-860X(93)85007-C
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
Titania-supported copper-manganese mixed oxides were investigated in view of the selective oxidation of ammonia to dinitrogen and characterized by X-ray diffraction, photoelectron spectroscopy and temperature programmed reduction. The mixed oxides proved to be more active than the corresponding individual oxides. The TPR-results show that the reduction occurs at lower temperatures than that of the unsupported oxides. It is concluded that titania facilitates the change of oxidation states. Most active and selective for N2-formation is a catalyst with a molar ratio of Cu:Mn = 20:80. It contains a crystalline Cu1+xMn2-xO4 spinel phase (determined by XRD) and an additional X-ray amorphous Mn2+-containing species (determined by XPS), possibly Mn3O4 or MnO. Copper is present in the mono- and divalent oxidation state (shown by XPS). All catalysts hardly loose activity with time on stream, above all the copper-rich catalysts are very stable.
引用
收藏
页码:181 / 203
页数:23
相关论文
共 59 条
[1]   A STUDY OF A NUMBER OF MIXED TRANSITION-METAL OXIDE SPINELS USING X-RAY PHOTOELECTRON-SPECTROSCOPY [J].
ALLEN, GC ;
HARRIS, SJ ;
JUTSON, JA ;
DYKE, JM .
APPLIED SURFACE SCIENCE, 1989, 37 (01) :111-134
[2]  
BALKENENDE AR, 1991, CATALYTIC SCI TECHNO, P177
[3]  
BALTANAS MA, 1987, ACTA CHIM HUNG, V124, P357
[4]   STUDIES OF SURFACE BEHAVIOR OF OXIDE CATALYSTS BY SECONDARY ION MASS-SPECTROMETRY (SIMS) .1. SURFACE COMPOSITION OF COPPER-CONTAINING SPINEL CATALYSTS AND THEIR PRECURSORS [J].
BARBER, M ;
SHARPE, PK ;
VICKERMAN, JC .
JOURNAL OF CATALYSIS, 1976, 41 (02) :240-248
[5]  
BELEY M, 1978, ANN CHIM-SCI MAT, V3, P429
[6]   COPPER OXIDE SUPPORTED ON ALUMINA .2. ELECTRON SPIN RESONANCE STUDIES OF HIGHLY DISPERSED PHASES [J].
BERGER, PA ;
ROTH, JF .
JOURNAL OF PHYSICAL CHEMISTRY, 1967, 71 (13) :4307-&
[7]  
Bosch H., 1988, CATAL TODAY, V2, P369, DOI DOI 10.1016/0920-5861(88)80002-6
[8]   X-RAY PHOTOELECTRON-SPECTROSCOPY STUDY OF THE CATION VALENCIES IN NICKEL MANGANITE [J].
BRABERS, VAM ;
VANSETTEN, FM ;
KNAPEN, PSA .
JOURNAL OF SOLID STATE CHEMISTRY, 1983, 49 (01) :93-98
[9]  
BRIGGS D, 1983, PRACTICAL SURFACE AN
[10]   USE OF X-RAY PHOTOELECTRON SPECTROSCOPY TO STUDY BONDING IN CR, MN, FE, AND CO COMPOUNDS [J].
CARVER, JC ;
CARLSON, TA ;
SCHWEITZER, GK .
JOURNAL OF CHEMICAL PHYSICS, 1972, 57 (02) :973-+