X-ray photoelectron spectroscopic study of the surface state during ethane oxidative dehydrogenation at millisecond contact times

被引:8
作者
Claycomb, Gregory D. [2 ]
Sherwood, Peter M. A. [2 ]
Traxel, Brent E. [1 ]
Hohn, Keith L. [1 ]
机构
[1] Kansas State Univ, Dept Chem Engn, Manhattan, KS 66506 USA
[2] Oklahoma State Univ, Dept Phys, Stillwater, OK 74078 USA
关键词
D O I
10.1021/jp073555q
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
The chemical nature of Pt/alpha-Al2O3 catalysts has been studied using X-ray photoelectron spectroscopy (XPS) during, catalyst preparation and after being exposed to different feed compositions during autothermal oxidative dehydrogenation of ethane. In addition, the axial variation in surface chemistry has been probed by studying the front and back sides of the catalyst. Significant surface changes were observed following the addition and removal of chlorine to the feed. Chlorine addition led to large carbon deposits throughout the catalyst, and a significant surface concentration of chlorine on the catalyst surface. Chlorine addition also changed the oxidation state of platinum, leading to more oxidized platinum at the front of the monolith and more reduced platinum at the back of the monolith. Subsequent removal of chlorine led to the disappearance of chlorine from the XPS spectrum and to the removal of a significant amount of carbon from the front and back of the catalytic monolith.
引用
收藏
页码:18724 / 18730
页数:7
相关论文
共 31 条
[1]   X-RAY PHOTOELECTRON SPECTROSCOPIC STUDIES OF ELECTRODE SURFACES USING A NEW CONTROLLED TRANSFER TECHNIQUE .2. RESULTS FOR A MOLYBDENUM ELECTRODE AND THE CURVE FITTING PROCEDURE [J].
ANSELL, RO ;
DICKINSON, T ;
POVEY, AF ;
SHERWOOD, PMA .
JOURNAL OF ELECTROANALYTICAL CHEMISTRY, 1979, 98 (01) :79-89
[2]   A CHEMISORPTION AND XPS STUDY OF BIMETALLIC PT-SN/AL2O3 CATALYSTS [J].
BALAKRISHNAN, K ;
SCHWANK, J .
JOURNAL OF CATALYSIS, 1991, 127 (01) :287-306
[3]   ESCA STUDY OF SPUTTERED PLATINUM FILMS [J].
BANCROFT, GM ;
ADAMS, I ;
COATSWORTH, LL ;
BENNEWITZ, CD ;
BROWN, JD ;
WESTWOOD, WD .
ANALYTICAL CHEMISTRY, 1975, 47 (03) :586-588
[4]   Oxidative dehydrogenation of ethane at millisecond contact times:: Effect of H2 addition [J].
Bodke, AS ;
Henning, D ;
Schmidt, LD ;
Bharadwaj, SS ;
Maj, JJ ;
Siddall, J .
JOURNAL OF CATALYSIS, 2000, 191 (01) :62-74
[5]   METHOD TO REDUCE HYDROCARBON CONTAMINATION OF SAMPLES IN X-RAY PHOTOELECTRON-SPECTROSCOPY [J].
CLARK, DT ;
THOMAS, HR ;
DILKS, A ;
SHUTTLEWORTH, D .
JOURNAL OF ELECTRON SPECTROSCOPY AND RELATED PHENOMENA, 1977, 10 (04) :455-460
[6]  
Dickinson T., 1973, Journal of Electron Spectroscopy and Related Phenomena, V2, P441, DOI 10.1016/0368-2048(73)80058-1
[7]   X-RAY PHOTOELECTRON SPECTROSCOPIC STUDIES OF OXIDE-FILMS ON PLATINUM AND GOLD ELECTRODES [J].
DICKINSON, T ;
POVEY, AF ;
SHERWOOD, PMA .
JOURNAL OF THE CHEMICAL SOCIETY-FARADAY TRANSACTIONS I, 1975, 71 (02) :298-311
[8]   INFLUENCE OF THE CHLORINE CONTENT ON THE BEHAVIOR OF CATALYSTS FOR NORMAL-HEPTANE REFORMING [J].
FIGOLI, NS ;
SAD, MR ;
BELTRAMINI, JN ;
JABLONSKI, EL ;
PARERA, JM .
INDUSTRIAL & ENGINEERING CHEMISTRY PRODUCT RESEARCH AND DEVELOPMENT, 1980, 19 (04) :545-551
[9]   HALOGENATION OF CARBON SURFACES BY ATOMIC-BEAMS - HOPG GRAPHITE [J].
FREEDMAN, A .
DIAMOND AND RELATED MATERIALS, 1995, 4 (03) :216-219
[10]   FORMATION OF A PLATINUM OXIDE DURING THE THERMAL-OXIDATION OF NOBLE-METAL ALLOYS [J].
GRAHAM, GW ;
POTTER, TJ ;
WEBER, WH .
JOURNAL OF VACUUM SCIENCE & TECHNOLOGY A-VACUUM SURFACES AND FILMS, 1989, 7 (03) :1694-1696