Palladium-gallium intermetallic compounds for the selective hydrogenation of acetylene -: Part I:: Preparation and structural investigation under reaction conditions

被引:256
作者
Osswald, Juergen [1 ]
Giedigkeit, Rainer [2 ]
Jentoft, Rolf E. [1 ]
Armbruester, Marc [1 ]
Girgsdies, Frank [1 ]
Kovnir, Kirill [1 ,2 ]
Ressler, Thorsten [3 ]
Grin, Yuri [2 ]
Schloegl, Robert [1 ]
机构
[1] Max Planck Gesell, Fritz Haber Inst, Dept Inorgan Chem, D-14195 Berlin, Germany
[2] Max Planck Inst Chem Phys Fester Stoffe, D-01187 Dresden, Germany
[3] Tech Univ Berlin, Inst Chem, D-10623 Berlin, Germany
关键词
palladium; gallium; PdGa; Pd3Ga7; acetylene; ethylene; hydrogenation; selectivity; stability; site isolation; intermetallic compound; hydride; XAS; XRD;
D O I
10.1016/j.jcat.2008.06.013
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 intemetallic compounds PdGa and Pd3Ga7 are introduced as selective catalysts for the hydrogenation of acetylene. Single phase PdGa and Pd3Ga7 can readily be prepared by the appropriate thermal treatment of the stoichiometric mixtures of the corresponding elements. The initial low surface areas of the as-prepared materials can be increased by careful mechanical treatment without decomposition. Detailed investigations of PdGa and Pd3Ga7 by DSC/TG, in situ powder X-ray diffraction and in situ X-ray absorption spectroscopy during thermal treatment under various inert or reactive gas atmospheres showed a high thermal stability. The long-range and short-range order in the crystal structures remained intact up to temperatures of about 600 K. Neither phase transitions nor decomposition were detectable. In addition to high thermal stability-preserving the active-site isolation under reaction conditions-no incorporation of hydrogen or carbon in the intemetallic compounds under reducing conditions was observed. Besides being interesting model systems, palladium-gallium intermetallic compounds are promising candidates for the application as highly selective hydrogenation catalysts. (C) 2008 Elsevier Inc. All rights reserved.
引用
收藏
页码:210 / 218
页数:9
相关论文
共 55 条
[1]   Poisoning and deactivation of palladium catalysts [J].
Albers, P ;
Pietsch, J ;
Parker, SF .
JOURNAL OF MOLECULAR CATALYSIS A-CHEMICAL, 2001, 173 (1-2) :275-286
[2]   Real-space multiple-scattering calculation and interpretation of x-ray-absorption near-edge structure [J].
Ankudinov, AL ;
Ravel, B ;
Rehr, JJ ;
Conradson, SD .
PHYSICAL REVIEW B, 1998, 58 (12) :7565-7576
[3]  
Arnold H., 1997, HDB HETEROGENEOUS CA, V5, P2165
[4]   Photoelectron diffraction study of a catalytically active overlayer:: C2H2 on Pd{111} [J].
Baddeley, CJ ;
Lee, AF ;
Lambert, RM ;
Giessel, T ;
Schaff, O ;
Fernandez, V ;
Schindler, KM ;
Theobald, A ;
Hirschmugl, CJ ;
Lindsay, R ;
Bradshaw, AM ;
Woodruff, DP .
SURFACE SCIENCE, 1998, 400 (1-3) :166-175
[5]   COEXISTENT PHASES OF FESI-TYPE IN MIXTURES OF NI-PD-GA AND NI-PT-GA [J].
BHARGAVA, MK ;
GADALLA, AA ;
SCHUBERT, K .
JOURNAL OF THE LESS-COMMON METALS, 1975, 42 (01) :69-76
[6]   HYDROGENATION OF ACETYLENE .2. REACTION OF ACETYLENE WITH HYDROGEN CATALYZED BY ALUMINA-SUPPORTED PALLADIUM [J].
BOND, GC ;
WELLS, PB .
JOURNAL OF CATALYSIS, 1966, 5 (01) :65-+
[7]   Selective hydrogenation of ethyne in ethene-rich streams on palladium catalysts. Part 1. Effect of changes to the catalyst during reaction [J].
Borodzinki, Andrzej .
CATALYSIS REVIEWS-SCIENCE AND ENGINEERING, 2006, 48 (02) :91-144
[8]   MECHANISM AND KINETICS OF THE SELECTIVE HYDROGENATION OF ETHYNE AND ETHENE [J].
BOS, ANR ;
WESTERTERP, KR .
CHEMICAL ENGINEERING AND PROCESSING-PROCESS INTENSIFICATION, 1993, 32 (01) :1-7
[9]   Bimetallic palladium catalysts: influence of the co-metal on the catalyst performance [J].
Coq, B ;
Figueras, F .
JOURNAL OF MOLECULAR CATALYSIS A-CHEMICAL, 2001, 173 (1-2) :117-134
[10]   2ND EUROPEAN SYMPOSIUM ON CATALYSIS BY METALS - MULTIMETALLIC CATALYSTS IN SYNTHESIS AND TRANSFORMATION OF HYDROCARBONS - CONCLUDING REMARKS, CRITICAL ISSUES AND PERSPECTIVES [J].
DEROUANE, EG .
JOURNAL OF MOLECULAR CATALYSIS, 1984, 25 (1-3) :51-58